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This study proposes an innovative strategy for achieving PN in synthetic domestic wastewater by side-stream sludge treatment using sulfide as the sole control factor. By conducting controllable batch experiments and response surface analysis, optimal sulfide treatment conditions were firstly determined as 90 mg/L of sulfide, 7.5 of pH, 100 rpm of rotation and 12 h of treatment time. After treatment, half of ammonia oxidizing bacteria (AOB) activity remained, but nitrite oxidizing bacteria (NOB) activity was barely detected. Nitrite accumulation rate of long-term running PN steadily reached 83.9 % with 99.1 % of ammonia removal efficiency. Sulfide treatment increased community diversity and facilitated stability of microbiota functioning with PN phenotype, which might be sustained by the positive correlation between ammonia oxidation gene (amoA) and sulfur oxidation gene (soxB). Correspondingly, the network analysis identified the keystone microbial taxa of persistent PN microbiota as Nitrosomonas, Thauera, Truepera, Defluviimonas and Sulitalea in the later stage of long-term reactor., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

Currently, headspace gas chromatography-mass spectrometry is a widely used method to identify the key odorants of sludge. However, the effect of incubation temperature on the generation and emission of key odorants from sludge was still uncertain. Thus, in this paper, headspace solid-phase microextraction gas chromatography-mass spectrometry (HS-SPME-GC-MS) and headspace gas chromatography-coupled ion mobility spectrometry (HS-GC-IMS) were carried out to analyze the volatiles emitted from the sludge incubated at different temperatures (30 °C, 50 °C, 60 °C, and 80 °C). The results indicated that the total volatile concentration of the sludge increased with temperatures, which affected the identified proportion of sludge key odorants to a certain extent. Differently from the aqueous solutions, the variation of volatile emission from the sludge was inconsistent with temperature changes, suggesting a multifactorial influence of incubation temperature on the identification of sludge odorants. The microbial community structure and adenosine triphosphate (ATP) metabolic activity of the sludge samples were analyzed at the initial state, 30 °C, and 80 °C. Although no significant effect of incubation temperature on the microbial community structure of the sludge, the incubation at 80 °C led to a noticeable decrease in microbial ATP metabolic activity, accompanied by a significant change in the proportion of odor-related microorganisms with low relative abundances. Changes in the composition and activity of these communities jointly contributed to the differences in odor emission from sludge at different temperatures. In summary, the incubation temperature affects the production and emission of volatiles from sludge through physicochemical and biochemical mechanisms, by which the microbial metabolism playing a crucial role. Therefore, when analyzing the key odorants of sludge, these factors should be considered., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

Waste activated sludge serves an important reservoir for antibiotics within wastewater treatment plants, and understanding the occurrence and evolution of antibiotics during sludge treatment is crucial to mitigate the potential risks of subsequent resource utilization of sludge. This study explores the degradation and transformation mechanisms of three typical antibiotics, oxytetracycline (OTC), ofloxacin (OFL), and azithromycin (AZI) during sludge hydrothermal treatment (HT), and investigates the influence of biopolymers transformation on the fate of these antibiotics. The findings indicate that HT induces a shift of antibiotics from solid-phase adsorption to liquid-phase dissolution in the initial temperature range of 25-90 °C, underscoring this phase's critical role in preparing antibiotics for subsequent degradation phases. Proteins (PN) and humic acids emerge as crucial for antibiotic binding, facilitating their redistribution within sludge. Specifically, the binding capacity sequence of biopolymers to antibiotics is as follows: OFL>OTC>AZI, highlighting that OFL-biopolymers display stronger electrostatic attraction, more available adsorption sites, and more stable binding strength. Furthermore, antibiotic degradation mainly occurs above 90 °C, with AZI being the most temperature-sensitive, degrading 92.97% at 180 °C, followed by OTC (91.26%) and OFL (52.51%). Concurrently, the degradation products of biopolymers compete for active sites to form novel amino acid-antibiotic conjugates, which inhibits the further degradation of antibiotics. These findings illuminate the effects of biopolymers evolution on intricate dynamics of antibiotics fate in sludge HT and are helpful to optimize the sludge HT process for effective antibiotics abatement., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

Tire wear particles (TWPs) are considered a significant contributor of microplastics (MPs) in the sludge during heavy rainfall events. Numerous studies have shown that hydrothermal treatment (HT) of sludge can accelerate the leaching of MP-derived compound into hydrothermal liquid, thus impairing the performance of subsequent anaerobic digestion and the quality of the hydrothermal liquid fertilizer. However, the leaching behavior of TWPs in the HT of sludge remains inadequately explored. This study examined the molecular composition of TWP-derived compounds and transformation pathways of representative tire-related additives under different hydrothermal temperatures using liquid chromatography-tandem mass spectrometry (LC-MS/MS) combined with mass difference analysis. The acute toxicity and phytotoxicity of TWP leachates were assessed using Vibrio qinghaiensis Q67 and rice hydroponics experiments. The results indicated that elevating the hydrothermal temperature not only amplified the leaching behavior of TWPs but also enhanced the chemical complexity of the TWP leachate. Utilizing both suspect and non-target screenings, a total of 144 compounds were identified as additives, including N-(1,3-dimethylbutyl)-N'-phenyl-p-phenylenediamine (6-PDD), hexa(methoxymethyl)melamine (HMMM), dibutyl phthalate (DBP). These additives underwent various reactions, such as desaturation, acetylation, and other reactions, leading to the formation of different transformation products (TPs). Moreover, certain additives, including caprolactam and 2,2,6,6-tetramethyl-4-piperidinol, demonstrated the potential to form conjugate products with amino acids or Maillard products. Meanwhile, TWP-derived compounds showed significant acute toxicity and detrimental effects on plant growth. This study systematically investigated the environmental fate of TWPs and their derived compounds during the HT of sludge, offering novel insights into the intricate interactions between the micropollutants and dissolved organic matter (DOM) in sludge., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

Phosphorus is enriched in waste activated sludge (WAS) during wastewater treatment, and organic phosphorus (OP) is a potential slow-release P fertilizer. The chemical coagulants used in sludge dewatering leave numerous residues in WAS that affect sludge composting. In this study, the effects of polyaluminum chloride (PAC) and polyferric sulfate (PFS) on the bioconversion of dissolved OP (DOP) during sludge composting were investigated. The results revealed that PFS conditioning promoted the transformation and bioavailability of DOP, whereas PAC conditioning inhibited. Results indicated that PFS conditioning enhanced the transformation of OP molecules in the thermophilic phase. Through oxidation and dehydrogenation reactions, 1-hydroxy-pentane-3,4-diol-5-phosphate and D-ribofuranose 5-phosphate with high bioactivity were generated in the PFS-conditioned compost. Enzymatic hydrolysis experiments further verified that PFS conditioning enhanced the DOP bioavailability in the compost, whereas PAC conditioning inhibited it. The study has provided molecular insights into the effects of chemical conditioning on DOP conversion during sludge composting., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

Alkali-hydrothermal treatment (AHT) of sewage sludge is often used to recover value-added dissolved organic matters (DOM) enriched with artificial humic acids (HA). Microplastics (MPs), as emerging contaminants in sewage sludge, can leach organic compounds (MP-DOM) during AHT, which potentially impact the characteristics of thermally treated sludge's DOM. This study employed spectroscopy and Fourier transform-ion cyclotron resonance mass spectrometry (FT-ICR-MS) to explore the impacts of MPs on DOM composition and transformation during AHT. The biological effects of DOM were also investigated by hydroponic experiments. The results showed that the leaching of MP-DOM led to a substantial increase in DOC content of DOM of thermally treated sludge. Conversely, the HA content significantly decreased in the presence of MPs, resulting in a decline of plant growth facilitation degree. FT-ICR-MS analysis revealed that the reduction in HA content was characterized by a notable decline in the abundance of O 6-7 and N 1-3 O 6-7 molecules. Reactomics results indicated that the leaching of MP-DOM inhibited the Maillard reaction but bolstered oxidation reactions. The inhibition of Maillard reaction, resulting in a decrease in crucial precursors (dicarbonyl compounds, ketoses, and deoxyglucosone), was responsible for the decrease of HA content. The primary mechanism responsible for inhibiting the Maillard reaction was the consumption of reactive amino reactants through two pathways. Firstly, the leaching of organic acids in MP-DOM caused decrease of sludge pH, leading to the protonation of amino groups. Secondly, the lipid-like compounds in MP-DOM underwent oxidation (-2H+O), producing fatty aldehydes that consumed the reactive amino reactants. These discoveries offer enhanced insights into the specific contribution of MPs to the composition, transformation, bioactivity of DOM during AHT process., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

