Search

Antibiotics usually induce the hormetic effects on bacteria, featured by low-dose stimulation and high-dose inhibition, which challenges the central belief in toxicity assessment and environmental risk assessment of antibiotics. However, there are currently no ideal parameters to quantitatively characterize hormesis. In this study, an effective area in hormesis (A H ) was developed to quantify the biphasic dose-responses of single antibiotics (sulfonamides (SAs), sulfonamides potentiators (SAPs), and tetracyclines (TCs)) and binary mixtures (SAs-SAPs, SAs-TCs, and SAs-SAs) to the bioluminescence of Aliivibrio fischeri. Using E bind (the lowest interaction energy between antibiotic and target protein) and K ow (octanol-water partition coefficient) as the structural descriptors, the reliable quantitative structure-activity relationship (QSAR) models were constructed for the A H values of test antibiotics and mixtures. Furthermore, a novel method based on A H was established to judge the joint toxic actions of binary antibiotics, which mainly exhibited synergism. The results also indicated that SAPs (or TCs) contributed more than SAs in the hormetic effects of antibiotic mixtures. This study proposes a new quantitative parameter for characterizing and predicting antibiotic hormesis, and considers hormesis as an integrated whole to reveal the combined effects of antibiotics, which will promote the development of risk evaluation for antibiotics and their mixtures., 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 B.V. All rights reserved.)

Aqueous Zn metal batteries are attracting tremendous interest as promising energy storage systems due to their intrinsic safety and cost-effectiveness. Nevertheless, the reversibility of Zn metal anodes (ZMAs) is hindered by water-induced parasitic reactions and dendrite growth. Herein, a novel hydrated eutectic electrolyte (HEE) consisting of Zn(BF 4 ) 2 ·xH 2 O and sulfolane (SL) is developed to prevent the side reactions and achieve the outstanding cyclability of ZMAs. The strong coordination between Zn 2+ and SL triggers the eutectic feature, enabling the low-temperature availability of HEEs. The restriction of BF 4 - hydrolysis in the eutectic system can realize favorable compatibility between Zn(BF 4 ) 2 -based electrolyte and ZMAs. Besides, the newly-established solvation structure with the participation of SL, H 2 O, and BF 4 - , can induce in situ formation of desirable SEI with gradient structure consisting of B,O-rich species, ZnS, and ZnF 2 , to offer satisfactory protection toward ZMAs. Consequently, the HEE allows the Zn||Zn symmetric cell to cycle over 1650 h at 2 mA cm -2 and 1 mA h cm -2 . Moreover, the Zn||NH 4 V 4 O 10 full batteries can deliver a prolonged lifespan for 1000 cycles with a high capacity retention of 83.4%. This work represents a feasible approach toward the elaborate design of advanced electrolyte systems for next-generation batteries., (© 2024 Wiley‐VCH GmbH.)

A large amount of antibiotics enters the soil environment and accumulates therein as individuals and mixtures, threatening the soil safety. However, there is little information regarding the influence of single and mixed antibiotics on key soil proteins at molecular level. In this study, setting sulfadiazine (SD) and tetracycline hydrochloride (TC) as the representative antibiotics, the interactions between these agents and α-amylase (an important hydrolase in soil carbon cycle) were investigated through multi-spectroscopic approaches, X-ray photoelectron spectrometry, and molecular modeling. It was found that both SD and TC spontaneously bound to α-amylase with 1:1 stoichiometry mainly via forming stable chemical bonds. The interactions altered the polarity of aromatic amino acids, protein backbone, secondary structure, hydrophobicity and activity of α-amylase. The SD-TC mixtures were designed based on the direct equipartition ray to comprehensively characterize the possible concentration distribution, and interactive effects indicated that the mixtures antagonistically impacted α-amylase. These findings reveal the binding characteristics between α-amylase and typical antibiotics, which probably influence the ecological functions of α-amylase in soil. This study clarifies the potential harm of antibiotics on soil functional enzyme, which is significant for the environmental risk assessment of antibiotics and their mixtures., 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 B.V. All rights reserved.)

Metal phthalocyanine molecules with Me-N 4 centers have shown promise in electrocatalytic CO 2 reduction (eCO 2 R) for CO generation. However, iron phthalocyanine (FePc) is an exception, exhibiting negligible eCO 2 R activity due to a higher CO 2 to * COOH conversion barrier and stronger * CO binding energy. Here, amine functional groups onto atomic-Fe-rich carbon dots (Af-Fe-CDs) are introduced via a one-step solvothermal molecule fusion approach. Af-Fe-CDs feature well-defined Fe-N 4 active sites and an impressive Fe loading (up to 8.5 wt%). The synergistic effect between Fe-N 4 active centers and electron-donating amine functional groups in Af-Fe-CDs yielded outstanding CO 2 -to-CO conversion performance. At industrial-relevant current densities exceeding 400 mA cm -2 in a flow cell, Af-Fe-CDs achieved >92% selectivity, surpassing state-of-the-art CO 2 -to-CO electrocatalysts. The in situ electrochemical FTIR characterization combined with theoretical calculations elucidated that Fe-N 4 integration with amine functional groups in Af-Fe-CDs significantly reduced energy barriers for * COOH intermediate formation and * CO desorption, enhancing eCO 2 R efficiency. The proposed synergistic effect offers a promising avenue for high-efficiency catalysts with elevated atomic-metal loadings., (© 2024 Wiley‐VCH GmbH.)

Quorum sensing inhibitors (QSIs), as a kind of ideal antibiotic substitutes, have been recommended to be used in combination with traditional antibiotics in medical and aquaculture fields. Due to the co-existence of QSIs and antibiotics in environmental media, it is necessary to evaluate their joint risk. However, there is little information about the acute toxicity of mixtures for QSIs and antibiotics. In this study, 10 QSIs and 3 sulfonamides (SAs, as the representatives for traditional antibiotics) were selected as the test chemicals, and their acute toxic effects were determined using the bioluminescence of Aliivibrio fischeri ( A. fischeri ) as the endpoint. The results indicated that SAs and QSIs all induced S-shaped dose-responses in A. fischeri bioluminescence. Furthermore, SAs possessed greater acute toxicity than QSIs, and luciferase (Luc) might be the target protein of test chemicals. Based on the median effective concentration (EC 50 ) for each test chemical, QSI-SA mixtures were designed according to equitoxic (EC 50(QSI) :EC 50(SA)  = 1:1) and non-equitoxic ratios (EC 50(QSI) :EC 50(SA)  = 1:10, 1:5, 1:0.2, and 1:0.1). It could be observed that with the increase of QSI proportion, the acute toxicity of QSI-SA mixtures enhanced while the corresponding TU values decreased. Furthermore, QSIs contributed more to the acute toxicity of test binary mixtures. The joint toxic actions of QSIs and SAs were synergism for 23 mixtures, antagonism for 12 mixtures, and addition for 1 mixture. Quantitative structure-activity relationship (QSAR) models for the acute toxicity QSIs, SAs, and their binary mixtures were then constructed based on the lowest CDOCKER interaction energy ( E bind-Luc ) between Luc and each chemical and the component proportion in the mixture. These models exhibited good robustness and predictive ability in evaluating the toxicity data and joint toxic actions of QSIs and SAs. This study provides reference data and applicable QSAR models for the environmental risk assessment of QSIs, and gives a new perspective for exploring the joint effects of QSI-antibiotic mixtures., Competing Interests: 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., (© 2024 The Author(s).)

