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Anoxic ammonium oxidation (anammox) is an energy-efficient nitrogen removal process for wastewater treatment. However, the unstable nitrite supply and residual nitrate in the anammox process have limited its wide application. Recent studies have proven coupling of sulfur-based denitrification with anammox (SDA) can achieve an effective nitrogen removal, owing to stable provision of substrate nitrite from the sulfur-based denitrification, thus making its process control more efficient in comparison with that of partial nitrification and anammox process. Meanwhile, the anammox-produced nitrate can be eliminated through sulfur-based denitrification, thereby enhancing SDA's overall nitrogen removal efficiency. Nonetheless, this process is governed by a complex microbial system that involves both complicated sulfur and nitrogen metabolisms as well as multiple interactions among sulfur-oxidising bacteria and anammox bacteria. A comprehensive understanding of the principles of the SDA process is the key to facilitating the development and application of this novel process. Hence, this review is conducted to systematically summarise various findings on the SDA process, including its associated biochemistry, biokinetic reactions, reactor performance, and application. The dominant functional bacteria and microbial interactions in the SDA process are further discussed. Finally, the advantages, challenges, and future research perspectives of SDA are outlined. Overall, this work gives an in-depth insight into the coupling mechanism of SDA and its potential application in biological nitrogen removal.

Endevours on the enhancement of nitrate removal efficiency during methane oxidation coupled with denitrification (AME-D) has always overlooked the role of membrane employed. It would be highly beneficial to enrich the biomass content and to manage biofilm on the membrane, in the utilization of methane and denitrification. In this study, an innovative and scalable double-layer membrane (DLM) was designed and prepared for a membrane biofilm reactor (MBfR), to simultaneously enhance nitrate removal flux and methane utilization efficiency during aerobic methane oxidation coupled with the denitrification (AME-D) process. The DLM allowed quick bacterial attachment and biomass accumulation for biofilm growth, which would be then self-regulated for well distribution of functional microbes on/within the DLM. Upon a high biofilm density of over 70 g-VSS m−2 achieved on the DLM, the methane utilization efficiency of the MBfR was enhanced significantly to over 1.3 times than the control MBfR with conventional polypropylene membrane. The MBfR employed DLM also demonstrated the maximum nitrate removal flux of 740 mg-NO3−-N m−2 d−1 that was approximately 1.64 times of that in control MBfR at continuous-mode operation. This DLM indeed favored the enrichment of Type II aerobic methanotrophs of Methylocystaceae, and methanol-utilization denitrifiers of Rhodocyclaceae that preferentially utilize methanol as the cross-feeding intermediates to promote the methane utilization efficiency, and thus to enhance the nitrate removal flux. These results raised from new designed DLM confirmed the importance of membrane surface properties on the effectiveness of MBfR, and offered great potential to address challenging problems of MBfRs during engineering application.

Solar irradiation of chlorine-containing waters enhances inactivation of chlorine-resistant pathogens (e.g., Cryptosporidium oocysts), through in situ formation of ozone, hydroxyl radical, and other reactive species during photolysis of free available chlorine (FAC) at UVB-UVA wavelengths of solar light (290–400 nm). However, corresponding effects on regulated disinfection byproduct (DBP) formation and associated dissolved organic matter (DOM) properties remain unclear. In this work, when compared to dark chlorination, sunlight-driven FAC photolysis over a range of conditions was found to yield higher DBP levels, depletion of DOM chromophores and fluorophores, preferential removal of phenolic groups versus carboxylic acid groups, and degradation of larger humic substances to smaller molecular weight compounds. Control experiments showed that increased DBP levels were not due to direct DOM photolysis and subsequent dark reactions with FAC, but to co-exposure of DOM to FAC and reactive species (e.g., O3, HO•, Cl•, Cl2•-, ClO•) generated by FAC photolysis. Because solar chlorine photolysis can enable inactivation of chlorine-resistant pathogens at far lower CTFAC values than chlorination alone, the increases in DBP formation inherent to this approach can likely be offset to some extent by the ability to operate at significantly decreased CTFAC. Nonetheless, these findings demonstrate that applications of solar chlorine photolysis will require careful attention to potential impacts on DBP formation.

