Microbial communities play crucial roles in pollutant removal and system stability in biological systems for coking wastewater(CWW)treatment,but a comprehensive understanding of their structure and functions is still ...Microbial communities play crucial roles in pollutant removal and system stability in biological systems for coking wastewater(CWW)treatment,but a comprehensive understanding of their structure and functions is still lacking.A five month survey of four sequential bioreactors,anoxic 1/oxic 1/anoxic 2/oxic 2(A1/O1/A2/O2),was carried out in a full-scale CWW treatment system in China to elucidate operational performance and microbial ecology.The results showed that A1/O1/A2/O2 had excellent and stable performance for nitrogen removal.Both total nitrogen(TN;(17.38±6.89)mgL1)and ammonium-nitrogen(NH4 t-N;(2.10±1.34)mg·L^(-1))in the final biological effluent satisfied the Chinese national standards for CWW.Integrated analysis of 16S ribosome RNA(rRNA)sequencing and metagenomic sequencing showed that the bacterial communities and metagenomic function profiles of A1 and O1 shared similar functional structures,while those of A2 significantly varied from those of other bioreactors(p<0.05).The results indicated that microbial activity was strongly connected with activated sludge function.Nitrosospira,Nitrosomonas,and SM1A02 were responsible for nitrification during the primary anoxic-oxic(AO)stage and Azoarcus and Thauera acted as important denitrifiers in A2.Nitrogen cycling-related enzymes and genes work in the A1/O1/A2/O2 system.Moreover,the hao genes catalyzing hydroxylamine dehydrogenase(EC 1.7.2.6)and the napA and napB genes catalyzing nitrate reductase(EC 1.9.6.1)played important roles in the nitrification and denitrification processes in the primary and secondary AO stages,respectively.The mixed liquor suspended solids(MLSS)/total solids(TS),TN removal rate(RR),total organic carbon(TOC)(RR),and NH_(4)^(+)t-N(RR)were the most important environmental factors for regulating the structure of core bacterial genera and nitrogen-cycling genes.Proteobacteria were the potential main participants in nitrogen metabolism in the A1/O1/A2/O2 system for CWW treatment.This study provides an original and comprehensive understanding of the microbial community and functions at the gene level,which is crucial for the efficient and stable operation of the full-scale biological process for CWW treatment.展开更多
Despite the extensive application of advanced oxidation processes(AOPs)in water treatment,the efficiency of AOPs in eliminating various emerging contaminants such as halogenated antibiotics is constrained by a number ...Despite the extensive application of advanced oxidation processes(AOPs)in water treatment,the efficiency of AOPs in eliminating various emerging contaminants such as halogenated antibiotics is constrained by a number of factors.Halogen moieties exhibit strong resistance to oxidative radicals,affecting the dehalogenation and detoxification efficiencies.To address these limitations of AOPs,advanced reduction processes(ARPs)have been proposed.Herein,a novel nucleophilic reductant—namely,the carbon dioxide radical anion(CO_(2)^(·-))—is introduced for the simultaneous degradation,dehalogenation,and detoxification of florfenicol(FF),a typical halogenated antibiotic.The results demonstrate that FF is completely eliminated by CO_(2)^(·-),with approximately 100%of Cland 46%of Freleased after 120 min of treatment.Simultaneous detoxification is observed,which exhibits a linear response to the release of free inorganic halogen ions(R^(2)=0.97,p<0.01).The formation of halogen-free products is the primary reason for the superior detoxification performance of this method,in comparison with conventional hydroxyl-radical-based AOPs.Products identification and density functional theory(DFT)calculations reveal the underlying dehalogenation mechanism,in which the chlorine moiety of FF is more susceptible than other moieties to nucleophilic attack by CO_(2)^(·-).Moreover,CO_(2)^(·-)-based ARPs exhibit superior dehalogenation efficiencies(>75%)in degrading a series of halogenated antibiotics,including chloramphenicol(CAP),thiamphenicol(THA),diclofenac(DLF),triclosan(TCS),and ciprofloxacin(CIP).The system shows high tolerance to the pH of the solution and the presence of natural water constituents,and demonstrates an excellent degradation performance in actual groundwater,indicating the strong application potential of CO_(2)^(·-)-based ARPs in real life.Overall,this study elucidates the feasibility of CO_(2)^(·-)for the simultaneous degradation,dehalogenation,and detoxification of halogenated antibiotics and provides a promising method for their regulation during water or wastewater treatment.展开更多
Municipal solid waste(MSW)is an important destination for abandoned plastics.During the waste disposal process,large plastic debris is broken down into microplastics(MPs)and released into the leachate.However,current ...Municipal solid waste(MSW)is an important destination for abandoned plastics.During the waste disposal process,large plastic debris is broken down into microplastics(MPs)and released into the leachate.However,current research only focuses on landfill leachates,and the occurrence of MPs in other leachates has not been studied.Therefore,herein,the abundance and characteristics of MPs in three types of leachates,namely,landfill leachate,residual waste leachate,and household food waste leachate,were studied,all leachates were collected from the largest waste disposal center in China.The results showed that the average MP abundances in the different types of leachates ranged from(129±54)to(1288±184)MP particles per liter(particlesL1)and the household food waste leachate exhibited the highest MP abundance(p<0.05).Polyethylene(PE)and fragments were the dominant polymer type and shape in MPs,respectively.The characteristic polymer types of MPs in individual leachates were different.Furthermore,the conditional fragmentation model indicated that the landfilling process considerably affected the size distribution of MPs in leachates,leading to a higher percentage(>80%)of small MPs(20–100 lm)in landfill leachates compared to other leachates.To the best of our knowledge,this is the first study discussing the sources of MPs in different leachates,which is important for MP pollution control during MSW disposal.展开更多