Metal-organic frameworks (MOFs) hold great promise for diverse applications when combined with polymers. However, a persistent challenge lies in the susceptibility of exposed MOF pores to molecule and polymer penetration, compromising the porosity and overall performance. Here, we design a molecular-caged MOF (MC-MOF) to achieve contracted window without sacrificing the MOF porosity by torsional conjugated ligands. These molecular cages effectively shield against the undesired molecule penetration during polymerization, thereby preserving the pristine porosity of MC-MOF and providing outstanding light and thermal management to the composites. The polymer containing 0.5 wt % MC-MOF achieves an 83% transmittance and an exceptional haze of 93% at 550 nanometers, coupled with remarkable thermal insulation. These MC-MOF/polymer composites offer the potential for more uniform daylighting and reduced energy consumption in sustainable buildings when compared to traditional glass materials. This work delivers a general method to uphold MOF porosity in polymers through molecular cage design, advancing MOF-polymer applications in energy and sustainability.

Amidoxime-based fiber adsorbents hold significant promise for uranium extraction. However, a notable issue is that these adsorbents primarily originate from synthetic polymer materials, which, aside from providing good mechanical support, have no other functions. In recent study, we shifted our focus to silk fiber (SF), a natural protein fiber known for its unique core-shell structure and rich amino acids. The shell layer, due to its abundant functional groups, makes it easily modifiable, while the core layer provides excellent mechanical strength. Leveraging these inherent properties, an amidoxime-based fiber adsorbent was developed. This adsorbent utilizes amino and carboxyl groups for enhanced performance synergistically. This method involves establishing uranium affinity sites on the outer sericin layer of SF via chemical initiation of graft polymerization (CIGP) and amidoximation (SF-g-PAO). The water absorption ratio of SF-g-PAO is as high as 601.16 % (DG = 97.17 %). Besides, SF-g-PAO demonstrates an exceptional adsorption capacity of 15.69 mg/g in simulated seawater, achieving a remarkable removal rate of uranyl ions at 95.06 %. It can withstand a minimum of five adsorption-elution cycles. Over a 4-week period in natural seawater, SF-g-PAO displayed an adsorption capacity of 4.95 mg/g. Furthermore, SF-g-PAO also exhibits impressive uranium removal efficiency in real nuclear wastewater, with a removal rate of 63 % in just 15 min and a final removal rate of 90 %. It is hoped that this SF-g-PAO, prepared through this straightforward method and characterized by the synergistic action of amino and carboxyl groups, can offer innovative insights into the development of uranium extraction adsorbents., 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 B.V. All rights reserved.)

Transition metal selenides are considered as promising anode materials for potassium-ion batteries (PIBs) due to their high theoretical capacities. However, their applications are limited by low conductivity and large volume expansion. Herein, sugar-gourd-shaped carbon nanofibers embedded with heterostructured ZnCo-Se nanocages are prepared via a facile template-engaged method combined with electrospinning and selenization process. In this hierarchical ZnCo-Se@NC/CNF, abundant phase boundaries of CoSe 2 /ZnSe heterostructure can promote interfacial electron transfer and chemical reactivity. The interior porous ZnCo-Se@NC nanocage structure relieves volume expansion and maintains structural integrity during K + intercalation and deintercalation. The exterior spinning carbon nanofibers connect the granular nanocages in series, which prevents the agglomeration, shortens the electron transport distance and enhances the reaction kinetics. As a self-supporting anode material, ZnCo-Se@NC/CNF delivers a high capacity (362 mA h g -1 at 0.1 A g -1 after 100 cycles) with long-term stability (95.9% capacity retention after 1000 cycles) and shows superior reaction kinetics with high-rate K-storage. Energy level analysis and DFT calculations illustrate heterostructure facilitates the adsorption of K + and interfacial electron transfer. The K + storage mechanism is revealed by ex situ XRD and EIS analyses. This work opens a novel avenue in designing high-performance heterostructured anode materials with ingenious structure for PIBs., (© 2023 Wiley‐VCH GmbH.)

Transition metal oxides are widely used as Fenton-like catalysts in the treatment of organic pollutants, but their synthesis usually requires a high temperature. Herein, an all-solid-state synthesis method controlled by graphene was used to prepare a double pyramid stacked CoO nano-crystal at a low temperature. The preparation temperature decreased by 200 °C (over 30% reduction) due to the introduction of graphene, largely reducing the reaction energy barrier. Interestingly, the corresponding degradation rate constants ( k obs ) of this graphene-supported pyramid CoO nano-crystals for organic molecules after their adsorption were over 2.5 and 35 times higher than that before adsorption and that of free CoO, respectively. This high catalytic efficiency is attributed to the adsorption of pollutants at the surface by supporting graphene layers, while free radicals activated by CoO can directly and rapidly contact and degrade them. These findings provide a new strategy to prepare low carbon-consuming transition metal oxides for highly efficient Fenton-like catalysts.

The severe hazards on ecological environment and human body caused by volatile organic compounds (VOCs) have attracted worldwide substantial attention. In this research, a series of novel modified Universitetet i Oslo-67 (UiO-67) with water resistance were prepared and characterized, which had modified by benzoic acid and dopamine hydrochloride (67-ben-DH). On this basis, the adsorption performance, adsorption kinetics, defect engineering and water resistance of adsorbent were investigated. The results indicated that the excellent pore structure and specific surface area of 67-ben-DH-6 (molar ratio of Zr 4+ to DH was 1:6) were retained while the adsorption performance and water resistance of the adsorbent were improved. Due to more defects, excellent adsorption diffusion and strong π-π interactions of 67-ben-DH-6, it performed the maximum adsorption capacity of toluene (793 mg g -1 ). Furthermore, the outstanding water resistance was attributed to the fact that N element of DH reduced the affinity of the adsorbent with water. Finally, the density functional theory (DFT) calculations showed that the adsorbent 67-ben-DH-6 had the maximum adsorption energy for toluene (-99.4 kJ mol -1 ) and the minimum adsorption energy for water (-17.8 kJ mol -1 ). Thus, the potential mechanism of 67-ben-DH for efficient toluene adsorption and water resistance was verified from a microscopic perspective., 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 Inc. All rights reserved.)

Biocompatible materials and biocarriers have attracted great attention in biological wastewater treatment owing to their excellent performance in improving pollutant removal. Graphene-based material, a biocarrier candidate, with excellent adsorbability and conductivity was increasingly applied in anaerobic digestion due to its exceptional potential in the adsorption and electron transfer process. Nevertheless, the green approach for the formation of bio-graphene complexes and their mechanism in dye removal is limited. The aim of this study is to investigate and assess the performance of biological graphene hydrogel (BGH) formed by Shewanella putrefaciens CN32 on the removal of methyl orange (MO) and methylene blue (MB). The results showed that the formation of BGH is determined by the physicochemical characteristics of graphene oxide, including sheet size, oxidation degree, and interlayer distance. BGHs significantly increased the removal efficiency of dyes in comparison to non-graphene samples, with a 24-h removal rate of MO and MB reaching 92.9% and 91%, respectively. The synergetic mechanism of BGH on the enhanced removal rate of organic dye can be ascribed to GO's ability in accelerating extracellular electron transfer and stimulating biodegradation pathways relating to c-type cytochromes, including MtrA and MtrC. These findings provided an understanding of the relationship between graphene-based nanomaterials and Shewanella, which facilitated their future application in environmental biotechnology., 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 Inc. All rights reserved.)