Dissolved organic matter (DOM) in aquatic environment significantly influences the behavior and fate of heavy metals via binding, complexation and thus changes the metal speciation; however detailed interfacial processes and mechanisms are still unclear. Here, differential absorbance and fluorescence spectra and two dimensional UV–FTIR heterospectral correlation analysis were applied to probe into the Pb(II)–DOM interaction at a wide range of pH and ionic strength (IS). The absorbance of DOM molecules under all conditions increased with metal addition, while the different extents of absorbance variations along the wavelength range in the differential zero-order and log-transformed absorbance spectra indicated the site heterogeneity within the DOM pool for metal binding. Spectral parameters, namely differential fluorescent components 1 and 2 (DFC1 and DFC2) and differential slopes of log-transformed absorbance in the range of wavelength 350–400 nm (DSlope350–400) were found to be highly correlated with the total amounts of DOM-bound Pb(II) predicted by the NICA-Donnan model, while the differential absorbance spectra at 235 nm (DA235) was related to the extent of Pb(II) bound by carboxylic groups. Thus, these parameters are an indicator or proxy for the in situ Pb(II)–DOM interaction extent. Aryl C–H gave the fastest response to Pb(II) binding at lower pH and IS (e.g., pH 4.7 and IS = 0.01 M), followed by carboxyl C=O and polysaccharide C–OH and then chromophoric groups at 265 nm (CDOM265). However, the CDOM265 bound to Pb(II) prior to aryl C–H and polysaccharide C–OH groups at higher pH and IS (6.0 and 0.1 M, respectively), showing that the binding sequences were highly dependent on solution chemistry. Differential spectra combined with two dimensional UV–FTIR heterospectral correlation analysis can be used as a promising approach to elucidate metal–DOM interaction processes, including site heterogeneity, binding sensitivity and sequence at the functional group level.

This study focused on developing surrogate indicators for predicting oxidation of phenolic groups in dissolved organic matter (DOM), suppression of halophenols' formation potential and abatement of estrogenic activity during ozonation of water and wastewater. The evolution of pH-dependent differential absorbance spectra suggests that O3 preferentially reacts with the DOM phenolic moieties and less so with the aromatic carboxylic groups with increasing O3/DOC (dissolved organic carbon) ratios and changes of UV absorbance and fluorescence. When ozonation used as pretreatment, the formation of halophenols in subsequent chlorination decreased linearly with increasing O3 doses or changes of UV absorbance until it reached 85% suppression of the halophenols' formation from unaltered DOM. The thresholds of decreases of UVA254, UVA280 and humic-like fluorescence corresponding to 85% suppression of halophenols’ formation were in the range of 25%–30%, 30%–35% and 30%–45%, respectively. Pre-ozonation also showed a moderate suppression of haloacetic acids (HAAs) formation potentials, ≤26.5% for reverse osmosis isolate of Suwannee River natural organic matter and ≤31.5% for Yangtze River at applied O3 doses. Measurement of changes of estrogenic activity during ozonation of water and wastewater showed that to attain a >90% abatement of estrogenic activity, the corresponding thresholds of decreases of UVA254, UVA280 and humic-like fluorescence were ∼30%, ∼40%, and ∼70%, respectively. Bromate formation was also suppressed to below 10 μg/L before these thresholds. This study suggests that optimal ozonation conditions and a balance between control of disinfection byproducts (halophenols, HAAs and bromate) and elimination of estrogenic activity can be reached based on online data.

This work aims to correlate signals of LED UV/fluorescence sensor with the degradation of dissolved organic matter (DOM) and trace-level organic contaminants (TOrCs) during ozonation process. Six sets of bench-scale ozonation kinetic experiments incorporated with three different water matrices and 14 TOrCs of different reactivity (group I ∼ V) were conducted. Calibrated by tryptophan and humic substances standards and verified by the lab benchtop spectroscopy, the newly developed portable/online LED sensor, which measures the UV280 absorbance, protein-like and humic-like fluorescence simultaneously, was feasible to monitor chromophores and fluorophores with good sensitivity and accuracy. The liquid chromatography with organic carbon detector combined with 2D synchronous correlation analysis further demonstrated how the DOM components of large molecular weight were transformed into small moieties as a function of the decrease of humic-like fluorescence. For TOrCs, their removal rates were well correlated with the decrease of the LED UV/fluorescence signals, and their elimination patterns were mainly determined by their reactivity with O3 and hydroxyl radicals. At approximately 50% reduction of humic-like fluorescence almost complete oxidation of TOrCs of group I and II was reached, a similar removal percentage (25-75%) of TOrCs of group III and IV, and a poor removal percentage (