This study explores household solid waste management (HSWM) practices and awareness among residents of Windhoek West, a rapidly urbanizing constituency in the Khomas Region of Namibia. Employing a descriptive methodol...This study explores household solid waste management (HSWM) practices and awareness among residents of Windhoek West, a rapidly urbanizing constituency in the Khomas Region of Namibia. Employing a descriptive methodology, the research investigates the interplay between public awareness, regulatory frameworks, and the availability of waste management facilities to assess their impact on waste management behaviors. Our findings indicate significant gaps in both knowledge and infrastructure that hinder effective waste management. The study reveals that while there is a high willingness among residents to engage in recycling and waste reduction, actual practices are limited due to inadequate facilities and lack of stringent enforcement of waste policies. This research identifies key factors that influence waste management practices, including demographic characteristics and access to waste management facilities. It also proposes actionable strategies such as expanding recycling and sorting facilities, enhancing educational campaigns tailored to local needs, and implementing regular enforcement mechanisms. These strategies are aimed at improving compliance with waste management protocols and fostering a culture of environmental responsibility. The results of this investigation show the critical role of ongoing education and infrastructural improvement in bridging existing knowledge gaps and facilitating effective waste management practices. This research lays a foundational step toward enhancing sustainable urban development and effective waste management in Windhoek, providing valuable insights for policymakers, community leaders, and stakeholders engaged in urban environmental management.展开更多
Species diversity of angiosperms(flowering plants) varies greatly among regions.Geographic patterns of variation in species diversity are shaped by the interplay of ecological and evolutionary processes.Here,using a c...Species diversity of angiosperms(flowering plants) varies greatly among regions.Geographic patterns of variation in species diversity are shaped by the interplay of ecological and evolutionary processes.Here,using a comprehensive data set for regional angiosperm floras across the world,we show geographic patterns of taxonomic(species) diversity,phylogenetic diversity,phylogenetic dispersion,and phylogenetic deviation(i.e.,phylogenetic diversity after accounting for taxonomic diversity) across the world.Phylogenetic diversity is strongly and positively correlated with taxonomic diversity;as a result,geographic patterns of taxonomic and phylogenetic diversity across the world are highly similar.Areas with high taxonomic and phylogenetic diversity are located in tropical regions whereas areas with low taxonomic and phylogenetic diversity are located in temperate regions,particularly in Eurasia and North America,and in northern Africa.Similarly,phylogenetic dispersion is,in general,higher in tropical regions and lower in temperate regions.However,the geographic pattern of phylogenetic deviation differs substantially from those of taxonomic and phylogenetic diversity and phylogenetic dispersion.As a result,hotspots and coldspots of angiosperm diversity identified based on taxonomic and phylogenetic diversity and phylogenetic dispersion are incongruent with those identified based on phylogenetic deviations.Each of these metrics may be considered when selecting areas to be protected for their biodiversity.展开更多
Photoelectrochemical(PEC) technology provides a promising prospect for the transformation of polyethylene terephthalate(PET) plastic wastes to produce value-added chemicals.The PEC catalytic systems with high activity...Photoelectrochemical(PEC) technology provides a promising prospect for the transformation of polyethylene terephthalate(PET) plastic wastes to produce value-added chemicals.The PEC catalytic systems with high activity,selectivity and long-term durability are required for the future up-scaling industrial applications.Herein,we employed the interfacial modification strategy to develop an efficient and stable photoanode and evaluated its PEC activity for ethylene glycol(EG,derived from PET hydrolysate) oxidation to formic acid.The interfacial modification between Fe_(2)O_(3)semiconductor and Ni(OH)xcocatalyst with ultrathin TiO_(x) interlayer not only improved the photocurrent density by accelerating the kinetics of photogenerated charge carriers,but also kept the high Faradaic efficiency(over 95% in 30 h) towards the value-added formic acid product.This work proposes an effective method to promote the PEC activity and enhance the long-term stability of photoelectrodes for upcycling PET plastic wastes.展开更多
The removal of emerging micropollutants in the aquatic environment remains a global challenge.Conventional routes are often chemically,energetically,and operationally intensive,which decreases their sustainability dur...The removal of emerging micropollutants in the aquatic environment remains a global challenge.Conventional routes are often chemically,energetically,and operationally intensive,which decreases their sustainability during applications.Herein,we develop an advanced chemical-free strategy for micropollutants decontamination that is solely based on sequential electrochemistry involving ubiquitous sulfate anions in natural and engineered waters.This can be achieved via a chain reaction initiated by electrocatalytic anodic sulfate(SO_(4)^(2-))oxidation to produce persulfate(S_(2)O_(8)^(2-))and followed by a cathodic persulfate reduction to produce sulfate radicals(SO_(4)^(·-)).These SO_(4)^(·-)are powerful reactive species that enable the unselective degradation of micropollutants and yield SO_(4)^(2-)again in the treated water.The proposed flow-through electrochemical system achieves the efficient degradation(100.0%)and total organic carbon removal(65.0%)of aniline under optimized conditions with a single-pass mode.We also reveal the effectiveness of the proposed system for the degradation of a wide array of emerging micropollutants over a broad pH range and in complex matrices.This work provides the first proof-ofconcept demonstration using ubiquitous sulfate for micropollutants decontamination,making water purification more sustainable and more economical.展开更多