Extracellular polymeric substances (EPS) are the key components determining the dewatering behavior of wastewater sludge. However, current technical optimization of sludge conditioning for dewatering is limited by the poor understanding of the conditioner-EPS interactions at molecular levels. Herein, a combination of molecular dynamic (MD) simulations, dewaterability assessment and EPS characterization was used to reveal the sludge dewatering mechanisms using dual conditioning processes (prevalent inorganic (poly aluminum chloride (PAC)) and organic (poly dimethyl diallyl ammonium chloride (PDDA)). Results suggested that PAC and PDDA bridged the biopolymers mainly through electrostatic interactions, promoting the agglomeration of biopolymers and reducing their contact probability with water molecules. Water molecules were tightly bound to EPS mainly through hydrogen bonding with polar oxygen-containing functional groups. The adsorption of PAC and PDDA on hydrophilic components reduced the molecular polarity of biopolymers and altered the conformation of water molecules in the hydration shell, resulting in a decreased hydration capacity of EPS and the release of bound water, and sludge dewaterability was improved. PAC was found to be more effective than PDDA in disrupting the hydrogen bonding between water molecules and EPS, especially the protein β-sheet structure inside the molecular clusters with its high charge strength and diffusivity. Sludge bound water decreased by 73.16 % after PAC conditioning. In addition, PDDA exhibited superior agglomeration ability to biopolymers and promoted the electrostatic interaction between PAC and polar groups during dual conditioning. The strength and hydrophobicity of EPS molecular clusters were thus enhanced, and the conditioning efficiency was improved. This study offers molecular-level insights into the coagulation treatment process of sludge and provides theoretical references for process optimization and new conditioner development., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier B.V. All rights reserved.)

Phosphorus reclamation from sewage sludge is essential for sustainable phosphorus management, as large quantities of phosphorus afflux into wastewater treatment plants and are finally enriched in sewage sludge via phosphorus removal technologies. Meanwhile, vermicomposting is a cost-effective biotechnique for sludge stabilization. This work unveiled the molecular transformation pathway and bioavailability of organic phosphorus (OP) in sludge under vermicomposting with solution 31 P NMR, FT-ICR MS and enzymatic hydrolysis assay. In conclusion, vermicomposting transformed OP in two stages. In stage I (day 0 to 14), macromolecule CHONP such as phospholipids, phosphoproteins and nucleic acid were decomposed into orthophosphate and high bioavailability OP including flavin mononucleotide, flavin mononucleotide hydrate and N6-isopentenyladenosine 5'-monophosphate under the action of earthworm intestinal flora. This resulted in the bioavailability of OP reaching a maximum of 13.58 mg/L on day 14. In stage II (day 14 to 28), the enzyme in vermicompost began to dominate the transformation of OP. Under the catalysis of phosphate, high bioavailability orthophosphate monoester was decomposed into orthophosphate. Nitrogen-containing aromatic OP polymerization produced humic acid-like OP under the catalysis of ligase. And phytic acid-like OP were produced under the catalysis of transferase. These led to the OP bioavailability decreasing to 5.60 mg/L on day 28. This work provides a new perspective on sludge phosphorus recovery and use., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier B.V. All rights reserved.)

Microplastic-derived dissolved organic matter (MP-DOM) is crucial for assessing ecological and environmental impact of microplastics. However, the factors that influence the ecological effects of MP-DOM are yet to be determined. This study investigated the influence of plastic type and leaching conditions (thermal hydrolysis, TH; hydrothermal carbonization, HTC) on the molecular properties and toxicity of MP-DOM using spectroscopy and Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS). Results revealed that plastic type was the main factor affecting the chemodiversity of MP-DOM, compared to leaching conditions. Polyamide 6 (PA6) dissolved the largest number of DOM due to the presence of heteroatoms, followed by polypropylene (PP) and polyethylene (PE). From TH to HTC processes, the molecular composition of PA-DOM remained constant, with CHNO compounds being dominant, and labile compounds (lipids-like, and protein/amino sugar-like compounds) accounting for >90 % of the total compounds. In polyolefin-sourced DOM, CHO compounds were dominant, and the relative concentration of labile compounds decreased dramatically, resulting in the higher degree of unsaturation and humification than PA-DOM. The mass difference network analysis showed that the main reaction in PA-DOM and PE-DOM was oxidation while in PP-DOM, it was the carboxylic acid reaction. However, plastic type and leaching conditions jointly influenced the toxic effects of MP-DOM. PA-DOM was bioavailable, while polyolefin-sourced DOM leached under HTC treatment exhibited toxicity, with lignin/CRAM-like compounds being the dominant toxic compounds. Notably, the 2-fold higher relative intensity of the toxic compounds and the 6-fold higher abundance of highly unsaturated and phenolic-like compounds in PP-DOM HTC resulted in the higher inhibition rate than PE-DOM HTC . Toxic molecules in PE-DOM HTC mainly directly dissolved from PE polymers, while almost 20 % of toxic molecules in PP-DOM HTC resulted from molecular transformation, where dehydration (-H 2 O) was the core reaction. These findings offer advanced insights into the management and treatment of MPs in sludge., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier B.V. All rights reserved.)

Understanding the composition, transformation and bioactivity of dissolved organic matter (DOM) at the molecular level is crucial for investigating the hydrothermal humification process of wastewater sludge and producing ecological fertilizers. In this study, DOM transformation pathways under alkali-thermal humification treatment (AHT) were characterized by Fourier transform-ion cyclotron resonance mass spectrometry (FT-ICR MS) in conjunction with molecular reaction network analysis. The effects of DOM on plant growth were examined using hydroponics and transcriptomic analysis. In the wastewater sludge humification process, AHT produced maximum amounts of protein (3260.56 mg/L) and humic acid (5788.24 mg/L) after 12 h. FT-ICR MS results indicated that protein-like structures were prone to continuous oxidation and were ultimately transformed into aromatic N-containing compounds resembling humic substances. Several reactive fragments (such as -C 2 H 2 O 2 , -C 3 H 4 O 2 , and -C 4 H 6 O 2 ) formed by the Maillard reaction (MR) were identified as potential precursors to humic acid (HA). In terms of biological effects, DOM 12h showed the highest rice germination and growth activity, whereas that produced by AHT for a longer period (> 12 h) displayed phytotoxicity owing to the accumulation of toxic substances. Plant biostimulants (such as amino acids and HAs) in DOM improved energy metabolism and carbohydrate storage in rice seedlings by upregulating the "starch and sucrose metabolism" pathways. Toxic substances (such as pyrrole, pyridine, and melanoidin) in DOM can activate cell walls formation to inhibit abiotic stimuli in rice seedlings through the biosynthesis of phenylpropanoid pathway. These findings provide a theoretical basis for optimizing sludge hydrothermal humification and recovering high-quality liquid fertilizers., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

Interactions between cations and extracellular polymeric substances (EPS) play an important role in the formation of microbial aggregates and have key effects on the physical properties of activated sludge across wastewater and sludge treatment process. Here, a molecular model of EPS cluster in activated sludge was constructed and simulated by molecular dynamics (MD) to probe the structural properties of EPS and the interaction between EPS and prevalent multivalent cations (Ca 2+ , Mg 2+ , Al 3+ ). Then the predicted changes in physical properties were validated against the dynamic light scattering, XAD resin fractionation and rheology test. The binding dynamics and interactions mechanisms between multivalent cations and EPS functional groups were further investigated using MD in combination with spectroscopic analysis. Results suggest that biopolymers are originally aggregated by electrostatic and intermolecular interactions forming dynamic clusters with negatively charged surface functional groups, which induced electrostatic repulsion preventing further agglomeration of biopolymer clusters. In the presence of multivalent cations, surface polar functional groups in biopolymers are connected, causing the rearrangement of EPS molecular conformation that forms larger and denser agglomerates. Reduced solvent accessible surface area, enhanced hydrophobicity, and increased binding free energy lead to a strong gel-like network of EPS. Ca 2+ and Al 3+ predominantly interact with functional groups in polysaccharides, promoting agglomeration of macromolecules. In contrast, Mg 2+ and Al 3+ disrupted the secondary structure of proteins, exposing hydrophobic interaction sites. Al 3+ can better agglomerate biopolymers with its higher positive charge and shorter coordination distance as compared to Ca 2+ and Mg 2+ , but compromised by the effect of hydration. This work offers a novel approach to explore the construction and molecular aggregation of EPS, enriching the theoretical basis for optimization of wastewater and sludge treatment., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