Inefficient charge separation and slow interfacial reaction dynamics significantly hamper the efficiency of photocatalytic CO 2 reduction. Herein, a facile EDC/NHS-assisted linking strategy was developed to enhance charge separation in heterojunction photocatalysts. Using this approach, we successfully synthesized amide-bonded carbon quantum dot- g -C 3 N 4 (CQD-CN) heterojunction photocatalysts. The formation of amide covalent bonds between CN and CQDs in the CN-CQD facilitates efficient carrier migration, CO 2 adsorption, and activation. Exploiting these advantages, the CN-CQD photocatalysts exhibit high selectivity with CO and CH 4 evolution rates of 79.2 and 2.7 μmol g -1 h -1 , respectively. These rates are about 1.7 and 3.6 times higher than those of CN@CQD and bulk CN, respectively. Importantly, the CN-CQD photocatalysts demonstrate exceptional stability, even after 12 h of continuous testing. The presence of the COOH* signal is identified as a crucial intermediate species in the conversion of CO 2 to CO. This study presents a covalent bonding engineering strategy for developing high-performance heterojunction photocatalysts for efficient solar-driven reduction of CO 2 .

Biotechnology is a promising approach to environmental remediation but requires improvement in efficiency and convenience. The improvement of biotechnology has been illustrated with the help of biocompatible materials as biocarrier for environmental remediations. Recently, graphene-based materials (GBMs) have become promising materials in environmental biotechnology. To better illustrate the principle and mechanisms of GBM application in biotechnology, the comprehension of the biological response of microorganisms and enzymes when facing the GBMs is needed. The review illustrated distinct GBM-microbe/enzyme composites by providing the GBM-microbe/enzyme interaction and the determining factors. There are diverse GBM modifications for distinct biotechnology applications. Each of these methods and applications depends on the physicochemical properties of GBMs. The applications of these composites were mainly categorized as pollutant adsorption, anaerobic digestion, microbial fuel cells, and organics degradation. Where information was available, the strategies and mechanisms of GBMs in improving application efficacies were also demonstrated. In addition, the biological response, from microbial community changes, extracellular polymeric substances changes to biological pathway alteration, may become important in the application of these composites. Furthermore, we also discuss challenges facing the environmental application of GBMs, considering their fate and toxicity in the ecosystem, and offer potential solutions. This research significantly enhances our comprehension of the fundamental principles, underlying mechanisms, and biological pathways for the in-situ utilization of GBMs., 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.)

Electrocatalysts for highly efficient oxygen reduction reaction (ORR) are crucial for energy conversion and storage devices. Single-atom catalysts with maximized metal utilization and altered electronic structure are the most promising alternatives to replace current benchmark precious metals. However, the atomic level understanding of the functional role for each species at the anchoring sites is still unclear and poorly elucidated. Herein, we report Fe single atom catalysts with the sulfur and oxygen functional groups near the atomically dispersed metal centers (Fe1/NSOC) for highly efficient ORR. The Fe1/NSOC delivers a half-wave potential of 0.92 V vs. RHE, which is much better than those of commercial Pt/C (0.88 V), Fe single atoms on N-doped carbon (Fe1/NC, 0.89 V) and most reported nonprecious metal catalysts. The spectroscopic measurements reveal that the presence of sulfur group induces the formation of epoxy groups near the FeN4S2 centers, which not only modulate the electronic structure of Fe single atoms but also participate the catalytic process to improve the kinetics. The density functional theory calculations demonstrate the existence of sulfur and epoxy group engineer the charges of Fe reactive center and facilitate the reductive release of OH* (rate-limiting step), thus boosting the overall oxygen reduction efficiency., (© 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)

Solid-state electrolytes (SEs) have attracted overwhelming attention as a promising alternative to traditional organic liquid electrolytes (OLEs) for high-energy-density sodium-metal batteries (SMBs), owing to their intrinsic incombustibility, wider electrochemical stability window (ESW), and better thermal stability. Among various kinds of SEs, inorganic solid-state electrolytes (ISEs) stand out because of their high ionic conductivity, excellent oxidative stability, and good mechanical strength, rendering potential utilization in safe and dendrite-free SMBs at room temperature. However, the development of Na-ion ISEs still remains challenging, that a perfect solution has yet to be achieved. Herein, we provide a comprehensive and in-depth inspection of the state-of-the-art ISEs, aiming at revealing the underlying Na + conduction mechanisms at different length scales, and interpreting their compatibility with the Na metal anode from multiple aspects. A thorough material screening will include nearly all ISEs developed to date, i.e. , oxides, chalcogenides, halides, antiperovskites, and borohydrides, followed by an overview of the modification strategies for enhancing their ionic conductivity and interfacial compatibility with Na metal, including synthesis, doping and interfacial engineering. By discussing the remaining challenges in ISE research, we propose rational and strategic perspectives that can serve as guidelines for future development of desirable ISEs and practical implementation of high-performance SMBs.

This study investigates the mechanism behind the enhanced photocatalytic performance of carbon quantum dot (CQD)-induced photocatalysts. Red luminescent CQDs (R-CQDs) were synthesized using a microwave ultrafast synthesis strategy, exhibiting similar optical and structural properties but varying in surface functional group sites. Model photocatalysts were synthesized by combining R-CQDs with graphitic carbon nitride (CN) using a facile coupling technique, and the effects of different functionalized R-CQDs on CO 2 reduction were investigated. This coupling technique narrowed the band gap of R1-CQDs/CN, made the conduction band potentials more negative, and made photogenerated electrons and holes less likely to recombine. These improvements greatly enhanced the deoxygenation ability of the photoinduced carriers, increased light absorption of solar energy, and raised the carrier concentration, resulting in excellent stability and remarkable CO production. R1-CQDs/CN demonstrated the highest photocatalytic activity, with CO production up to 77 μmol g -1 within 4 h, which is approximately 5.26 times higher than that of pure CN. Our results suggest that the superior photocatalytic performance of R1-CQDs/CN arises from its strong internal electric field and high Lewis acidity and alkalinity, attributed to the abundant pyrrolic-N and oxygen-containing surface groups, respectively. These findings offer a promising strategy for producing efficient and sustainable CQD-based photocatalysts to address global energy and environmental problems.

Electrochemical carbon dioxide reduction reaction (CO 2 RR) provides a promising way to convert CO 2 to chemicals. The multicarbon (C 2+ ) products, especially ethylene, are of great interest due to their versatile industrial applications. However, selectively reducing CO 2 to ethylene is still challenging as the additional energy required for the C-C coupling step results in large overpotential and many competing products. Nonetheless, mechanistic understanding of the key steps and preferred reaction pathways/conditions, as well as rational design of novel catalysts for ethylene production have been regarded as promising approaches to achieving the highly efficient and selective CO 2 RR. In this review, we first illustrate the key steps for CO 2 RR to ethylene (e.g., CO 2 adsorption/activation, formation of *CO intermediate, C-C coupling step), offering mechanistic understanding of CO 2 RR conversion to ethylene. Then the alternative reaction pathways and conditions for the formation of ethylene and competitive products (C 1 and other C 2+ products) are investigated, guiding the further design and development of preferred conditions for ethylene generation. Engineering strategies of Cu-based catalysts for CO 2 RR-ethylene are further summarized, and the correlations of reaction mechanism/pathways, engineering strategies and selectivity are elaborated. Finally, major challenges and perspectives in the research area of CO 2 RR are proposed for future development and practical applications., (© 2023. The Author(s).)