The deoxygenation of organic acids, important biomass feedstocks and derivatives, to synthesize hydrocarbon products under mild electrochemical conditions, holds significant importance for the production of carbon-neu...The deoxygenation of organic acids, important biomass feedstocks and derivatives, to synthesize hydrocarbon products under mild electrochemical conditions, holds significant importance for the production of carbon-neutral biofuels. There is still limited research on the influential factors of the electrochemical decarboxylation reaction of medium-chain fatty acids. In this study, n-octanoic acid (OA) was chosen as the research subject to investigate the electrochemical decarboxylation behavior of OA on a platinum electrode, focusing on the influence of different alkali metal cations (Li^(+), Na^(+), K^(+)), common anions (SO^(4)^(2−), Cl^(−)), and electrolyte pH. It was found that KOH as an electrolyte exhibited the best performance for OA. Possibly, the larger size of K^(+) increased the alkalinity of the electrode surface, facilitating OA deprotonation. LiOH electrolyte reduced the solubility of OA, thereby inhibiting the decarboxylation reaction. SO^(4)^(2−) exhibited a weak promoting effect on the decarboxylation reaction of OA, while Cl^(−) showed no adverse effect although Cl^(−) may adsorb on the electrode surface. Furthermore, unlike short-chain fatty acids, medium-chain OA can only achieve efficient decarboxylation under alkaline conditions due to its solubility properties. This study provides references and foundations for future efforts to enhance the efficiency of electrochemical decarboxylation synthesis of hydrocarbon biofuels from medium-chain fatty acids.展开更多
Objective Our objective was to investigate the occurrence of opportunistic pathogens and characterize the bacterial community structures in the water system of a pulmonary hospital.Methods The water samples were colle...Objective Our objective was to investigate the occurrence of opportunistic pathogens and characterize the bacterial community structures in the water system of a pulmonary hospital.Methods The water samples were collected from automatic and manual faucets in the consulting room,treatment room,dressing room,respiratory ward,and other non-medical rooms in three buildings of the hospital.Quantitative polymerase chain reaction was used to quantify the load of several waterborne opportunistic pathogens and related microorganisms,including Legionella spp.,Mycobacterium spp.,and M.avium.Illumina sequencing targeting 16 S r RNA genes was performed to profile bacterial communities.Results The occurrence rates of Legionella spp.,Mycobacterium spp.,and M.avium were 100%,100%,and 76%,respectively in all samples.Higher occurrence rates of M.avium were observed in the outpatient service building(building 1,91.7%)and respiration department and wards(building 2,80%)than in the office building(building 3),where no M.avium was found.M.avium were more abundant in automatic faucets(average 2.21×10~4 gene copies/L)than in manual faucets(average 1.03×10~4 gene copies/m L)(P<0.01).Proteobacteria,Actinobacteria,Bacteroidetes,Cyanobacteria,Firmicutes,and Acidobacteria were the dominant bacterial phyla.Disinfectant residuals,nitrate,and temperature were found to be the key environmental factors driving microbial community structure shifts in water systems.Conclusion This study revealed a high level of colonization of water faucets by opportunistic pathogens and provided insight into the characteristics of microbial communities in a hospital water system and approaches to reduce risks of microbial contamination.展开更多
Graphene, a well-known two-dimensional(2 D) material, has sparked broad enthusiasm in both scientific and industrial communities in these years, due to its exceptional electrical, thermal, mechanical, and versatile pr...Graphene, a well-known two-dimensional(2 D) material, has sparked broad enthusiasm in both scientific and industrial communities in these years, due to its exceptional electrical, thermal, mechanical, and versatile properties. However, many properties and applications of graphene are layer-number dependent. The preparation of high-quality graphene with controlled layer numbers is full of challenge, since the layer number varies much with the synthesis routes and relevant experimental conditions. Hence, there is an urgent need to improve the layer-number controllability of graphene preparation. Generally, graphene can be prepared by two complementary approaches: "top-down" and "bottom-up". Since they have their own advantages, the recent advances in the layer-number tunable preparation of high-quality graphene are separately studied from the two aspects in this review, especially those dedicated to single parameter. Some effective strategies are discussed in detail, mainly including 1) supercritical-CO2 assisted sonication, electrochemical exfoliation of graphite intercalation compounds, and layer-by-layer thinning with plasma or laser, for "top-down" graphene;2) chemical vapor deposition(CVD) on dual-metal substrate, ion-implantation CVD, layer-by-layer CVD, plasma-enhanced CVD, layered-double-hydroxides template-assisted CVD;and 3) graphite-enclosure assisted epitaxial growth and pulsed-magnetron-sputtering assisted physical vapor deposition for "bottom-up" graphene on various substrates. In addition, the respective advantages of graphene with different layer numbers in properties and applications are also presented. Finally, the contribution concludes with some important perspectives on the remained challenges and future perspectives.展开更多
Iron and oxalic acids are widely distributed in the atmosphere and easily form ferric oxalate complex(Fe(III)-Ox).The tropospheric aqueous-phase could provide a medium to enable the photo-Fenton reaction with Fe(III)-...Iron and oxalic acids are widely distributed in the atmosphere and easily form ferric oxalate complex(Fe(III)-Ox).The tropospheric aqueous-phase could provide a medium to enable the photo-Fenton reaction with Fe(III)-Ox under solar irradiation.Although the photolysis mechanisms of Fe(III)-Ox have been investigated extensively,information about the oxidation of volatile organic compounds(VOC),specifically the potential for Secondary Organic Aerosol(SOA)formation in the Fe(III)-Ox system,is lacking.In this study,a ubiquitous VOC methacrolein(MACR)is chosen as a model VOC,and the oxidation of MACR with Fe(III)-Ox is investigated under typical atmospheric water conditions.The effects of oxalate concentration,Fe(III)concentration,MACR concentration,and pH on the oxidation of MACR are studied in detail.Results show that the oxidation rate of MACR greatly accelerates in the presence of oxalate when compared with only Fe(III).The oxidation rate of MACR also accelerates with increasing concentration of oxalate.The effect of Fe(III)is found to be more complicated.The oxidation rate of MACR first increases and then decreases with increasing Fe(III)concentration.The oxidation rate of MACR increases monotonically with decreasing pH in the common atmospheric water pH range or with decreasing MACR concentration.The production of ferrous and hydrogen peroxide,pH,and aqueous absorbance are monitored throughout the reaction process.The quenching experiments verify that·OH and O_(2)^(+)are both responsible for the oxidation of MACR.MACR is found to rapidly oxidize into small organic acids with higher boiling points and oligomers with higher molecular weight,which contributes to the yield of SOA.These results suggest that Fe(III)-Ox plays an important role in atmospheric oxidation.展开更多