High-resolution mass spectrometry was extensively applied in molecular composition and transformation pathways of dissolved organic matter (DOM) in wastewater sludge treatments. Sample pretreatment methods and electrospray ionization (ESI) modes significant affect the accuracy of molecular characterization for DOM. This study investigated the effects of pretreatment methods (styrene divinyl benzene polymer (PPL), octadecyl (C18), and electrodialysis (ED)) on molecular characteristics of DOM in two typical wastewater sludges (waste activated sludge (WAS) and anaerobic digestion sludge (ADS)) analyzed by FT-ICR MS in both positive ESI (ESI (+)) and negative ESI (ESI (-)) modes. The results indicated that ED pretreatment exhibited the highest recovery rate of 70% ‒ 95% for sludge-derived DOM. ED and PPL performed well in recovering the different sludge-derived DOM with a high similarity of molecular characteristics (e.g., lipids, proteins/aliphatic, and lignins/CRAM-like), and the C18 method was ineffective in extracting carbohydrates, unsaturated hydrocarbons, and amino sugars. In addition, compared with single ESI (-) analysis mode, the molecular number identified by ESI (+) analysis mode was increased by 200%, especially, more unsaturated hydrocarbons and N-containing compounds were detected. Except for biogenic DOM, plenty of emerging containments (ECs) in sludge-derived DOM were identified; ESI (-) mode was more effectively in recognizing the alkyl benzene sulfonic acids (e.g., anionic surfactants); and ESI (+) mode was more effectively for plasticizers identification, for example, dioctyl terephthalate and dibutyl phthalate. This study illustrated that ED pretreatment coupled with FT-ICR MS in dual ESI modes could give more insights in complexed molecular information for DOM in wastewater sludge, and provides a theoretical basis for subsequent sludge treatments and disposals., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

Recovering high-value biomaterials from anaerobic digestion sludge (ADS) has attracted considerable attention. However, the molecular features and biological effects of abundant dissolved organic matters (DOMs) in ADS are still unclear, which limits the efficient recycling and application of these bioproducts. This study investigated the molecular composition and transformation of DOMs recovered from ADS through a mild-temperature alkali-hydrothermal treatment (AHT) with ultrahigh-resolution mass spectrometry and energy spectroscopy, and the fertilizing effects of DOMs were evaluated by rice hydroponics. The results indicated that AHT processes significantly promoted the solubilization and release of DOMs from ADS, where most of DOMs molecules remained unchanged and mainly consisted of N-containing compounds with 1-3 N atoms, featuring aromatic or N-heterocyclic rings. Furthermore, AHT processes at pH of 9-10 induced the hydrolysis of partial protein-like substances in DOMs, which was accompanied by formation of heterocyclic-N compounds. Under AHT at pH of 11-12, protein-like and heterocyclic-N substances were increasingly decomposed into amino-N compounds containing 1 or 5 N atoms, while numerous oxygenated aromatic substances with phytotoxicity were degraded and removed from DOMs. Rice hydroponic test verified that ADS-derived DOMs recovered by AHT process at pH of 12 exhibited the highest bioactivity for rice growth, which was attributed to the abundance of amino compounds and humic substances. This study proposed a novel process for the recovery of high-quality liquid organic fertilizer from ADS through AHT process, which can further enrich the technical options available for the safe utilization of sludge resources., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 The Author(s). Published by Elsevier Ltd.. All rights reserved.)

Bioactive organic compounds (BOCs) contained in bio-stabilized products of waste activated sludge (WAS) have attracted considerable attention, as they can enhance the fertilizing effect of WAS in land applications. This study investigated the molecular composition and plant-growth-promoting mechanisms of various BOCs in the bio-stabilized products of WAS. After stepwise fractionation, aerobic composting sludge (ACS) and anaerobic digestion sludge (ADS) were chemically fractioned into five subcomponents, namely dissolved organic matter (DOM) (C1), weakly interacted organic matter (OM) (C2), metal-bonded OM (C3), NaOH-extracted OM (C4), and strongly interacted OM (C5), in sequence. The results showed that fatty acids and carboxylic acid (CAs) present in ACS C2 promoted plant growth and enhanced the ability of plants against stresses by upregulating pathways related to "carbohydrate metabolism," "lipid metabolism," "amino acid metabolism," and "phenylpropanoid biosynthesis." However, in ACS C4, plenty of amino acids could promote plant growth via upregulating "carbohydrate metabolism" and "amino acid metabolism" pathways. As an important precursor, aromatic amino acids inside ACS C4 also stimulated the production of indoleacetic acids. In ADS C1, amino sugar and phytohormone were the major BOCs causing the up-regulation of "carbohydrate metabolism" and AAA catabolism in "amino acid metabolism" pathways. CAs enriched in ADS C2 stimulated plant growth through "amino acid metabolism" pathway. In summary, alkali extraction can recycle a large proportion of BOCs with low environmental risk from the bio-stabilization products of WAS. The results from this study provide scientific guidance for safe and value-added resource utilization of bio-stabilization products of WAS in land applications., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 The Author(s). Published by Elsevier Ltd.. All rights reserved.)

Bio-stabilization sludge contains numerous dissolved organic matter (DOM) that could enter aquatic environments by soil leaching after sludge land use, but a clear understanding of their photochemical behavior is still lacking. In this study, we systematically investigated the photoactivity and photochemical transformation of aerobic composting sludge-derived DOM (DOM ACS ) and anaerobic digestion sludge-derived DOM (DOM ADS ) by using multispectral analysis coupled with Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS). The results indicated that DOM ACS and DOM ADS have a higher proportion of highly unsaturated and phenolic compounds (HuPh)with high DBE wa , but the different polyphenols (Polyph) abundance of them, causing the different photoactivity between them. DOM ACS had much higher apparent quantum yields (AQY) for triplet states of dissolved natural organic matter ( 3 DOM*) and hydroxyl radical (•OH) but slightly lower AQY for singlet oxygen ( 1 O 2 ) than DOM ADS under simulated sunlight conditions. As the irradiation time increased, HuPh and Polyph (associated with humic-like substances) contained in DOM ACS (DOM ADS ) decreased by 12.0% (14.1%) and 3.0% (0.2%), respectively, with concurrent decrease in average molecular weight and aromaticity moieties, resulting in more generation of aliphatic compounds. Furthermore, based on 27 types of photochemical transformation reactions, DOM ACS containing higher fractions of O 10-15 and N 1-3 O y class preferred dealkyl group and carboxylic acid reactions, whereas DOM ADS composed of more N 4 O y and S 2 O y fragments preferred oxygen addition and anmine reactions. Consequently, photochemical transformations reduced the Cd (II) ion activity in the presence of DOM ACS (DOM ADS ). This study is believed to unveil the photochemical transformation of bio-stabilization sludge-derived DOM and its impact on pollutants' fate in the aquatic environment., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022. Published by Elsevier Ltd.)

Sludge pyrolysis carbonization has shown potential to convert sludge biomass into multifunctional carbon materials. However, ecological risks of dissolved organic matters (DOMs) with obscure molecular characteristics retaining in sludge-based carbons (SBCs) have received little attention. This study investigated the impact of pyrolysis temperatures on the molecular conversion and biotoxicity effects of DOMs in SBCs. The results revealed that DOMs in SBCs 300-400 were mainly derived from depolymerization of biopolymers and the polycondensation and cyclization of small intermediate molecules, which mainly consisted of aromatic CHON compounds with 1-3 N atoms, featuring high unsaturation and molecular weights. High-temperature pyrolysis (500-800 °C) promoted the decomposition and ring-opening of aromatic CHON compounds into saturated aliphatic CHO compounds with 2-4 O atoms in SBCs 500-800 . Noteworthily, SBCs 300-400 -derived DOMs showed relatively strong biotoxicity on the growth and development of wild-type zebrafish embryos, pakchoi seeds, and Vibrio qinghaiensis Q67, which was significantly related to aromatic amines, phenols, and heterocyclic-N compounds in DOMs of SBCs 300-400 . SBCs 500-800 -derived DOMs were mainly straight-chain fatty acids and showed no observable acute biotoxicity. This study highlights the negative impact of DOMs in SBCs on the ecological environment, and provides the theoretical basis for controlling toxic byproducts in sludge pyrolysis process., (Copyright © 2021 Elsevier B.V. All rights reserved.)