Online monitoring dissolved organic matter (DOM) is urgent for water treatment management. In this study, high performance size exclusion chromatography with multi-UV absorbance and multi-emission fluorescence scans were applied to spectrally characterize samples from 16 drinking water sources across Yangzi River and Huai River Watersheds. The UV absorbance indices at 254 nm and 280 nm referred to the same DOM components and concentration, and the 280 nm UV light could excite both protein-like and humic-like fluorescence. Hence a novel UV fluorescence sensor was developed out using only one UV280 light-emitting diode (LED) as light source. For all samples, enhanced coagulation was mainly effective for large molecular weight biopolymers; while anion exchange further substantially removed humic substances. During chlorination tests, UVA280 and UVA254 showed similar correlations with yields of disinfection byproducts (DBPs); the humic-like fluorescence obtained from LED sensors correlated well with both trihalomethanes and haloacetic acids yields, while the correlation between protein-like fluorescence and trihalomethanes was relatively poor. Anion exchange exhibited more reduction of DBPs yields as well as UV absorbance and fluorescence signals than enhanced coagulation. The results suggest that the LED UV fluorescence sensors are very promising for online monitoring DOM and predicting DBPs formation potential during water treatment.

The application of anion exchange resins (AERs) has been limited by the critical problem of resin fouling, which increases the volume of the desorption concentrate and decreases treatment efficiency. To date, resin fouling has not been well studied and is poorly understood compared to membrane fouling. To reflect the resin fouling level, a resin fouling index (RFI) was established in this work according to the decrease of DOC removal after regeneration of the resin for the advanced treatment of municipal wastewater. Comparing the linear fitting results between the RFI and the fluorescence intensity indicated that the resin fouling was related to the protein-like substances with fluorescence peak T in the region of excitation wavelength

The need to track and characterize dissolved organic matter (DOM) has made fluorescence excitation-emission matrix (EEM) spectroscopy extensively used. In this work, reverse phase high-performance liquid chromatography (RP-HPLC) and high-performance size exclusion chromatography (HPSEC) with fluorescence detector (FLD) were used for EEM interpretation and DOM analysis. Given that fluorescence detectors can scan with multi-excitation or multi-emission mode, HPLC-FLD with multi-excitation scan directly verified the prevalence of multi-peak fluorophores in EEM, which provides a corrective insight for the current fluorescence regional integration (FRI) methods; whereas HPLC-FLD with multi-emission scan provided more informative fluorescence fingerprints for identification of DOM species, which is a chromatographic surrogate for determining the proper number of PARAFAC components. Besides providing a deep insight for the current EEM interpretation, the HPLC/HPSEC-FLD results also directly related physiochemical properties to DOM species, including polarity and molecular weight (MW) distribution, which is helpful for further characterization their behavior in water and wastewater treatment process. A chromatography technique with multi-excitation and multi-emission fluorescence scan can be an informative method for EEM interpretation and DOM identification and characterization.

Ozone is an effective oxidant and disinfectant commonly used for elimination of micropollutants and inactivation of resistant microbes. However, undesirable oxidation/disinfection byproducts such as bromate might form during ozonation. In this study, the UV absorbance and fluorescence indices were applied as surrogate indicators for predicting the inactivation of bacteria and formation of bromate during ozonation of water and wastewater effluents. The inactivation efficiencies of lab-cultured Escherichia coli (E. coli) and autochthonous bacteria were measured by plating (for E. coli­ only) and flow cytometry with fluorescence staining. During ozonation of E. coli spiked into wastewater effluents (~106 cell/mL), the priority of inactivation efficiency determined by different cell viability methods were in the order of CFU > membrane damage > DNA damage. Approximately, 99% membrane damage and/or 90% DNA damage are conservatively supposed as an indicator for sufficient bacterial inactivation as well as degradation of antibiotic resistance genes. The related required O3 dosing thresholds for sufficient inactivation of E. coli and autochthonous bacteria refer to ~0.6 O3/DOC, ~50% decrease of UVA254, ~60% decrease of UVA280, or ~80% decrease of humic-like fluorescence. Within the range of 106–108 cell/mL, the bacterial concentration did not have significant effects on the required thresholds of the specific O3 doses or spectroscopic indicators required for bacterial inactivation. The addition of 50 mM tert-BuOH as ·OH scavenger increased the required specific ozone doses but decreased the losses of spectroscopic indicators necessary for sufficient bacterial inactivation, and also suggested that the membrane/DNA damages for bacterial inactivation were mainly attributed to the direct O3 attacks. The bromate concentration was determined using ion chromatography with MS/MS detection. The results showed that when O3 was dosed at the required thresholds for sufficient bacterial inactivation, bromate formation could usually be suppressed below 10 μg/L. The present work supports that it is possible to reach a balance between bacterial inactivation and bromate formation.