Nitrogen is the most important component for living beings while the excessive discharge of organic and inorganic nitrogen may create severe environmental problems.In this study,a continuous anoxic/oxic(A/O)reactor ad...Nitrogen is the most important component for living beings while the excessive discharge of organic and inorganic nitrogen may create severe environmental problems.In this study,a continuous anoxic/oxic(A/O)reactor adopting activated sludge and sludge biofilms in the anoxic and oxic zones was applied for total nitrogen(TN)and chemical oxygen demand(COD)removal,and the efficiencies of nitrification and denitrification were compared as well.Results showed that when using activated sludge,the effluent concentrations of NH_(4)^(+)-N,NO_(3)^(-)-N,NO_(2)^(-)-N,TN and COD were inconsistent and fluctuated greatly,and the removal efficiencies of corresponding nitrification,denitrification and TN were also unstable;the obtained average COD removal efficiency was 85%.While using sludge biofilms,the acquired effluent concentrations of NH^(+)_(4)-N,NO^(-)_(3)-N,NO_(2)^(-)-N,TN and COD became stable and constant.The nitrification,denitrification,TN and COD removal efficiencies were 96%,84%and 65%and 94%,respectively.Bacterial community analysis of sludge biofilms indicated that the genus Arcobacter was the major denitrifiers in the anoxic zone with relative abundance of 76.1%,and in the oxic zone the abundances of Acinetobacter,Hydrogenophaga and Nitrospira responsible for complete nitrification were 20.05%,7.6%and 3.7%respectively.The high abundance of nitrifying bacteria and denitrifiers were related with the high and stable nitrogen and COD removal.展开更多
Electrocatalytic reduction of ethylenediamine tetraacetic acid copper(CuEDTA),a typical refractory heavy metal complexation pollutant,is an environmental benign method that operates at mild condition.Unfortunately,the...Electrocatalytic reduction of ethylenediamine tetraacetic acid copper(CuEDTA),a typical refractory heavy metal complexation pollutant,is an environmental benign method that operates at mild condition.Unfortunately,the selective reduction of CuEDTA is still a big challenge in cathodic process.In this work,we report a MoS_(2) nanosheet/graphite felt(GF)cathode,which achieves an average Faraday efficiency of 29.6%and specific removal rate(SRR)of 0.042 mol/cm^(2)/h for CuEDTA at−0.65 V vs SCE(saturated calomel electrode),both of which are much higher than those of the commonly reported electrooxidation technology-based removal systems.Moreover,a proofof-concept CuEDTA/Zn battery with Zn anode and MoS_(2)/GF cathode is demonstrated,which has bifunctions of simultaneous CuEDTA removal and energy output.This is one of the pioneer studies on the electrocatalytic reduction of heavy metal complex and CuEDTA/Zn battery,which brings new insights in developing efficient electrocatalytic reduction system for pollution control and energy output.展开更多
Hydrogen peroxide(H_(2)O_(2))in situ electrosynthesis by O_(2)reduction reaction is a promising alternative to the conventional Fenton treatment of refractory wastewater.However,O_(2)mass transfer limitation,cathodic ...Hydrogen peroxide(H_(2)O_(2))in situ electrosynthesis by O_(2)reduction reaction is a promising alternative to the conventional Fenton treatment of refractory wastewater.However,O_(2)mass transfer limitation,cathodic catalyst selectivity,and electron transfer in O_(2)reduction remain major engineering obstacles.Here,we have proposed a systematic solution for efficient H_(2)O_(2)generation and its electro-Fenton(EF)application for refractory organic degradation based on the fabrication of a novel ZrO_(2)/CMK-3/PTFE cathode,in which polytetrafluoroethylene(PTFE)acted as a hydrophobic modifier to strengthen the O_(2)mass transfer,ZrO_(2)was adopted as a hydrophilic modifier to enhance the electron transfer of O_(2)reduction,and mesoporous carbon CMK-3 was utilized as a catalyst substrate to provide catalytic active sites.Moreover,feasible mass transfer of O_(2)from the hydrophobic to the hydrophilic layer was designed to increase the contact between O_(2)and the reaction interface.The H_(2)O_(2)yield of the ZrO_(2)/CMK-3/PTFE cathode was significantly improved by approximately 7.56 times compared to that of the co nventional gas diffusion cathode under the same conditions.The H_(2)O_(2)generation rate and Faraday efficiency reached125.98 mg·cm^(-2)·h^(-1)(normalized to 5674.04 mmol·g^(-1)·h^(-1)by catalyst loading)and 78.24%at-1.3 V versus standard hydrogen electrode(current density of-252 mA·cm^(-2)),respectively.The high H_(2)O_(2)yield ensured that sufficient OH was produced for excellent EF performance,resulting in a degradation efficiency of over 96%for refractory organics.This study offers a novel engineering solution for the efficient treatment of refractory wastewater using EF technology based on in situ high-yield H_(2)O_(2)electrosynthesis.展开更多
Recalcitrance and the inherent heterogeneity of lignin structure are the major bottlenecks to impede the popularization of lignin-based chemicals production processes.Recent works suggested a promising pathway for lig...Recalcitrance and the inherent heterogeneity of lignin structure are the major bottlenecks to impede the popularization of lignin-based chemicals production processes.Recent works suggested a promising pathway for lignin depolymerization and lignin-derived bio-oil upgrading via an electrochemical biorefinery(a process in which lignin valorization is performed via electrochemical oxidation or reduction).This review presents the progress on chemicals synthesis and bio-oil upgrading from lignin by an electrochemical biorefinery,relating to the lignin biosynthesis pathway,reaction pathway of lignin electrochemical conversion,inner-sphere and outer-sphere electron transfer mechanism,basic kinetics and thermodynamics in electrochemistry,and the recent embodiments analysis with the emphasis on the respective feature and limitation for lignin electrochemical oxidative and reductive conversion.Lastly,the challenge and perspective associated with lignin electrochemical biorefinery are discussed.Present-day results indicate that more work should be performed to promote efficiency,selectivity,and stability in pursuing a lignin electrochemical biorefinery.One of the most promising developing directions appears to be integrating various types of lignin electrochemical conversion strategies and other existing or evolving lignin valorization technologies.This review aims to provide more references and discussion on the development for lignin electrochemical biorefinery.展开更多