Recovering high value-added resources from waste activated sludge (WAS) is a potential way for the sustainable wastewater treatment. In this study, hydrothermal treatment at 180 °C was used to simultaneously improve sludge dewaterability and recover sludge organic matters (SOMs). The recovered SOMs were subsequently employed as precursors to prepare nitrogen-doped porous carbon nanosheets via a facile stepwise synthesis method. The as-prepared optimal carbon (AP-SOM 800 ) was characterized with an ultrahigh specific surface area (3473 m 2 /g), appropriate porosity (1.77 cm 3 /g), and abundant heteroatoms (1.47% N and 7.44% O). AP-SOM 800 exhibited a high specific capacitance (409 F/g at 0.25 A/g), low resistance (0.52 Ω), and superior cyclic stability (only 9.09% loss after 10,000 cycles) in 6 M KOH aqueous electrolyte. Furthermore, AP-SOM 800 demonstrated an extraordinary adsorption capacity (1528 mg/g for methyl orange (MO) and 1265 mg/g for tetracycline (TC)) that can be maintained (˃ 1200 mg/g) over a wide range of pH conditions. Specifically, 80.97% of MO and 66.67% of TC were rapidly absorbed through AP-SOM 800 within 10 min, and 90.27% of MO and 81.24% of TC were eventually removed from wastewater after 60 min. The adsorption processes fit closely with the pseudo-second-order kinetic (R 2  > 0.999) and Langmuir models (R 2  > 0.914), revealing that the adsorption processes were dominated by a monolayer chemical adsorption reaction. This study suggests that high value-added materials can be obtained from the WAS through improving and extending the traditional sludge treatment processes, which will enrich the technical options available for future sustainable sludge treatment and disposal., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021 Elsevier B.V. All rights reserved.)

Electro-dewatering (ED) is an attractive technology for enhancing dewaterability of waste activated sludge (WAS), and the distribution and composition of EPS and secondary structure of extracellular protein in sludge has a great influence on the sludge dewaterability. Therefore, in order to optimize and regulate sludge ED process, it is necessary to study the influence of EPS components and composition on the efficiency of sludge ED. In this study, the effects of distribution and composition of EPS and the structure of extracellular proteins on the ED rates and performance were analyzed using eight sludges from different sewage treatment process. The results showed that ED rates at both electrodes were significantly negatively correlated with the concentration of soluble EPS (S-EPS) and loosely bound EPS (LB-EPS), and this correlation was gradually weakened with the in-depth structure of layered EPS structure. High concentration of S-EPS and LB-EPS decreased the initial current and the pH gradient, deteriorating the anodic oxidation and acidification, which affect the release and degradation of EPS. Additionally, the proteins secondary structure can be destroyed and transformed by anodic oxidation and acidification, which can impact the protein water-holding capacity and ED performance., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021. Published by Elsevier B.V.)

Thermal hydrolysis pretreatment (THP) is often used to improve the anaerobic digestion performance of waste activated sludge (WAS) in wastewater treatment plants (WWTPs). During the THP process, the proteins and polysaccharides in the biomass will undergo hydrolysis and Maillard reaction, producing biorefractory organic substances, such as recalcitrant dissolved organic nitrogen (rDON) and melanoidins. In this study, a series of spectroscopy methods were used to quantitatively analyze the Maillard reaction of glucose and lysine, and the interaction mechanisms of the Maillard reaction products (MRPs) and lysozyme were investigated. Results showed that the typical aromatic heterocyclic structures in MRPs, such as pyrazine and furan, were found to quench molecular fluorescence of lysozyme, resulting in an unfolding of standard protein structure and increase in lysozyme hydrophobicity. Significant loss of enzyme activity was detected during this process. Thermodynamic parameters obtained from isothermal titration calorimetry (ITC) confirmed that the interaction between MRPs and lysozyme occurred both exothermically and spontaneously. Density functional theory (DFT) calculations suggested that the molecular interactions of MRPs and protein included parallel dislocation aromatic stacking, T-shaped vertical aromatic stacking, H-bond and H-bond coupled to aromatic stacking., (Copyright © 2021. Published by Elsevier Ltd.)

Extracellular polymeric substances (EPS) are important components of activated sludge, whose content and composition have important effects on the macro-physical properties of sludge. In this study, the response of EPS in sludge to temperature (-40-200 °C) was systematically investigated using XAD resin fractionation, variable-temperature infrared spectra (VTIS) and two-dimensional correlation spectroscopy (2D-COS). The relationships between the molecular structure of EPS and the macro-physical properties (rheological property and dewatering performance) of waste activated sludge (WAS) at varying temperature were also established. During the freezing treatment, the solubilization of biopolymers and destruction of the hydrophilic functional groups (hydroxy, amino and carboxyl) resulted in the production of small organic matters, which enhanced EPS hydrophobicity and reduced electrostatic repulsion of sludge, and subsequent dewaterability improvement. For the hydrothermal treatment, the EPS transformation showed a two-stages reaction including stage I (70-120 °C) and stage II (>120 °C). Stage I (70-120 °C), a plenty of hydrophilic functional groups (hydroxy, amino and carboxyl) in EPS were exposed via the solubilization of biopolymers, which enhanced electrostatic repulsion of sludge and EPS hydrophilicity, and subsequence in deterioration of sludge dewaterability and fluidity. However, at stage II (>120 °C), the high temperature caused hydrolyzation of macromolecular organic matters in completely, in which the secondary structure of the protein was destroyed, causing the peptide chain to unfold. In addition, the reduction of α-helix and β-sheet content and intensified Maillard reaction decreased electrostatic repulsion of sludge, thus resulted in the improvement of sludge dewaterability and fluidity. This study enriched the theoretical basis of the optimal control of sludge treatment based on temperature regulation., (Copyright © 2021. Published by Elsevier Ltd.)

In this work, we employed waste activated sludge (WAS) as carbon source to prepare ultrahigh specific surface area (SSA) biopolymers-based carbons (BBCs) through alkali (KOH) treatment coupled to pyrolysis strategy. Before the pyrolysis process, the involvement of KOH made a great recovery of soluble biopolymers from WAS, resulting in highly-efficient catalytic pyrolysis. The Brunner-Emmett-Teller and pore volume of BBCs prepared at 800°C (BBC 800 ) reached the maximum at 2633.89 m 2 ·g -1 and 2.919 m 3 ·g -1 , respectively. X-ray photoelectron spectroscopy suggested that aromatic carbon in the form of C=C was the dominant fraction of C element in BBCs. The N element in BBCs were composed of pyrrolic nitrogen and pyridinic nitrogen at 700°C, while a new graphitic nitrogen appeared over 800°C. As a refractory pollutant of wastewater treatment plants, tetracycline (TC) was selected to evaluate adsorption performance of BBCs. The adsorption behavior of BBCs towards TC was conformed to the pseudo-second-order kinetic and the Langmuir models, signifying that chemisorption of monolayers was dominant in TC adsorption. The adsorption capacity of BBC 800 reached the maximum at 877.19 mg·g -1 for 90 min at 298 K. Thermodynamic analysis indicated that the adsorption process was endothermic and spontaneous. Hydrogen bonding and π-π stacking interaction were mainly responsible for TC adsorption, and interfacial diffusion was the main rate-control step in adsorption process. The presence of soluble microbial products (SMPs) enhanced TC removal. This work provided a novel strategy to prepare bio-carbon with ultrahigh SSA using WAS for highly-efficient removal of organic pollutants., (Copyright © 2021. Published by Elsevier B.V.)