The pervasive presence of persistent contaminants in water resources, including phosphate and antibiotics, has attracted significant attention due to their potential adverse effects on ecosystems and human health. Adsorption membranes packed with metal-organic frameworks (MOFs) have been proposed as a potential solution to this challenge due to their high surface area to volume ratio, and the tailored functionality they can provide for selective purification. However, devising a straightforward method to enhance the stability of MOF membranes on polymer supports and manipulate their surface morphology remains challenging. In this study, we present a facile solution immersion technique to fabricate a ZIF-L adsorption membrane on commercial supports by leveraging the self-polymerization characteristics of dopamine. The simple coating methodology provides a polydopamine-lined interface that regulates the ZIF-L heteroepitaxial growth, along with tailored nanoflake morphology. Compared with crystals prepared in bulk solution, the sorbents grown on the membrane exhibit a higher saturation capacity of 248 mg g -1 of phosphate (∼80 mg phosphorus per g sorbent) and 196 mg g -1 for tetracycline in static adsorption experiments at 30 °C. Additionally, the membranes are capable of selectively removing 99.5% of the phosphate in simulant solutions comprising competitive background ions in various concentrations, and efficiently removing tetracycline. The result from the static adsorption experiments directly translates to a flow-through process, showcasing the utility of a composite membrane with a 3 μm thick active layer in practical adsorption applications. The facile solution immersion fabrication protocol introduced in this work may offer a more efficient paradigm to harness the potential of MOF composite membranes in selective adsorption and resource recovery applications., Competing Interests: The authors declare that they have no competing interests., (This journal is © The Royal Society of Chemistry.)

Previous theoretical calculations have predicted that the incorporation of tellurium (Te) into carbon materials can significantly enhance their catalytic activity. Nevertheless, the experimental realization of efficient Te-doped carbon materials remains challenging. Here, we employed theoretical calculations to deduce the possible structure of Te-doped carbon materials. Our findings unveil that the formation of Te-O pairs in carbon materials with a relatively low oxygen coordination microenvironment can impart strong electron-donating capabilities, thereby boosting the electrocatalytic activity of oxygen reduction reaction (ORR). To verify our theoretical predictions, we synthesized Te-O pair-doped carbon materials using a tandem hydrothermal dehydration-pyrolysis strategy. This approach enabled efficient infiltration of Te into carbon materials. Our unconventional Te-O pair-doped carbon materials exhibit expanded interlayer distances and graphene-like nanosheet architectures, which provide enlarged active areas. These structural features contribute to the enhanced ORR catalytic performance of the as-prepared carbon catalyst. Our findings provide molecular-level insights into the design of various carbon-based electrocatalysts with binary-heteroatom-doped active sites.

Previous studies have reported the immunotoxicity of per- and polyfluoroalkyl substances (PFASs), but it remains a significant challenge to assess over 10,000 distinct PFASs registered in the distributed structure-searchable toxicity (DSSTox) database. We aim to reveal the mechanisms of immunotoxicity of different PFASs and hypothesize that PFAS immunotoxicity is dependent on the carbon chain length. Perfluorobutanesulfonic acid (PFBA), perfluorooctanoic acid (PFOA), and perfluorononanoic acid (PFNA) representing different carbon chain lengths (4-9) at environmentally relevant levels strongly reduced the host's antibacterial ability during the zebrafish's early-life stage. Innate and adaptive immunities were both suppressed after PFAS exposures, exhibiting a significant induction of macrophages and neutrophils and expression of immune-related genes and indicators. Interestingly, the PFAS-induced immunotoxic responses were positively correlated to the carbon chain length. Moreover, PFASs activated downstream genes of the toll-like receptor (TLR), uncovering a seminal role of TLR in PFAS immunomodulatory effects. Myeloid differentiation factor 88 (MyD88) morpholino knock-down experiments and MyD88 inhibitors alleviated the immunotoxicity of PFASs. Overall, the comparative results demonstrate differences in the immunotoxic responses of PFASs due to carbon chain length in zebrafish, providing new insights into the prediction and classification of PFASs mode of toxic action based on carbon chain length.

Since the environmental hazards of volatile organic compounds (VOCs) are well known, heterogeneous catalysis has become one of the most popular methods to treat VOCs due to its environmental friendliness and simplicity of operation. Although a large number of reports have reviewed the application of catalytic oxidation for the degradation of VOCs, relatively few reports are based on this direction of metal organic frameworks (MOFs) and MOF derivatives. Herein, this paper reviews the recent applications of heterogeneous catalytic technologies in the degradation of VOCs, including photocatalysis, thermal catalysis and other catalytic approaches. The applications of MOFs and their derivatives in VOCs degradation, such as the progress of MOF-derived metal oxides in the treatment of toluene, were highlighted. The mechanisms of VOCs degradation by different catalytic approaches were systematically presented. Finally, we presented the views and directions of VOCs treatment technology development. We hope that this reaction type-oriented review will provide important insights into MOFs and MOF-derived materials for VOCs pollution control., 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 Inc. All rights reserved.)

Dielectric encapsulation materials are promising for solar cell areas, but the unsatisfactory light-management capability and relatively poor dielectric properties restrict their further applications in photovoltaic and microelectronic devices. Herein, an interface fusion strategy to engineer the interface of MOF (UiO-66-NH 2 ) with anhydride terminated imide oligomer (6FDA-TFMB) is designed and a novel MOF cluster (UFT) with enhanced forward scattering and robust porosity is prepared. UFT is applied as an optical and dielectric modifier for bisphenol A epoxy resin (DGEBA), and UFT epoxy composites with high transmittance (>80%), tunable haze (45-58%) and excellent dielectric properties can be prepared at low UFT contents (0.5-1 wt%), which delivers an optimal design for dielectric encapsulation systems with efficient light management in solar cells. Additionally, UFT epoxy composites also show excellent UV blocking, and hydrophobic, thermal and mechanical properties. This work provides a template for the synthesis of covalent bond-mediated nanofillers and for the modulation of haze and dielectric properties of dielectric encapsulation materials for energy systems, semiconductors, microelectronics, and more., (© 2023 The Authors. Advanced Science published by Wiley-VCH GmbH.)

A highly stable interface for aqueous rechargeable Zn batteries is of importance to inhibit the growth of Zn dendrites and suppress the side reactions. In this work, we have developed a stable honeycomb-like ZnO passivation protective layer on the Zn surface, which is in situ generated with the assistance of a nonionic surfactant additive (polyethylene glycol tert-octylphenyl ether, denoted as PEGTE). The ZnO passivation layer can facilitate the uniform distribution of the electric field, guiding the uniform deposition of Zn 2+ and inhibit the generation of dendrites. As a result, the symmetric cell using the electrolyte with PEGTE shows an excellent performance at high areal capacity, reflected by stable cycling for over 2400 h at 5 mAh/cm 2 and 1300 h at 10 mAh/cm 2 . The full cell paired with V 2 O 5 demonstrates a long lifespan for more than 600 cycles at a low negative/positive capacity ratio.