The electrocatalytic carbon dioxide reduction reaction(eCO_(2)RR)into high-value-added chemicals and fuels is a promising strategy to mitigate global warming.However,it remains a significant stumbling block to the rat...The electrocatalytic carbon dioxide reduction reaction(eCO_(2)RR)into high-value-added chemicals and fuels is a promising strategy to mitigate global warming.However,it remains a significant stumbling block to the rationally tuning lattice plane of the catalyst with high activity to produce the target product in the eCO_(2)RR process.To attempt to solve this problem,the Culn bimetallic alloy nanocatalyst with specifically exposed lattice planes is modulated and electrodeposited on the nitrogen-doped porous carbon cloth by a simple two-step electrodeposition method,which induces high Faraday efficiency of 80%towards HCOO-(FEHCOO-)with a partial current density of 13.84 mA cm-2at-1.05 V(vs.RHE).Systematic characterizations and theoretical modeling reveal that the specific coexposed Culn(200)and In(101)lattice facets selectively adsorbed the key intermediate of OCHO*,reducing the overpotential of HCOOH and boosting the FEHCOO-in a wide potential window(-0.65--1.25 V).Moreover,a homogeneous distribution of Culn nanoparticles with an average diameter of merely~3.19 nm affords exposure to abundant active sites,meanwhile prohibiting detachment and agglomeration of nanoparticles during eCO_(2)RR for enhanced stability attributing to the self-assembly electrode strategy.This study highlights the synergistic effect between catalytic activity and facet effect,which opens a new route in surface engineering to tune their electrocatalytic performance.展开更多
Anaerobic digestion(AD)of organic fraction of municipal solid waste(OFMSW)is prone to system breakdown under high organic loading rates(OLRs)condition,which subsequently reduces the efficiency of digestion process and...Anaerobic digestion(AD)of organic fraction of municipal solid waste(OFMSW)is prone to system breakdown under high organic loading rates(OLRs)condition,which subsequently reduces the efficiency of digestion process and results in substantial economic losses.In this perspective paper,the substances metabolisms,electrons flow,as well as microbial interaction mechanisms within AD process are comprehensively discussed,and the underlying bottleneck that causes inefficient methane production is identified,which is“electrons surplus”.Systems encountering severe electron surplus are at risk of process failure,making it crucial to proactively prevent this phenomenon through appropriate approaches.On this basis,the present perspective proposes three potential electronic regulation strategies to prevent electrons surplus,namely,electron shunt,accelerating electron transfer and regulating methanogenic metabolism pathway,and presents specific methodologies for each strategy.Furthermore,the potential solutions to challenges that may occur during the electronic regulation process are also presented in this paper.This perspective aims to provide innovative approaches to achieve the efficient and stable operation of OFMSW anaerobic digestion,especially under high OLRs condition.展开更多
The deep-learning protein structure prediction method AlphaFold2 has garnered enormous attention beyond the realm of structural biology,for its groundbreaking contribution to solving the"protein foiding problem&q...The deep-learning protein structure prediction method AlphaFold2 has garnered enormous attention beyond the realm of structural biology,for its groundbreaking contribution to solving the"protein foiding problem"In this perspective,we explore the connection between protein structure studies and environmental research,delving into the potential for addressing specific environmental challenges.Proteins are promising for environmental applications because of the functional diversity endowed by their structural complexity.However,structural studies on proteins with environmental significance remain scarce.Here,we present the opportunity to study proteins by advancing experimental determination and deep-learning prediction methods.Specifically,the latest progress in environmental research via cryogenic electron microscopy is highlighted.It allows us to determine the structure of protein complexes in their native state within cells at molecular resolution,revealing environmentally-associated structural dynamics.With the remarkable advancements in computational power and experimental resolution,the study of protein structure and dynamics has reached unprecedented depth and accuracy.These advancements will undoubtedly accelerate the establishment of comprehensive environmental protein structural and functional databases.Tremendous opportunities for protein engineering exist to enable innovative solutions for environmental applications,such as the degradation of persistent contaminants,and the recovery of valuable metals as well as rare earth elements.展开更多
Tetramethylammonium hydroxide(TMAH)is an important compound that utilized and released by the rapidly expanding semiconductor industry,which could hardly be removed by the conventional wastewater treatment techniques....Tetramethylammonium hydroxide(TMAH)is an important compound that utilized and released by the rapidly expanding semiconductor industry,which could hardly be removed by the conventional wastewater treatment techniques.As a cholinergic agonist,the tetramethylammonium ion(TMA^(+))has been reported to induce toxicity to muscular and respiratory systems of mammals and human,however the toxicity on aquatic biota remains poorly known.We investigated the neurotoxic effects of TMA^(+)exposure on zebrafish,based on neurobehavior tests and a series of biomarkers.Significant inhibitions on the swimming distance of zebrafish larvae were observed when the exposure level exceeded 50 mg/L,and significant alterations on swimming path angles(straight and deflective movements)occurred even at 10 mg/L.The tested neurobehavioral endpoints of zebrafish larvae were significantly positively correlated with reactive oxygen species(ROS)and malondialdehyde(MDA),significantly negatively related with the activities of antioxidant enzymes,but not significantly correlated with the level of acetylcholinesterase(AChE).Such relationship indicates that the observed neurotoxic effects on swimming behavior of zebrafish larvae is mainly driven by oxidative stress,rather than the alterations of neurotransmitter.At the highest exposure concentration(200 mg/L),TMA^(+)evoked more severe toxicity on zebrafish juveniles,showing significantly stronger elevation on the MDA activity,and greater inhibitions on the activities of antioxidant enzymes and ACh E,suggesting juveniles were more susceptible to TMA^(+)exposure than larval zebrafish.展开更多
基金financially supported by the National Natural Science Foundation of China(52270076 and 51922078)the China Baowu Low Carbon Metallurgy Innovation Foundation(BWLCF202105).