In this study, the molecular transformation of sludge biopolymers during hydrothermal treatment with the temperature ranging from 25 °C to 200 °C was examined and was seen to significantly affect the macrophysical properties (dewaterability and rheological property) of sludge. The results showed that the sludge dewaterability and flow ability under high shear stress deteriorated by a hydrothermal process at 25 °C to 120 °C, but the deterioration alleviated above the temperature threshold of 120 °C. The consistence of changes in sludge dewaterability and rheological property in HT process was mainly attributed to the variation in gel properties of soluble biopolymer. Two-stage changes in biopolymer transformation were identified, beginning with a solubilization stage from 25 °C to 120 °C in which a biopolymer with a gel-like network structure was released into liquid phase, creating flow resistance under high shear stress such that sludge dewaterability deteriorated. The second stage was identified as a conversion stage (120 °C-200 °C) in which proteins and polysaccharides hydrolyzed and experienced a Maillard reaction, leading to the degradation of the biopolymer network structure. The newly formed recalcitrant Maillard products showed weak flow response to high shear stress, allowing for an improvement in sludge dewaterability. The pathways of a Maillard reaction were identified via gas chromatography-mass spectrometer (GC-MS), 1 H nuclear magnetic resonance spectroscopy ( 1 H NMR) and two-dimensional correlation spectral analysis (2D-COS) of Fourier-transform infrared spectrometer (FTIR), etc. Three-dimensional excitation-emission matrix (3D-EEM) proved to be an applicable method for tracking Maillard reaction in sludge hydrothermal process due to the distinctive fluorescence characteristics of Maillard products. This study further clarifies the obscure process of sludge hydrothermal treatment and will help improve the accuracy of subsequent research., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021 Elsevier B.V. All rights reserved.)

Organic polymeric flocculants are commonly used in improving dredged sludge dewaterability, but less attention has been paid to residual water quality. In this paper, the effects of cationic etherified starch (CS) and poly-dimethyl diallyl ammonium chloride (PDDA) on dredged sludge dewatering efficiency and residual water quality of Baiyangdian lake were comprehensively investigated and evaluated by analytic hierarchy process (AHP). The results indicated that PDDA had stronger electrical effect and flocculation performance compared with CS, resulting in more efficient dewatering performance. PDDA can reduce the pollutants of discharged residual water, while CS significantly promoted the increase of NH 4 + -N and NO 3 - -N in the residual water. The increase of NH 4 + -N in the residual water of CS was due to the release of dredged sludge, while the increase of NO 3 - -N was introduced by CS leaching. AHP showed that PDDA performed better in flocculation treatment of dredged sludge than other organic polymers. This work provides a method for optimization of flocculation treatment for dredged sludge dewaterability., (Copyright © 2020. Published by Elsevier B.V.)

In this work, a novel carbon-based hydrotalcite-like compounds materials (LDO-SBCs) were prepared by coupling layered double hydroxides (LDHs) conditioning and pyrolytic carbonization, and characterized by X-ray diffraction (XRD), Thermogravimetric Analyzer (TGA), X-ray photoelectron spectroscopy (XPS) and Brunner-Emmet-Teller (BET) measurements. The synthesized LDO-SBCs composites were used in wastewater treatment for simultaneous removal of phosphate and dissolved organic matter (DOM). The adsorption of DOM and phosphate were well conformed to pseudo-second-order mode. Adsorption equilibrium was better fitted by Langmuir model for phosphate, while Freundlich model for DOM. Compared with the raw sludge carbon, the removal efficiency of DOM and phosphate by LDO-SBCs were increased by 8% and 13%, respectively. Based on the fluorescence spectrum and parallel factor analysis (PARAFAC), LDO-SBCs performed well in promoting the removal of protein substances (TPN and APN). Pore filling, hydrogen bonding, electrostatic adsorption and surface complexation might be dominant in the adsorption of DOM, while, surface complexation and ion exchange between the LDO layers were mainly responsible for the adsorption of phosphate. The difference of adsorption capacity of LDO-SBCs was related to the superior channel structure of composite materials and the composition of interlayer anions of LDO., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020. Published by Elsevier Ltd.)

In previous studies, we interestingly found that several ligands (e.g., nitrilotriacetate and humic acid) could significantly accelerate the oxidation of NaClO by ferrous ion, via complexing with Fe(II). This inspired us to hypothesis that organic acids (OA) chelated Fe(II) might enhance the NaClO oxidation for improving sludge dewaterability. In this work, the OA chelated ferrous ions activated NaClO (OA-Fe(II)-NaClO) process was utilized for sludge conditioning, which exhibited significantly improved dewatering performance, as evidenced by capillary suction time (CST), specific resistance to filtration (SRF) and cake moisture of sludge. The normalized CST (CSTn) and SRF decreased to 1.22 s × L/g and 3.24 × 10 8  m/kg, when ratio dosage of [ClO - ]/[Fe 2+ ] (NaClO: 0.75%(v/v)) was 1 at pH of 2. During the NaClO activation by Fe(II), tightly bound extracellular polymeric substances (TB-EPS) was cracked into soluble EPS (S-EPS), followed by oxidizing into smaller molecular organic matters due to the production of hydroxyl radicals. Meanwhile, OA complexed to ferrous ion inhibited hydrolysis of ferric ions, leading to better catalytic performance of NaClO under neutral pH conditions. In addition, the molecular structure of OA determined the low complexing ability and steric hindrance for OA-Fe(II). When molar ratio of [Oxalic acid]/[Fe 2+ ] was 1, oxalic acid-Fe(II)-NaClO improved sludge dewaterability significantly due to the coagulation and skeleton builder properties of formed iron oxalate precipitates. This work provides an eco-friendly and cost-effective method for improving sludge dewaterability., (Copyright © 2020 Elsevier Ltd. All rights reserved.)

Extracellular polymeric substances (EPS) form a stable gel-like structure to combine with water molecules through steric hindrance, making the mechanical dewatering of wastewater sludge considerably difficult. Coagulation/flocculation has been widely applied in improving the sludge dewatering performance, while sludge properties (organic fraction and solution chemistry conditions) are highly changeable and have important effects on sludge flocculation process. In this work, the alkalinity effects on sludge conditioning with hydroxy-aluminum were comprehensively investigated, and the interaction mechanisms between EPS and hydroxy-aluminum with different speciation were unraveled. The results showed that the effectiveness of hydroxy-aluminum conditioning gradually deteriorated with increase in alkalinity. Meanwhile, the polymeric hydroxy-aluminum (Al 13 ) and highly polymerized hydroxy-aluminum (Al 30 ) were hydrolysed and converted into amorphous aluminum hydroxide (Al(OH) 3 ), which changed the flocculation mechanism from charge neutralization and complexing adsorption to hydrogen bond interaction. Additionally, both Al 13 and Al 30 showed higher binding capacity for proteins and polysaccharides in EPS than monomeric aluminum and Al(OH) 3 . Al 13 and Al 30 coagulation changed the secondary structure of proteins in EPS, which caused a gelation reaction to increase molecular hydrophobicity of proteins and consequently sludge dewaterability. This study provided a guidance for optimizing the hydroxy-aluminum flocculation conditioning of sludge with high solution alkalinity., (Copyright © 2020. Published by Elsevier B.V.)

The bound water in waste activated sludge (WAS) is trapped in extracellular polymeric substances (EPS) in the form of gel-like structure, leading to a great challenge in the sludge deep dewatering. Traditional flocculation conditioning is unable to destroy EPS and ineffective to remove the bound water in WAS. In this study, we employed integration of Fe(II)-sulfite oxidation and polyacrylamide flocculation (F/S-PAM) treatment for removing the bound water and improving sludge dewaterability under aerobic conditions. Meanwhile, the floc microstructure and EPS properties were examined to understand the mechanisms of F/S-PAM conditioning. F/S produced SO 3 ·- radicals which could decompose the EPS in sludge, releasing bound water into free water. In addition, the formed Fe(III) from F/S led to re-coagulation of decomposed EPS, and C=O groups of tryptophan played the leading role in Fe-EPS association binding, causing transformation of the secondary structure of proteins (especially β-sheets and α-helices). Then, the introduction of PAM caused re-flocculation of disintegrated sludge flocs, enhancing the sludge filterability. This work provides a novel and cost-effective method for efficient removal of bound water in sludge, and subsequence improvement in sludge dewaterability., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier Ltd. All rights reserved.)