Water polluted by pharmaceutically active compounds (PhACs) and water-borne pathogens urgently need to develop eco-friendly and advanced water treatment techniques. This paper evaluates the potential of using calcium peroxide (CaO 2 ), a safe and biocompatible oxidant both PhACs (thiamphenicol, florfenicol, carbamazepine, phenobarbital, and primidone) and pathogens (Escherichia coli, Staphylococcus aureus) in water. This paper evaluates the potential of using calcium peroxide (CaO 2 ) as a safe and biocompatible oxidant to remove both PhACs (thiamphenicol, florfenicol, carbamazepine, phenobarbital, and primidone) and pathogens (Escherichia coli, Staphylococcus aureus) in water. The increased CaO 2 dosage increased efficiencies of PhACs attenuation and pathogens inactivation, and both exhibited pseudo-first-order degradation kinetics (R 2  > 0.90). PhACs attenuation were mainly via oxidization (H 2 O 2 , •OH/O •- , and O 2 •- ) and alkaline hydrolysis (OH - ) from CaO 2 . Moreover, concentrations of these reactive species and their contributions to PhACs attenuation were quantified, and mechanistic model was established and validated. Besides, possible transformation pathways of target PhACs except primidone were proposed. As for pathogen indicators, the suitable inactivation dosage of CaO 2 was 0.1 g L -1 . The oxidability (18-64%) and alkalinity (82-36%) generated from CaO 2 played vital roles in pathogen inactivation. In addition, CaO 2 at 0.01-0.1 g L -1 can be applied in remediation of SW contaminated by PhACs and pathogenic bacteria, which can degrade target PhACs with efficiencies of 21-100% under 0.01 g L -1 CaO 2 , and inactivate 100% of test bacteria under 0.1 g L -1 CaO 2 . In short, capability of CaO 2 to remove target PhACs and microbial pathogens reveals its potential to be used as a representative technology for the advanced treatment of waters contaminated by organic compounds and microbial pathogens., (Copyright © 2022 Elsevier Inc. All rights reserved.)

Magnetic field is a simple and powerful means that enables controlled the transport of electrode particles in flow electrode capacitive deionization (FCDI). However, the magnetic particles are easily stripped from hybrid suspension electrodes and the precise manipulation of the charge percolation network remains challenging. In this study, a programmable magnetic field was introduced into the FCDI system to enhance the desalination performance and operational stability of magnetic FCDI, with core-shell magnetic carbon (MC) used as an alternative electrode additive. The results showed that the pulsed magnetic field (PMF) was more effective in enhancing the average salt removal rate (ASRR) compared to the constant magnetic field (CMF), with 51.6% and 67.7% enhancement, respectively, compared to the magnetic field-free condition. The outstanding advantage of the PMF lies in the enhancement in the trapping and mediating effects in the switching magnetic field, which keeps the concentration of the electrode particles near the current collector at a high level and greatly facilitates electron transport. In long-term operation (20,000 cycles), the pulsed magnetic FCDI achieved a stable desalinating rate of 0.4-0.68 μmol min -1  cm -2 and a charge efficiency of >96%. In brief, our study introduces a new approach for the precise manipulation of charge percolation networks of the suspension electrodes and provides insight into the charging mechanism of the magnetic FCDI., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

Phosphorus-rich iron phosphides (FeP 2 ) have been regarded as excellent anode candidates for lithium storage owing to their low cost, high natural abundance, high theoretical capacity, and reasonable redox potential. However, FeP 2 suffers from a few challenging problems such as low reversibility, fast capacity degradation, and big volume variation. Herein, we have designed and synthesized a 3D honeycomb-like carbon skeleton with embedded FeP 2 nanoparticles (denoted as FeP 2 NPs@CK), which can significantly promote the kinetics and maintain the structural stability during the cycling, resulting in an excellent electrochemical performance reflected by high reversibility and long-term cycling stability. FeP 2 NPs@CK shows high reversibility, delivering a reversible capacity as high as 938 mA h g -1 at 0.5 A g -1 . It also shows excellent cycling stability, delivering a capacity of 620 mA h g -1 after 500 cycles at 1 A g -1 . Moreover, the fast kinetics and lithium storage mechanism of FeP 2 NPs@CK are investigated by quantitative analysis and in situ X-ray diffraction. Such superior performance demonstrates that FeP 2 NPs@CK could be a promising and attractive anode candidate for lithium storage.

Cadmium (Cd) pollution in mining areas is the most important challenge for soil environment management in China. Assessing the actual Cd pollution risk in various mining areas and identifying the core areas requiring supervision can provide a basis for government departments and industries to carry out detailed further investigations in key areas. In this study, we collated published data on metal mine circumjacent soil contaminated by Cd in China from 2002 to 2020 to conduct a comprehensive study on soil cadmium pollution and ecological and health risks in mining areas. The temporal and spatial variations of Cd concentrations and the pollution source were investigated. Results indicated that the Cd concentration in soil was strongly associated with the types of mining area. The Cd pollution in the circumjacent soil of lead-zinc and tungsten mines with high heavy metal pollution discharging coefficient was more serious than the soil around other mines. Identification of temporal and spatial variations for soil Cd in China indicated that the high Cd concentrations were found in the central, southern, and southwestern regions of China, and the distribution of mining activities in these regions are relatively concentrated. Meanwhile, a temporal turning point in the mean soil Cd concentration occurred in these regions in 2012, which indicated that the heavy metal control management policy implemented by the government was effective. The ecological risk of soil Cd pollution around mining areas was moderate to high. Health risk assessment showed that some regions adjacent mining areas had a high non-carcinogenic risk, notably, lead-zinc and tungsten mining areas were more serious. Supervision should focus on reducing ecological risks and protecting the safety of agricultural products rather than concentrating on health risks. The research results provide a reference for the priority management of contaminated soil in mining areas., (Copyright © 2022. Published by Elsevier Ltd.)

Histidine (His) is widely involved in the structure and function of biomolecules. Transition-metal ions, such as Zn 2+ and Cu 2+ , widely exist in biological environments, and they are crucial to many life-sustaining physiological processes. Herein, by employing density function calculations, we theoretically show that the water affinity of His can be enhanced by the strong cation-π interaction between His and Zn 2+ and Cu 2+ . Further, the solubility of His is experimentally demonstrated to be greatly enhanced in ZnCl 2 and CuCl 2 solutions. The existence of cation-π interaction is demonstrated by fluorescence, ultraviolet (UV) spectroscopy and nuclear magnetic resonance (NMR) experiments. These findings are of great importance for the bioavailability of aromatic drugs and provide new insight for understanding the physiological functions of transition metal ions.

Fluoxetine (FLU), a selective serotonin reuptake inhibitor, is commonly found in aquatic environments. Ultraviolet (UV) photolysis is widely used to remove certain pharmaceuticals from water and wastewater. The present study aimed to investigate the toxicity of FLU and its transformed products formed during UV photolysis by using zebrafish embryos (Danio rerio) as a model. The degradation rates of FLU for five days were approximately 63.6% ± 2.14%, 84.6% ± 0.99%, and 97.5% ± 0.25% after 15, 30, and 60 min of UV irradiation, respectively. Furthermore, the degradation mechanism was explored using LC-MS measurements and density flooding theory (DFT) theoretical calculations. Comprehensive toxicity preassessment of FLU and its degradation products was carried out using the T.E.S.T. software. The effects of physiological and biochemical parameters and neuron- and apoptosis-related gene expression were examined in zebrafish embryos exposed to non-irradiated (0-min) and irradiated (15, 30- and 60-min) solutions from 4 h post-fertilization (hpf) to 120 hpf. The hatching time of zebrafish embryos exposed to the non-irradiated solution (0-min) and irradiated solution (60-min) was delayed, their heart rate at 48 and 72 hpf increased, and their body length at 120 hpf decreased. Significant differences were found between the non-irradiated (0-min) and UV-irradiated (15- or 30-min) groups. A dynamic response involving acetylcholinesterase (AChE) and superoxide dismutase (SOD) activity was also observed in the non-irradiated and UV-irradiated groups. During the UV treatment experiments, the expression levels of neuron-related and apoptosis-related genes were significantly reduced over time alongside the formation of FLU degradation products. Overall, this study provides new concepts to remove and assess the toxicity of emerging contaminants in aquatic environments and highlights the need to consider the formation and persistence of toxic transformation products., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