文摘Microbial communities play crucial roles in pollutant removal and system stability in biological systems for coking wastewater(CWW)treatment,but a comprehensive understanding of their structure and functions is still lacking.A five month survey of four sequential bioreactors,anoxic 1/oxic 1/anoxic 2/oxic 2(A1/O1/A2/O2),was carried out in a full-scale CWW treatment system in China to elucidate operational performance and microbial ecology.The results showed that A1/O1/A2/O2 had excellent and stable performance for nitrogen removal.Both total nitrogen(TN;(17.38±6.89)mgL1)and ammonium-nitrogen(NH4 t-N;(2.10±1.34)mg·L^(-1))in the final biological effluent satisfied the Chinese national standards for CWW.Integrated analysis of 16S ribosome RNA(rRNA)sequencing and metagenomic sequencing showed that the bacterial communities and metagenomic function profiles of A1 and O1 shared similar functional structures,while those of A2 significantly varied from those of other bioreactors(p<0.05).The results indicated that microbial activity was strongly connected with activated sludge function.Nitrosospira,Nitrosomonas,and SM1A02 were responsible for nitrification during the primary anoxic-oxic(AO)stage and Azoarcus and Thauera acted as important denitrifiers in A2.Nitrogen cycling-related enzymes and genes work in the A1/O1/A2/O2 system.Moreover,the hao genes catalyzing hydroxylamine dehydrogenase(EC 1.7.2.6)and the napA and napB genes catalyzing nitrate reductase(EC 1.9.6.1)played important roles in the nitrification and denitrification processes in the primary and secondary AO stages,respectively.The mixed liquor suspended solids(MLSS)/total solids(TS),TN removal rate(RR),total organic carbon(TOC)(RR),and NH_(4)^(+)t-N(RR)were the most important environmental factors for regulating the structure of core bacterial genera and nitrogen-cycling genes.Proteobacteria were the potential main participants in nitrogen metabolism in the A1/O1/A2/O2 system for CWW treatment.This study provides an original and comprehensive understanding of the microbial community and functions at the gene level,which is crucial for the efficient and stable operation of the full-scale biological process for CWW treatment.
基金financially supported by the National Natural Science Foundation of China(22176059,21777042,and 22076045)the authors would also like to acknowledge support from the Science and Technology Commission of Shanghai Municipality’s Yangfan Special Project(23YF1408400)the Fundamental Research Funds for the Central Universities.
文摘Despite the extensive application of advanced oxidation processes(AOPs)in water treatment,the efficiency of AOPs in eliminating various emerging contaminants such as halogenated antibiotics is constrained by a number of factors.Halogen moieties exhibit strong resistance to oxidative radicals,affecting the dehalogenation and detoxification efficiencies.To address these limitations of AOPs,advanced reduction processes(ARPs)have been proposed.Herein,a novel nucleophilic reductant—namely,the carbon dioxide radical anion(CO_(2)^(·-))—is introduced for the simultaneous degradation,dehalogenation,and detoxification of florfenicol(FF),a typical halogenated antibiotic.The results demonstrate that FF is completely eliminated by CO_(2)^(·-),with approximately 100%of Cland 46%of Freleased after 120 min of treatment.Simultaneous detoxification is observed,which exhibits a linear response to the release of free inorganic halogen ions(R^(2)=0.97,p<0.01).The formation of halogen-free products is the primary reason for the superior detoxification performance of this method,in comparison with conventional hydroxyl-radical-based AOPs.Products identification and density functional theory(DFT)calculations reveal the underlying dehalogenation mechanism,in which the chlorine moiety of FF is more susceptible than other moieties to nucleophilic attack by CO_(2)^(·-).Moreover,CO_(2)^(·-)-based ARPs exhibit superior dehalogenation efficiencies(>75%)in degrading a series of halogenated antibiotics,including chloramphenicol(CAP),thiamphenicol(THA),diclofenac(DLF),triclosan(TCS),and ciprofloxacin(CIP).The system shows high tolerance to the pH of the solution and the presence of natural water constituents,and demonstrates an excellent degradation performance in actual groundwater,indicating the strong application potential of CO_(2)^(·-)-based ARPs in real life.Overall,this study elucidates the feasibility of CO_(2)^(·-)for the simultaneous degradation,dehalogenation,and detoxification of halogenated antibiotics and provides a promising method for their regulation during water or wastewater treatment.
基金supported by the National Key Research and Development Program of China(2023YFC3711600)the National Natural Science Foundation of China(22076045 and 22376066)the Shanghai Talent Development Funding,and the Shanghai Youth Talent Support Program.