This study aimed to explore the adsorption performance of sludge-based activated carbon (SBC) towards dissolved organic matters (DOMs) removal from sewage, and investigated the modification effect of different types of chemicals on the structure of synthesized SBC. Waste activated sludge (WAS) was used as a carbon source, and HCl, HNO 3 , and NaOH were used as different types of chemicals to modify the SBC. With the aid of chemical activation, the modified SBC showed higher adsorption performances on DOMs removal with maximum adsorption of 29.05 mg/g and second-order constant (k) of 0.1367 (L/mol/sec) due to the surface elution of ash and minerals by chemicals. The surface elemental composition of MSBC suggested that the content of C-C and C-O functional groups on the surface of modified sludge-based activated carbon (MSBC) played an important role on the adsorption capacities of MSBC towards DOMs removal in sewage. Additionally, the residual molecular weight of DOMs in sewage was investigated using a 3-dimension fluorescence excitation-emission matrix (3D-EEM) and high-performance size exclusion chromatography (HP-SEC). Results showed that the chemical modification significantly improved the adsorption capacity of MSBC on humic acids (HA) and aromatic proteins (APN), and both of NaOH-MSBC and HCl-MSBC were effective for a wide range of different AMW DOMs removal from sewage, while the HNO 3 -MSBC exhibited poorly on AMW organics of 2,617 Da and 409 Da due to the reducing content of macropore. In brief, this study provides reference values for the impact of the chemicals of the activation stage before the SBCs application., (Copyright © 2020. Published by Elsevier B.V.)

Sludge is an inevitable by product of sewage treatment, and it includes pathogens, heavy metals, organic pollutants and other toxic substances. The components of sludge are complex and variable with extracellular polymeric substances (EPS) being one. EPS are highly hydrophilic and compressible, and make sludge dewatering difficult. Therefore, the development of efficient sludge-dewatering technology is an important means of mitigating rapid sludge growth. At present, the main methods used for sludge deep-dewatering technology are chemical preconditioning with high-pressure filtration and electrical mechanical dewatering. The selection of chemical preconditioning directly determines the final efficiency of the sludge-dewatering process. In this paper, we conduct a comprehensive review of the problems related to sludge dewatering and systematically summarise the impact of different chemical conditioning technologies on the efficiency of sludge dewatering. Furthermore, the characteristics of different enhanced dewatering technologies are evaluated and analysed for their adaptability and final disposal methods. We believe that this review can clarify the chemical conditioner mechanism to improve sludge dewatering, provide reference debugging information for the sludge-dewatering process and promote the development of efficient and environmentally friendly sludge-dewatering technology., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier Ltd. All rights reserved.)

The work evaluated the influence of different operating conditions (voltage, ionic strength and mechanical pressure) on algae electro-osmotic dewatering effect and extracellular organic matter (EOM) regionalization. It was found that the algae electro-dewatering effect became better as the voltage and ionic strength increased, but electro-dewatering effect was decreased when ionic strength was more than 0.006gNaCl/gTSS, this indicated that too high ionic strength will reduce algae electro-dewatering effect. In addition, electro-osmosis effect first increases and then weakens when the pressure was increased. The content of dissolved organic materials (DOM) in the filtrate of both electrodes was increased when the voltage and ionic strength enhanced, the DOM content of filtrate at cathode and anode were increased from 42.9 mg/L, 36.7 mg/L to 68.2 mg/L, 85.3 mg/L when ionic strength raised from 0gNaCl/gTSS to 0.01gNaCl/gTSS, this indicated that a large amount of EOM dissolution as the voltage and ionic strength increased. The DOM content of both electrodes did not change significantly when mechanical pressure changed, anodic oxidation can oxidize and decompose macromolecular weight substances into mid-molecular weight and low molecular weight substances., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020. Published by Elsevier Ltd.)

Extracellular polymeric substances (EPS) in wastewater sludge form a network structure that is highly hydrophilic and compressible. Thus chemical conditioning is always required to improve sludge dewaterability by changing the gelatinous structure of sludge flocs. Layered double hydroxides (LDH) are generally characterized by large surface area and high anion exchange capacity, so we prepared three types of hydrotalcite-like compounds (Ca/Mg/Al-LDHs) from a typical solid waste, blast furnace slag, using NaOH precipitation (giving LDH a ), a hydrothermal method (LDH b ), and NaOH-Na 2 CO 3 precipitation (LDH c ). The physicochemical properties of the three LDH were comprehensively characterized, and their effectiveness as sludge conditioners was evaluated. The results showed that LDH conditioning was able to promote sludge dewaterability, and conditioning efficiency was strongly dependent on LDH structural properties. LDH neutralized the negative charges onto sludge particles and interacted with EPS to increase floc strength. LDH also formed a skeletal structure that reduced sludge compressibility. In addition, there were interactions between the LDH surfaces and the OC-OH in EPS proteins, which altered the secondary structure of protein molecules, consequently increasing sludge dewaterability. The biomolecules of low-molecular-weight fractions (such as peptides and humic acids) in soluble EPS intercalated LDH. Both the surface complexation of organic matter containing carboxyl groups and the intercalation of small molecules in soluble EPS were responsible for EPS-LDH interactions. The combination of skeleton formation, electrostatic interaction, and EPS-LDH interactions resulted in compression of gel-like structure and improved sludge dewatering performance. We finally suggested a novel sludge treatment process that increases sludge dewaterability using slag-derived Ca/Mg/Al-LDH to condition the sludge, and it could be combined with pyrolysis to prepare multi-functional materials or bio-oil., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

Anaerobically digested sludge is generally difficult to dewater due to the release of sticky soluble microbial products in anaerobic digestion. Traditional flocculation processes have the disadvantages of high chemical dosing and solid increase, thus affecting subsequent land application. Therefore, it is desirable to develop low-cost, biodegradable, nontoxic and environmentally friendly sludge conditioners. In this work, the chitosan (CTS) was chemically modified by incorporating functional groups (amino group and the carboxyl group) to improve its water solubility and flocculation efficiency, and the anaerobically digested sludge conditioning effectiveness of different chitosan based flocculants were comparatively investigated. Results indicated that aminated chitosan (CTS-DMDAAC) and CTS performed well in sludge dewatering improvement in terms of specific resistance to filtration (SRF) and Capillary suction time (CST), which decreased to a minimum when the concentration of conditioner reached to 35 mg/g TSS. Flocs conditioned by CTS-DMDAAC were more compact and aggregated more efficiently than that flocculated with CTS and C-CTS (carboxylated chitosan). CTS-DMDAAC and CTS interacted with extracellular polymeric substance (EPS) by charge neutralization and complexation adsorption, which caused the densification of gel-like structure and enhancement of floc strength of sludge. Scanning electron microscope (SEM) analysis showed that after CTS-DMDAAC treatment, there were plentiful large pores distributed on floc surface, which provided channels for water release under pressure filtration. Confocal laser scanning microscopy (CLSM) confirmed that protein-like substances were agglomerated under flocculation conditioning, which was responsible for the promotion of sludge dewatering performance. This study provides a green and promising solution for the improvement of anaerobically digested sludge dewatering performance., (Copyright © 2019 Elsevier B.V. All rights reserved.)