Diet is known to be one of the main sources from which human intake many environmental contaminants, for example, antibiotics. To determine the effect of dietary factors on antibiotic intake, we identified the levels of antibiotics present in the urine of the general population from two regions of Shanghai. Moreover, we assessed the amount of exposure to these substances and the health risks they posed. There were a total of 18 antibiotics, which were sorted into five categories. Based on the above, we used the Food Frequency Questionnaire (FFQ) and demographic data to evaluate the effects of food consumption and demographic factors on levels of the antibiotics in urine. The results found that food sourced from animals had a direct relation to the level of veterinary antibiotics or preferred veterinary antibiotics (VAs/PVAs) detected in urine. Those who regularly consumed, for example, meat, milk and eggs, had considerably more VAs/PVAs in their urine compared to those who didn't. These results demonstrated that animal-derived foods are the main causes of unintentional exposure to antibiotics in human. Our study, therefore, evidenced that more attention must be paid to the residues of unneeded VAs/PVAs derived from animal-sourced food.

Lithium/sodium metal batteries have attracted enormous attention as promising candidates for high-energy storage devices. However, their practical applications are impeded by the growth of dendrites upon Li/Na plating. Here, we report that holey 2D N-doped TiNb 2 O 7 (N-TNO) nanosheets with high electroactive surface area and large amounts of lithiophilic/sodiophilic sites can effectively regulate Li/Na deposition as an interfacial layer, leading to an excellent cycling stability. The N-TNO interfacial layer enables the Li||Li symmetric cell to sustain stable electrodeposition over 1000 h as well as the Na||Na cell to stably cycle for 2400 h at 1 mA cm -2 and 3 mA h cm -2 with a depth of discharge as high as 50%. The full cells of the Li/Na anodes based on the N-TNO layer paired with the LiFePO 4 and NaTi 2 (PO 4 ) 3 cathodes, respectively, show a very stable cycling over 1000 cycles at a negative-to-positive electrode capacity (N/P) ratio up to 3.

The safety of energy storage equipment has always been a stumbling block to the development of battery, and sodium ion battery is no exception. However, as an ultimate solution, the use of non-flammable electrolyte is susceptible to the side effects, and its poor compatibility with electrode, causing failure of batteries. Here, we report a non-flammable electrolyte design to achieve high-performance sodium ion battery, which resolves the dilemma via regulating the solvation structure of electrolyte by hydrogen bonds and optimizing the electrode-electrolyte interphase. The reported non-flammable electrolyte allows stable charge-discharge cycling of both sodium vanadium phosphate@hard carbon and Prussian blue@hard carbon full pouch cell for more than 120 cycles with a capacity retention of >85 % and high cycling Coulombic efficiency (99.7 %)., (© 2021 Wiley-VCH GmbH.)

To accelerate the commercial implementation of high-energy batteries, recent research thrusts have turned to the practicality of Si-based electrodes. Although numerous nanostructured Si-based materials with exceptional performance have been reported in the past 20 years, the practical development of high-energy Si-based batteries has been beset by the bias between industrial application with gravimetrical energy shortages and scientific research with volumetric limits. In this context, the microscale design of Si-based anodes with densified microstructure has been deemed as an impactful solution to tackle these critical issues. However, their large-scale application is plagued by inadequate cycling stability. In this review, we present the challenges in Si-based materials design and draw a realistic picture regarding practical electrode engineering. Critical appraisals of recent advances in microscale design of stable Si-based materials are presented, including interfacial tailoring of Si microscale electrode, surface modification of SiO x microscale electrode, and structural engineering of hierarchical microscale electrode. Thereafter, other practical metrics beyond active material are also explored, such as robust binder design, electrolyte exploration, prelithiation technology, and thick-electrode engineering. Finally, we provide a roadmap starting with material design and ending with the remaining challenges and integrated improvement strategies toward Si-based full cells.

Metallic zinc (Zn) has been considered to be an ideal anode material for aqueous batteries, but is impeded by the growth of Zn dendrites and its side reactions with an aqueous electrolyte. Here, it is reported that an artificial protective layer filled with novel 2D Zn 2+ adsorbed Sb 3 P 2 O 14 3- (denoted as Zn-Sb 3 P 2 O 14 ) nanosheets provide an effective route to mitigate the above challenging problems. The Zn-Sb 3 P 2 O 14 protection layer not only avoids the direct contact with the aqueous electrolyte to suppress the side reactions but also allows for Zn-ions to pass through the protection layer rapidly. Moreover, the 2D Sb 3 P 2 O 14 3- skeleton with negative charge also confines the 2D diffusion of Zn-ion along the lateral surface of Zn anode, resulting in a uniform electron-deposition. This unique protection layer not only enables dendrite-free Zn plating/stripping with an average Coulombic efficiency of 99.2% for 200 cycles, but also sustains the symmetric Zn||Zn cell over 1300 h at 1 mA cm -2 and 1 mAh cm -2 as well as for 450 h at 10 mA cm -2 and 10 mAh cm -2 . Such advantages bring high reversibility to full Zn batteries with MnO 2 cathodes, which deliver a discharge capacity of 111.7 mAh g -1 after 1000 cycles., (© 2021 Wiley-VCH GmbH.)

Developing hard carbon with a high initial Coulombic efficiency (ICE) and very good cycling stability is of great importance for practical sodium-ion batteries (SIBs). Defects and oxygen-containing groups grown along either the carbon edges or the layers, however, are inevitable in hard carbon and can cause a tremendous density of irreversible Na + sites, decreasing the efficiency and therefore causing failure of the battery. Thus, eliminating these unexpected defect structures is significant for enhancing the battery performance. Herein, we develop a strategy of applying a soft-carbon coating onto free-standing hard-carbon electrodes, which greatly hinders the formation of defects and oxygen-containing groups on hard carbon. The electrochemical results show that the soft-carbon-coated, free-standing hard-carbon electrodes can achieve an ultrahigh ICE of 94.1% and long cycling performance (99% capacity retention after 100 cycles at a current density of 20 mA g -1 ), demonstrating their great potential in practical sodium storage systems. The sodium storage mechanism was also investigated by operando Raman spectroscopy. Our sodium storage mechanism extends the "adsorption-intercalation-pore filling-deposition" model. We propose that the pore filling in the plateau area might be divided into two parts: (1) sodium could fill in the pores near the inner wall of the carbon layer; (2) when the sodium in the inner wall pores is close to saturation, the sodium could be further deposited onto the existing sodium.