文摘Municipal solid waste(MSW)is an important destination for abandoned plastics.During the waste disposal process,large plastic debris is broken down into microplastics(MPs)and released into the leachate.However,current research only focuses on landfill leachates,and the occurrence of MPs in other leachates has not been studied.Therefore,herein,the abundance and characteristics of MPs in three types of leachates,namely,landfill leachate,residual waste leachate,and household food waste leachate,were studied,all leachates were collected from the largest waste disposal center in China.The results showed that the average MP abundances in the different types of leachates ranged from(129±54)to(1288±184)MP particles per liter(particlesL1)and the household food waste leachate exhibited the highest MP abundance(p<0.05).Polyethylene(PE)and fragments were the dominant polymer type and shape in MPs,respectively.The characteristic polymer types of MPs in individual leachates were different.Furthermore,the conditional fragmentation model indicated that the landfilling process considerably affected the size distribution of MPs in leachates,leading to a higher percentage(>80%)of small MPs(20–100 lm)in landfill leachates compared to other leachates.To the best of our knowledge,this is the first study discussing the sources of MPs in different leachates,which is important for MP pollution control during MSW disposal.
文摘This study explores household solid waste management (HSWM) practices and awareness among residents of Windhoek West, a rapidly urbanizing constituency in the Khomas Region of Namibia. Employing a descriptive methodology, the research investigates the interplay between public awareness, regulatory frameworks, and the availability of waste management facilities to assess their impact on waste management behaviors. Our findings indicate significant gaps in both knowledge and infrastructure that hinder effective waste management. The study reveals that while there is a high willingness among residents to engage in recycling and waste reduction, actual practices are limited due to inadequate facilities and lack of stringent enforcement of waste policies. This research identifies key factors that influence waste management practices, including demographic characteristics and access to waste management facilities. It also proposes actionable strategies such as expanding recycling and sorting facilities, enhancing educational campaigns tailored to local needs, and implementing regular enforcement mechanisms. These strategies are aimed at improving compliance with waste management protocols and fostering a culture of environmental responsibility. The results of this investigation show the critical role of ongoing education and infrastructural improvement in bridging existing knowledge gaps and facilitating effective waste management practices. This research lays a foundational step toward enhancing sustainable urban development and effective waste management in Windhoek, providing valuable insights for policymakers, community leaders, and stakeholders engaged in urban environmental management.
基金This research was partly supported by the Shanghai Municipal Natural Science Foundation(Grant No.20ZR1418100)National Natural Science Foundation of China(Grant No.32030068)to J.Z.
文摘Species diversity of angiosperms(flowering plants) varies greatly among regions.Geographic patterns of variation in species diversity are shaped by the interplay of ecological and evolutionary processes.Here,using a comprehensive data set for regional angiosperm floras across the world,we show geographic patterns of taxonomic(species) diversity,phylogenetic diversity,phylogenetic dispersion,and phylogenetic deviation(i.e.,phylogenetic diversity after accounting for taxonomic diversity) across the world.Phylogenetic diversity is strongly and positively correlated with taxonomic diversity;as a result,geographic patterns of taxonomic and phylogenetic diversity across the world are highly similar.Areas with high taxonomic and phylogenetic diversity are located in tropical regions whereas areas with low taxonomic and phylogenetic diversity are located in temperate regions,particularly in Eurasia and North America,and in northern Africa.Similarly,phylogenetic dispersion is,in general,higher in tropical regions and lower in temperate regions.However,the geographic pattern of phylogenetic deviation differs substantially from those of taxonomic and phylogenetic diversity and phylogenetic dispersion.As a result,hotspots and coldspots of angiosperm diversity identified based on taxonomic and phylogenetic diversity and phylogenetic dispersion are incongruent with those identified based on phylogenetic deviations.Each of these metrics may be considered when selecting areas to be protected for their biodiversity.
基金supported by the NSFC(21777096,21777097)the Ministry of Science and Technology of China(2018YFC1802001)+1 种基金the OU–SJTU strategic partnership development fundInternational Joint Research Promotion Program in Osaka University。
文摘Photoelectrochemical(PEC) technology provides a promising prospect for the transformation of polyethylene terephthalate(PET) plastic wastes to produce value-added chemicals.The PEC catalytic systems with high activity,selectivity and long-term durability are required for the future up-scaling industrial applications.Herein,we employed the interfacial modification strategy to develop an efficient and stable photoanode and evaluated its PEC activity for ethylene glycol(EG,derived from PET hydrolysate) oxidation to formic acid.The interfacial modification between Fe_(2)O_(3)semiconductor and Ni(OH)xcocatalyst with ultrathin TiO_(x) interlayer not only improved the photocurrent density by accelerating the kinetics of photogenerated charge carriers,but also kept the high Faradaic efficiency(over 95% in 30 h) towards the value-added formic acid product.This work proposes an effective method to promote the PEC activity and enhance the long-term stability of photoelectrodes for upcycling PET plastic wastes.
基金supported by the National Natural Science Foundation of China(52170068 and U21A20161)the Open Project of State Key Laboratory of Urban Water Resource and Environment,Harbin Institute of Technology(QAK202108)。
文摘The removal of emerging micropollutants in the aquatic environment remains a global challenge.Conventional routes are often chemically,energetically,and operationally intensive,which decreases their sustainability during applications.Herein,we develop an advanced chemical-free strategy for micropollutants decontamination that is solely based on sequential electrochemistry involving ubiquitous sulfate anions in natural and engineered waters.This can be achieved via a chain reaction initiated by electrocatalytic anodic sulfate(SO_(4)^(2-))oxidation to produce persulfate(S_(2)O_(8)^(2-))and followed by a cathodic persulfate reduction to produce sulfate radicals(SO_(4)^(·-)).These SO_(4)^(·-)are powerful reactive species that enable the unselective degradation of micropollutants and yield SO_(4)^(2-)again in the treated water.The proposed flow-through electrochemical system achieves the efficient degradation(100.0%)and total organic carbon removal(65.0%)of aniline under optimized conditions with a single-pass mode.We also reveal the effectiveness of the proposed system for the degradation of a wide array of emerging micropollutants over a broad pH range and in complex matrices.This work provides the first proof-ofconcept demonstration using ubiquitous sulfate for micropollutants decontamination,making water purification more sustainable and more economical.