The effects of typical sludge properties (solids concentration, soluble extracellular polymeric substances (SEPS) and alkalinity) on waste activated sludge flocculation-dewatering behavior and mechanisms under chemical conditioning with inorganic polymer flocculant-polyaluminum chloride (PACl) were systematically examined in this study. The results indicated that increasing the solids concentration was conductive to sludge dewatering and could greatly decrease the PACl demand in chemical conditioning. Solids concentration had important effects on properties of sludge floc flocculated with PACl, floc structure was more compact and of low EPS concentration at high solids concentrations. High levels of SEPS were adverse to sludge dewaterability after flocculation with PACl, since the SEPS could interact with hydroxy-aluminium through complexation and increase the demand of coagulants. In addition, advantageous speciations of hydroxy-aluminium were rapidly converted into amorphous hydroxides with low flocculation activity at high alkalinity, so the sludge conditioning efficiency was greatly declined. At the same time, the dominant mechanism of chemical conditioning was changed from charge neutralization to sweep coagulation. Finally, this study provides control strategies at complex sludge properties for improving the effectiveness of PACl as a chemical conditioner., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

Sludge treatment and disposal have become critical environmental issues in China. Electro-dewatering (ED) is an attractive technology for enhancing dewaterability and improving the sustainability of waste activated sludge (WAS) handling. However, electrically assisted mechanical dewatering processes consume more energy and the extracellular polymeric substance (EPS) dissolution caused by electrochemical reactions can lead to clogging of the filter cloth. Carbon-based materials (CBMs) such as activated carbon and graphite have electrical conductivity and well-developed pore structures which can adsorb the biopolymers. Therefore, addition of CBMs is expected to improve WAS electro-dewatering performance for fuel treatment by enhancing sludge conductivity and filterability. In this study, we evaluated the effects of the three carbon materials (AC-0, AC-5, and graphite) on sludge electro-dewatering behavior and the flammability of sludge cakes. The results showed that CBMs promote the performance of WAS electro-dewatering, and the promoting effect of the carbon materials on the sludge electro-dewatering is proportional to the electrical conductivity of the carbon material, and carbon materials can increase the electrophoretic mobility of sludge flocs and the electro-osmotic effect. Moreover, CBMs can adsorb the dissolved EPS, thus alleviate the plugging and filtration resistance of the filter medium. The addition of CBMs also decreases the energy consumption for water removal during the electro-dewatering process and improves the calorific value and sustainable combustion time of the sludge cake. Our approach can facilitate the resource utilization of the dewatered sludge cake in electro-dewatering processes., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

Anaerobic digestion (AD) has been widely used in sludge treatment for biogas recovery, organic fraction stabilization, and sludge reduction. However, after AD, sludge filterability is extremely deteriorated due to the release of biopolymers and the formation of fine particles. AD sludge is generally rich in nutrients, mainly ammonium nitrogen and phosphates, that result from biopolymer degradation. We designed a conditioning process that combines the in-situ crystallization of magnesium ammonium phosphate (MAP), as a skeleton builder, with organic polymer flocculation. We show that crystallized MAP can bind with extracellular polymeric substance fractions to increase sludge floc density. The molecular structure and electrical charge of organic polymers importantly influence sludge particle flocculation and aggregation. We found that cationic polyacrylamides form flocs that aggregate with branching structures which are characterized by a larger size and a more compact structure. Simultaneous crystallization and flocculation produced by a magnesium-organic polymer gel improved AD dewaterability more than the separate addition of magnesium ions and organic polymers. The method of sludge conditioning that we propose was tested by extensive use in different AD sludge conditioning protocols. The method reduces the ammonium nitrogen load in AD liquor and increases the suitability of the biosolids for use as land fertilizer., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

Proteins are the dominant organic component of extracellular polymeric substances (EPS) in waste activated sludge (WAS), and play an important role during sludge dewatering processes. Methanol is a polar hydrophilic reagent and can denature proteins, which suggested to us that the modification of protein configurations with methanol could improve sludge dewatering performance. In this study, methanol was used to precondition WAS prior to adding inorganic coagulants for dewatering enhancement. The morphology and EPS properties (especially of proteins) were investigated to analyze and explain the effects of methanol in the sludge conditioning process. The results show that methanol performed much better than traditional inorganic coagulants in improving sludge dewaterability in term of specific resistance to filtration (SRF) and cake solid content (CSC). Extractable proteins in EPS increased to a maximum when the concentration of methanol reached 40% (w/w) because cell membranes were destroyed and intracellular substances and water were released. Floc protein content was reduced with the further increase in methanol concentration due to protein precipitation. Confocal laser scanning microscopy analysis indicated that proteins precipitated and formed larger aggregates because methanol destroyed both the hydration shell and the hydrophobic clusters of proteins and expanded the protein tertiary structure to release interstitial water and bound water. The combination treatment of methanol and inorganic coagulants (PAC or FeCl 3 ) showed significant synergetic effects on enhancing sludge dewatering and cake drying. In practical applications, methanol from the dewatering sludge can be returned to the biochemical pool and used as the carbon source for nitrogen removal in the denitrification process. This integrated process is appropriate for sludge final disposal technologies that have high energy demands, such as incineration and pyrolysis. This paper describes a novel approach to improving sludge dewaterability through the alteration of protein properties by use of physiochemical techniques., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

Sludge treatment and disposal have become important environmental issues in China. Mechanical dewatering is widely used to reduce the amount of sludge to be disposed and relieve the rapid growth pressure of waste sludge. In comparison to traditional sludge dewatering processes, pressure electro-osmotic dewatering has many advantages on sludge dewatering efficiency, low conditioner dosage and concentrated cake are both beneficial to further recycling of waste sludge. In general, complex electrochemical effects (eg. electrochemical oxidation, ohmic heating and pH gradient effect) are accompanied by the pressure electro-osmotic dewatering process. These electrochemical effects will inevitably cause solubilization and/or degradation of key constituents of wastewater sludge - extracellular polymeric substances (EPS). In this study, the effects of voltage, pH and ionic strength on sludge electro-osmotic dewatering performance and electrochemical effects were investigated. The solubilization and degradation of EPS were analyzed by examining the variation of dissolved organic matter (DOM) in the filtrate, and the relationships between microstructural properties of sludge cake and DOM and electro-osmosis dewatering performance in electro-dewatering process was examined. It was found that electro-dewatering properties were improved by raising the operating voltage or decreasing the pH value, while dewatering rate initially increased at low ionic strength it decreases with increased ionic strength. In addition, the porous structure of cathodic cake was more plentiful than that at the anode. At the cathode, the EPS dissolution was mainly related to alkalization, while the oxidation and acidification were responsible for release of EPS at the anode. Meanwhile, electrophoresis effect was able to promote migration of EPS toward the anode. The average electro-osmotic dewatering rate at the anode (R 2 .>0.79, p < 0.02) and at the cathode (R 2 .>0.87, p < 0.03) strongly correlated with the volume of pore of sludge cake. There was no correlation between the total content of anodic DOM (R 2 <0.31, p>0.08) and electro-osmotic dewatering rate at the anode, however, the content of cathodic DOM (R 2  > 0.62, p < 0.09) negatively correlated with average electro-osmosis dewatering rate of cathode. Since cathode is the main water-permeable side in sludge electro-dewatering, and the sticky biopolymers (proteins and humic subtances) could not be converted into small molecules, higher EPS release was associated with worse sludge filterability. As for the anode, the biopolymers were degraded into small molecules due to electrochemical oxidation, which greatly reduced the impact of DOM on dewatering effect. Therefore, the operating conditions (voltage, pH and ionic strength) caused changes in electrochemical effects, which played a crucial role in compartmentalization of sludge EPS dissolution and consequently sludge electro-dewatering behavior., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

In this study, the effects of chemical conditioning using titanium salt coagulants (TSCs) of different hydrolysis speciation in combination with magnetic nano-particles on dewatering performance of waste activated sludge were evaluated by means of specific resistance to filtration (SRF) and capillary suction time (CST). The morphological and extracellular polymeric substances (EPS) properties under chemical conditioning were investigated in detail to understand the reaction mechanisms involved. The results showed that the TSC with basicity of 0.5 performed better in improving sludge dewatering performance than other TSCs. Sludge floc formed by TSC 0.5 treatment was characterized by larger floc size and higher floc strength than that conditioned by other TSCs. EPS compression and densification were the major mechanisms of sludge conditioning, and TSC 0.5 had better performance in compressing EPS structure. In addition, reduction of soluble EPS concentration, especially protein-like substances contributed to improvement of sludge filterability under conditioning. Furthermore, addition of Fe 2 O 3 nanoparticles could further improve dewatering performance and decrease compressibility of sludge system by acting as skeleton builders and enhancing floc strength. The sludge particles aggregation efficiency was effectively improved with addition of nano-Fe 2 O 3 . They also were able to bind with protein-like substance in EPS component, which might contribute to promotion of sludge filterability., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