In China, organophosphate esters (OPEs) are widely used in indoor environments. However, there is little information regarding the internal and external exposure of university students to OPEs. Therefore, in this study, nine OPEs and eight OPE metabolites (mOPEs) were measured in indoor dust and atmospheric PM 2.5 samples from a university campus in Shanghai, as well as in urine samples collected from the university students. The total concentration of OPEs in the indoor dust in female dormitories (1420 ng/g) was approximately twice that in male dormitories (645 ng/g). In terms of indoor PM 2.5 , the highest OPE concentration was found in meeting rooms (105 ng/m 3 , on average), followed by chemical laboratories (51.2 ng/m 3 ), dormitories (44.9 ng/m 3 ), and offices (34.9 ng/m 3 ). The total concentrations of the eight mOPEs ranged from 279 pg/mL to 14,000 pg/mL, with a geometric mean value of 1590 pg/mL. The estimated daily intake values based on the indoor dust and PM 2.5 OPE samples (external exposure) were 1-2 orders of magnitude lower than that deduced from the concentration of urinary mOPEs (internal exposure), indicating that dermal contact, dust ingestion, and inhalation do not contribute significantly to OPE exposure in the general population. Moreover, additional exposure routes lead to the accumulation of OPEs in the human body.

Bismuth (Bi) has been considered as a promising alloying-type anode for potassium-ion batteries (PIBs), owing to its high theoretical capacity and suitable working voltage plateaus. However, Bi suffers from dramatic volume fluctuation and significant pulverization during the discharge/charge processes, resulting in fast capacity decay. Herein, we synthesize Bi nanoparticles confined in carbonaceous nanospheres (denoted as Bi@C) for PIBs by first utilizing BiOCl nanoflakes as a hard template and a Bi precursor. The construction of the loose structure buffers the mechanical stresses resulting from the volume expansion of Bi during the alloying reaction and avoids the fracture of the electrode structure, thus improving the cycling performance. Moreover, the carbonaceous layers increase the electronic conductivity and disperse the Bi nanoparticles, enhancing the charge transportation and ionic diffusion, which further promotes the rate capability of Bi@C. It exhibits a superior capacity (389 mAh g -1 at 100 mA g -1 after 100 cycles), excellent cycling stability (206 mAh g -1 at 500 mA g -1 over 1000 cycles), and an improved rate capability (182 mAh g -1 at 2.0 A g -1 ). This work provides a new structuring strategy in alloying materials for boosting reversible and stable potassium-ion storage.

Due to their widespread use and harmful effects on aquatic environment, sulfonamide antibiotics (SAs) have become an emerging pollutant of great concern around the world. In this study, we investigated the degradation process and mechanism of sulfamerazine (SMR), sulfadiazine (SDZ), and sulfapyridine (SPD) by electron-beam irradiation (EBI). The results showed that the three SAs were well suited to the pseudo-first-order reaction kinetics, and they could be almost completely removed with high efficiency (5 kGy). Among the environmental factors, pH (3.0) and O 2 atmosphere can further enhance the removal of the sulfonamides (SAs), while NO 2 - has the most pronounced degrading inhibitory effects among the many ions, these results illustrate that hydroxyl radicals play a dominant role. Compared with SMR and SDZ, the degree of mineralization of lower molecular weight SPD is obvious (45%). LC-MS and DFT calculations indicate that the concentrations of degradation products of the three SAs show a tendency to increase and then decrease, demonstrating that EBI can achieve efficient removal and further mineralization of SAs. Meanwhile, the results of the common product 4-Aminophenol produced during the degradation process further indicate that HO is the predominant reactive oxygen species (ROS). In addition, acute toxicity experiments with luminescent bacteria and predictions of ECOSAR procedures proved the toxic effects greatly decreased after the degradation. This study provides new ideas for achieving efficient and profound removal of emerging pollutants from 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 © 2021 Elsevier Ltd. All rights reserved.)

High-efficiency electrochemical hydrogen evolution reaction (HER) offers a promising strategy to address energy and environmental crisis. Platinum is the most effective electrocatalyst for the HER. However, challenging scarcity, valuableness, and poor electrochemical stability still hinder its wide application. Here, we designed an outstanding HER electrocatalyst, highly dispersed rhodium (Rh) nanoparticles with an average diameter of only 3 nm supported on boron (B) nanosheets. The HER catalytic activity is even comparable to that of commercial platinum catalysts, with an overpotential of only 66 mV in 0.5 M H 2 SO 4 and 101 mV in 1 M KOH to reach the current density of 10 mA cm -2 . Meanwhile, the catalyst exhibited impressive electrochemical durability during long-term electrochemical processes in acidic and alkaline media, even the simulated seawater environment. Theoretical calculations unraveled that the structure-activity relationship between B(104) crystal plane and Rh(111) crystal plane is beneficial to the release of hydrogen, and surface O plays a vital role in the catalysis process. Our work may gain insights into the development of supported metal catalysts with robust catalytic performance through precise engineering of the strong metal-supported interaction effect.

Pt-based catalysts are commercial electrocatalysts for the hydrogen evolution reaction (HER), but their shortcomings of expensive and imperfect efficiency hinder their large-scale application. Here, we report an Ir-based HER catalyst supported by N-doped carbon nanosheets (Ir-NCNSs). The NCNSs, with a high surface area and unique atomic composition, enable Ir nanoparticles (NPs) to disperse at 2-3 nm and strongly coordinate to the Ir through Ir-N bonds, which exposes many active sites and strengthens their durability. The catalyst displays a low overpotential and a small Tafel slope of 46.3 mV at 10 mA cm -2 and 52 mV dec -1 in 0.5 M H 2 SO 4 , respectively. When used in 1.0 M KOH, Ir-NCNSs also show excellent electrocatalytic activity with a low overpotential of 125 mV at 10 mA cm -2 . The calculated results further suggest that Ir NPs and NCNSs have excellent selectivity for strong metal-support interactions, corresponding to a significant and stable HER characteristic. Our findings provide insight into the design of high-efficiency Ir-based HER catalysts.

The contamination of soil by lead (Pb) is a serious and widespread problem in China, especially in mining areas. This paper summarized the available data regarding Pb-contaminated soils around various metal mines in China. Based on these data, the Pb concentration in the soil and its temporal and spatial changes were analyzed. Potential ecological hazards and adult lead models were also used to estimate ecological and health risks. The results indicated that the concentration of Pb was closely related with the type of mine. Compared with other types of mine, soil around lead-zinc (Pb-Zn) and tin (Sn) mines with high Pb contents in the metallic ores and high pollutant emission coefficient were more strongly polluted by Pb. The characteristic spatial and temporal variations of Pb pollution status in China were clarified, and the results showed that the concentration was high in the southern, southwestern, and central regions of China where many mining areas were located, and the mean value passed a turning point in 2012. Ecological risk assessments indicated that some areas around mines were at considerable to high risk, and the risk was relatively severe in Pb-Zn mining areas. According to the adult lead model, Pb-Zn mines had a greater impact on blood Pb concentration than the other types of mine.

Sodium metal is regarded as one of the most prospective next-generation anodes material owing to its high theoretical capacity, low redox potential, low cost, and natural abundance. Its most notable problem is the dendrite growth during Na plating/striping, which causes not only the safety concern but also the generation of inactive Na. Here, it is demonstrated that 2D carbon nanosheets embedded by bismuth nanoparticles (NPs) (denoted as Bi⊂CNs) serve as a robust nucleation buffer layer to endow the sodium metal anodes (SMAs) with high Coulombic efficiencies (CEs) and dendrite-free deposition during long-term cycling. The embedded Bi nanoparticles significantly reduce the nucleation barrier through the "sodiophilic" Na-Bi alloy. Meanwhile, the carbon frameworks effectively circumvent the gradual failure of those Na-Bi nucleation sites. As a result, the metallic Na on the Bi⊂CNs nucleation layer is repeatedly plated/stripped for nearly 7700 h (1287 cycles) at 3 mA h cm -2 with an average CE of 99.92%. Moreover, the Na||Na symmetric cells with the Bi⊂CNs buffer layer are stably plated/stripped for 4000 h at 1 mA cm -2 and 1 mA h cm -2 . It is found that the cycling stability is closely related to the Na utilization of SMAs and current rate., (© 2021 Wiley-VCH GmbH.)