Chemical conditioning is one of the most important processes for improve the performance of sludge dewatering device. Aluminum salt coagulant has been widely used in wastewater and sludge treatment. It is generally accepted that pre-formed speciation of aluminum salt coagulants (ASC) has an important influence on coagulation/flocculation performance. In this study, the interaction mechanisms between sludge particles and aluminum salt coagulants with different speciation of hydroxy aluminum were investigated by characterizing the changes in morphological and EPS properties. It was found that middle polymer state aluminum (Al b ) and high polymer state aluminum (Al c ) performed better than monomer aluminum and oligomeric state aluminum (Al a ) in reduction of specific resistance to filtration (SRF) and compressibility of wastewater sludge due to their higher charge neutralization and formed more compact flocs. Sludge was significantly acidified after addition Al a , while pH was much more stable under Al b and Al c conditioning due to their hydrolysis stability. The size of sludge flocs conditioned with Al b and Al c was small but flocs structure was denser and more compact, and floc strength is higher, while that formed from Al a is relatively large, but floc structure was loose, floc strength is relatively lower. Scanning environmental microscope analysis revealed that sludge flocs conditioned by Al b and Al c (especially PAC 2.5 and Al 13 ) exhibited obvious botryoidal structure, this is because sludge flocs formed by Al b and Al c were more compact and floc strength is high, it was easy generated plentiful tiny channels for water release. In addition, polymeric aluminum salt coagulant (Al b , Al c ) had better performance in compressing extracellular polymeric substances (EPS) structure and removing sticky protein-like substances from soluble EPS fraction, contributing to improvement of sludge filtration performance. Therefore, this study provides a novel solution for improving sludge dewatering property by controlling aluminum speciation., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

The effects of combined calcium peroxide (CaO2) oxidation with chemical re-flocculation on dewatering performance and physicochemical properties of waste activated sludge was investigated in this study. The evolutions of extracellular polymeric substances (EPS) distribution, composition and morphological properties were analyzed to unravel the sludge conditioning mechanism. It was found that sludge filtration performance was enhanced by calcium peroxide oxidation with the optimal dosage of 20 mg/gTSS. However, this enhancement was not observed at lower dosages due to the absence of oxidation and the performance deteriorated at higher dosages because of the release of excess EPS, mainly as protein-like substances. The variation in soluble EPS (SEPS) component can be fitted well with pseudo-zero-order kinetic model under CaO2 treatment. At the same time, extractable EPS content (SEPS and loosely bound EPS (LB-EPS)) were dramatically increased, indicating sludge flocs were effectively broken and their structure became looser after CaO2 addition. The sludge floc structure was reconstructed and sludge dewaterability was significantly enhanced using chemical re-flocculation (polyaluminium chloride (PACl), ferric iron (FeCl3) and polyacrylamide (PAM)). The inorganic coagulants performed better in improving sludge filtration dewatering performance and reducing cake moisture content than organic polymer, since they could act as skeleton builders and decrease the sludge compressibility., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

Extracellular polymeric substances (EPS) are highly hydrated biopolymers and play important roles in bioflocculation, floc stability, and solid-water separation processes. Destroying EPS structure will result in sludge reduction and release of trapped water. In this study, the effects of combined process of peracetic acid (PAA) pre-oxidation and chemical re-flocculation on morphological properties and distribution and composition of EPS of the resultant sludge flocs were investigated in detail to gain insights into the mechanism involved in sludge treatment. It was found that sludge particles were effectively solubilized and protein-like substances were degraded into small molecules after PAA oxidation. A higher degradation of protein-like substances was observed at acid environments under PAA oxidation. Microscopic analysis revealed that no integral sludge floc was observed after oxidation with PAA at high doses. The floc was reconstructed with addition of inorganic coagulants (polyaluminium chloride (PACl) and ferric chloride (FeCl3)) and PACl performed better in flocculation due to its higher charge neutralization and bridging ability. Combined oxidative lysis and chemical re-flocculation provide a novel solution for sludge treatment., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

The feasibility of combined process of composite enzymatic treatment and chemical flocculation with inorganic salt coagulants was investigated in this study. The evolution of extracellular polymeric substances (EPS) distribution, composition and morphological properties were analyzed to unravel the sludge conditioning mechanism. It was found that sludge filtration performance was deteriorated due to release of a large amount of biopolymers after enzymatic treatment. The change in EPS followed the pseudo-first-order kinetic equation well under enzymatic treatment. The feeding modes of enzymes had a significant influence on sludge lysis efficiency under compound enzymes treatment. Alpha amylase + protease was more effective in solubilization than other two addition modes (protease + α-amylase or simultaneous addition). The sludge floc re-formed and macromolecule biopolymers were effectively removed through coagulation process. At the same time, both of filtration rate and cake solid content of sludge treated with enzymes were improved with increasing dosage of coagulants, and ferric iron (FeCl3) had better performance in sludge dewaterability enhancement than polyaluminium chloride (PACl). In addition, sludge filtration property was slightly deteriorated, while the cake moisture reduction was favored at the optimal dosage of inorganic coagulants., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

Digested sludges generally exhibit poorer dewaterability than activated sludges. This study investigated the effects of acidification and oxidation on EPS properties and dewaterability of anaerobic digested sludge in Fenton treatment in order to unravel the underlying mechanism of sludge conditioning. The results indicated that sludge dewatering property was improved after acidification treatment. Meanwhile, fluorescence analysis revealed that the protein-like substances were effectively removed from sludge bulk after acidification treatment. Acidification and Fenton oxidation showed a significant synergetic effect in enhancing sludge dewatering process. Solubilization and decomposition of bound EPS occurred synchronously during Fenton conditioning. Oxidation process is very likely to play a more important role in sludge conditioning than Fenton coagulation. According to pilot test, Fenton treatment performed much better in cake moisture content reduction than chemical conditioning with traditional inorganic coagulants. Additionally, full-scale application of Fenton conditioning will not have detrimental effects on performance of wastewater treatment system., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

This study investigated the effects of chemical conditioning with three representative inorganic coagulants (FeCl3, polyaluminum chloride (PACl) and high performance PACl (HPAC) on sludge dewaterability. We monitored the particle size, kinetic viscosity (KV), fractal dimension (D(F)) and extracellular polymeric substances (EPS) located in different layers of sludge floc (soluble, loosely-bound (LB), tightly-bound (TB)) to understand the correlation of dewaterability and physicochemical properties of sludge under chemical conditioning. The conditioning process included the rapid aggregation of sludge particles induced by charge neutralization and bridging followed by floc densification caused by double electric layer compression. The floc size and D(F) were increased after chemical conditioning, indicating that larger and more compact floc formed. The floc conditioned with FeCl3 was smaller but denser than that of PACl and HPAC. Furthermore, sludge dewaterability correlated well with the change in concentration of soluble EPS, LB-EPS and TB-EPS, but not with KV, D(F), floc size., (Copyright © 2013. Published by Elsevier Ltd.)

Thefeasibility of reusing hypersaline wastewater containing ahigh concentration of organic contaminants by a combined process ofpowdered activated carbon (PAC) adsorption and Fenton oxidation wasinvestigated in this study. Operating conditions of the integratedprocess were optimized by jar tests. According to the results of molecularweight (MW) and full wavelength scanning analysis, most of the aromaticcompounds with high MW (>1000 Da) were removed after adsorptionpretreatment,but the effects of PAC adsorption on hydrophilic organic pollutantsof low MW were rather limited. The adsorption followed a pseudo-second-orderkinetic equation. Additionally, the strategy for maximizing the efficiencyof both H2O2and organic removal in saline wastewaterwas proposed. The Fenton efficiency was strongly dependent on bothreaction conditions and feeding modes of reagents. Organic removalwas significantly enhanced by slowing down the feeding rate of Fenton’sreagents. Moreover, rapid acidification of the wastewater was observedafter adding a small amount of Fenton’s reagents, and the H2O2dosage required for achieving a sufficient organicremoval (effluent total organic carbon (TOC) < 200 mg/L) decreasedby 22.2% with pH 3.0 maintained throughout oxidation process. Underthe optimal oxidation conditions (reaction temperature = 80–90°C, pH = 3, Fe2+/H2O2molarratio = 0.03), overall TOC removal efficiency of the integrated processwas more than 95% of which 30% corresponds to the adsorption of PACand 65% to the Fenton oxidation process. Furthermore, a pilot testindicated that the final effluent of the integrated process couldconform to the standard for saline water recycle, confirming thatthis process provided a more economical and feasible alternative forreusing the hypersaline water contaminated with a high concentrationof organic compounds. [ABSTRACT FROM AUTHOR]