2D MXene-based nanomaterials have attracted tremendous attention because of their unique physical/chemical properties and wide range of applications in energy storage, catalysis, electronics, optoelectronics, and photonics. However, MXenes and their derivatives have many inherent limitations in terms of energy storage applications. In order to further improve their performance for practical application, the nanoengineering of these 2D materials is extensively investigated. In this Review, the latest research and progress on 2D MXene-based nanostructures is introduced and discussed, focusing on their preparation methods, properties, and applications for energy storage such as lithium-ion batteries, sodium-ion batteries, lithium-sulfur batteries, and supercapacitors. Finally, the critical challenges and perspectives required to be addressed for the future development of these 2D MXene-based materials for energy storage applications are presented., (© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The widespread existence of antibiotics has caused inevitable influence on ecology and humans. In this study, we screened the most commonly used antibiotics, and 64 antibiotics were detected in Shanghai, an international metropolis. Most of the target substances were detected in all 46 water samples including main rivers and districts in Shanghai, with concentrations ranging from 0.02 to 502.43 ng L -1 . In particular, sulfadiazine (502.43 ng L -1 ) had the highest maximum concentration. Besides, risk quotients based on fish suggested that sulfonamides had a medium risk (0.12) in Shanghai. Correlation studies had shown that most compounds with frequencies exceeding 60% were significantly positively correlated with the total concentration. Based on further analysis, sulfadiazine, sulfamerazine, and sulfapyridine were screened as indicators to reflect the pollution status of antibiotics in Shanghai for a long time. The screening conditions for these indicators include detection rate (> 60%), maximum concentration (> 100 ng L -1 ), RQ (> 0.01), and correlation (> 0). In addition, population density may be the main factor for antibiotic pollution through regional comparison. In a word, this work can systematically reflect the overall situation of Shanghai antibiotics and provide support for global data comparison in the future. Meanwhile, we provided the potential indicators that can be applied in the long term and economical monitoring of antibiotics.

Knowing the correlation of reaction parameters in the preparation process of carbon dots (CDs) is essential for optimizing the synthesis strategy, exploring exotic properties, and exploiting potential applications. However, the integrated screening experimental data on the synthesis of CDs are huge and noisy. Machine learning (ML) has recently been successfully used for the screening of high-performance materials. Here, we demonstrate how ML-based techniques can offer insight into the successful prediction, optimization, and acceleration of CDs' synthesis process. A regression ML model on hydrothermal-synthesized CDs is established capable of revealing the relationship between various synthesis parameters and experimental outcomes as well as enhancing the process-related properties such as the fluorescent quantum yield (QY). CDs exhibiting a strong green emission with QY up to 39.3% are obtained through the combined ML guidance and experimental verification. The mass of precursors and the volume of alkaline catalysts are identified as the most important features in the synthesis of high-QY CDs by the trained ML model. The CDs are applied as an ultrasensitive fluorescence probe for monitoring the Fe 3+ ion because of their superior optical behaviors. The probe exhibits the linear response to the Fe 3+ ion with a wide concentration range (0-150 μM), and its detection limit is 0.039 μM. Our findings demonstrate the great capability of ML to guide the synthesis of high-quality CDs, accelerating the development of intelligent material.

Under ambient conditions, the only known valence state of calcium ions is +2, and the corresponding crystals with calcium ions are insulating and nonferromagnetic. Here, using cryo-electron microscopy, we report direct observation of two-dimensional (2D) CaCl crystals on reduced graphene oxide (rGO) membranes, in which the calcium ions are only monovalent (i.e. +1). Remarkably, metallic rather than insulating properties are displayed by those CaCl crystals. More interestingly, room-temperature ferromagnetism, graphene-CaCl heterojunction, coexistence of piezoelectricity-like property and metallicity, as well as the distinct hydrogen storage and release capability of the CaCl crystals in rGO membranes are experimentally demonstrated. We note that such CaCl crystals are obtained by simply incubating rGO membranes in salt solutions below the saturated concentration, under ambient conditions. Theoretical studies suggest that the formation of those abnormal crystals is attributed to the strong cation-π interactions of the Ca cations with the aromatic rings in the graphene surfaces. The findings highlight the realistic potential applications of such abnormal CaCl material with unusual electronic properties in designing novel transistors and magnetic devices, hydrogen storage, catalyzers, high-performance conducting electrodes and sensors, with a size down to atomic scale., (© The Author(s) 2020. Published by Oxford University Press on behalf of China Science Publishing & Media Ltd.)

Quantum dots have innate advantages as the key component of optoelectronic devices. For white light-emitting diodes (WLEDs), the modulation of the spectrum and color of the device often involves various quantum dots of different emission wavelengths. Here, we fabricate a series of carbon quantum dots (CQDs) through a scalable acid reagent engineering strategy. The growing electron-withdrawing groups on the surface of CQDs that originated from acid reagents boost their photoluminescence wavelength red shift and raise their particle sizes, elucidating the quantum size effect. These CQDs emit bright and remarkably stable full-color fluorescence ranging from blue to red light and even white light. Full-color emissive polymer films and all types of high-color rendering index WLEDs are synthesized by mixing multiple kinds of CQDs in appropriate ratios. The universal electron-donating/withdrawing group engineering approach for synthesizing tunable emissive CQDs will facilitate the progress of carbon-based luminescent materials for manufacturing forward-looking films and devices., (Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).)

Enslaved to the large-size K-ions, the construction of suitable anode materials with superior and stable potassium-ion storage properties is a major challenge. 1T phase MoS 2 possesses higher conductivity, bigger interlayer distance, and more electrochemically active sites than the 2H phase, which offers intriguing benefits for energy-related applications. In this work, the 1T/2H-phase hybrid MoS 2 nanosheets are successfully anchored in the N-doped carbon nanotube hollow polyhedron (1T/2H-MoS 2 /NCNHP) by a bottom-up solvothermal method. For the synthesized 1T/2H-MoS 2 /NCNHP, the fewer-layer 1T/2H-MoS 2 nanosheets are embedded in an N-doped carbon nanotube hollow polyhedron, with an enlarged interlayer spacing of 0.96 nm. When evaluated as anode material for potassium-ion batteries, the 1T/2H-MoS 2 /NCNHP hybrid presents outstanding potassium storage performance. It delivers a high-specific capacity of 519.2 mAh g -1 at 50 mA g -1 and maintains 281.2 mAh g -1 at 1 A g -1 over 500 cycles. The good potassium-ion electrochemical performance is attributed to the rational structural design and the synergistic effect of the components. Moreover, the 1T-MoS 2 nanosheet has excellent electrical conductivity and its enlarged interlayer spacing reduces the barrier for the embedding and stripping of K ions. Finally, the practical application of the 1T/2H-MoS 2 /NCNHP electrode material is also evaluated by assembled K-ion full cells., (© 2020 Wiley-VCH GmbH.)