基金The authors gratefully acknowledge the financial support from Shanghai Pujiang Program(20PJ1404800)“Scientific and Technical Innovation Action Plan”Basic Research Field of Shanghai Science and Technology Committee(19JC1410500).
文摘The deoxygenation of organic acids, important biomass feedstocks and derivatives, to synthesize hydrocarbon products under mild electrochemical conditions, holds significant importance for the production of carbon-neutral biofuels. There is still limited research on the influential factors of the electrochemical decarboxylation reaction of medium-chain fatty acids. In this study, n-octanoic acid (OA) was chosen as the research subject to investigate the electrochemical decarboxylation behavior of OA on a platinum electrode, focusing on the influence of different alkali metal cations (Li^(+), Na^(+), K^(+)), common anions (SO^(4)^(2−), Cl^(−)), and electrolyte pH. It was found that KOH as an electrolyte exhibited the best performance for OA. Possibly, the larger size of K^(+) increased the alkalinity of the electrode surface, facilitating OA deprotonation. LiOH electrolyte reduced the solubility of OA, thereby inhibiting the decarboxylation reaction. SO^(4)^(2−) exhibited a weak promoting effect on the decarboxylation reaction of OA, while Cl^(−) showed no adverse effect although Cl^(−) may adsorb on the electrode surface. Furthermore, unlike short-chain fatty acids, medium-chain OA can only achieve efficient decarboxylation under alkaline conditions due to its solubility properties. This study provides references and foundations for future efforts to enhance the efficiency of electrochemical decarboxylation synthesis of hydrocarbon biofuels from medium-chain fatty acids.
基金supported by the National Natural Science Foundation of China[No.51878468 and No.51508397]the Hospital Management Research Fund of Shanghai Medical Association[No.Q1902037]+1 种基金the Fundamental Research Funds for the Central Universitiesthe National Major Science and Technology Project for Water Pollution Control and Treatment[No.2017ZX07201002]。
文摘Objective Our objective was to investigate the occurrence of opportunistic pathogens and characterize the bacterial community structures in the water system of a pulmonary hospital.Methods The water samples were collected from automatic and manual faucets in the consulting room,treatment room,dressing room,respiratory ward,and other non-medical rooms in three buildings of the hospital.Quantitative polymerase chain reaction was used to quantify the load of several waterborne opportunistic pathogens and related microorganisms,including Legionella spp.,Mycobacterium spp.,and M.avium.Illumina sequencing targeting 16 S r RNA genes was performed to profile bacterial communities.Results The occurrence rates of Legionella spp.,Mycobacterium spp.,and M.avium were 100%,100%,and 76%,respectively in all samples.Higher occurrence rates of M.avium were observed in the outpatient service building(building 1,91.7%)and respiration department and wards(building 2,80%)than in the office building(building 3),where no M.avium was found.M.avium were more abundant in automatic faucets(average 2.21×10~4 gene copies/L)than in manual faucets(average 1.03×10~4 gene copies/m L)(P<0.01).Proteobacteria,Actinobacteria,Bacteroidetes,Cyanobacteria,Firmicutes,and Acidobacteria were the dominant bacterial phyla.Disinfectant residuals,nitrate,and temperature were found to be the key environmental factors driving microbial community structure shifts in water systems.Conclusion This study revealed a high level of colonization of water faucets by opportunistic pathogens and provided insight into the characteristics of microbial communities in a hospital water system and approaches to reduce risks of microbial contamination.
基金Sponsored by the JSPS Invitational Fellow ship for Research in Japan (Grant No. L18516)the National Natural Science Foundation of China(Grant No. 51273148)
文摘Graphene, a well-known two-dimensional(2 D) material, has sparked broad enthusiasm in both scientific and industrial communities in these years, due to its exceptional electrical, thermal, mechanical, and versatile properties. However, many properties and applications of graphene are layer-number dependent. The preparation of high-quality graphene with controlled layer numbers is full of challenge, since the layer number varies much with the synthesis routes and relevant experimental conditions. Hence, there is an urgent need to improve the layer-number controllability of graphene preparation. Generally, graphene can be prepared by two complementary approaches: "top-down" and "bottom-up". Since they have their own advantages, the recent advances in the layer-number tunable preparation of high-quality graphene are separately studied from the two aspects in this review, especially those dedicated to single parameter. Some effective strategies are discussed in detail, mainly including 1) supercritical-CO2 assisted sonication, electrochemical exfoliation of graphite intercalation compounds, and layer-by-layer thinning with plasma or laser, for "top-down" graphene;2) chemical vapor deposition(CVD) on dual-metal substrate, ion-implantation CVD, layer-by-layer CVD, plasma-enhanced CVD, layered-double-hydroxides template-assisted CVD;and 3) graphite-enclosure assisted epitaxial growth and pulsed-magnetron-sputtering assisted physical vapor deposition for "bottom-up" graphene on various substrates. In addition, the respective advantages of graphene with different layer numbers in properties and applications are also presented. Finally, the contribution concludes with some important perspectives on the remained challenges and future perspectives.
基金The authors gratefully acknowledge financial support from the Ministry of Science and Technology of the People’s Republic of China(Grant Nos.2017YFC0210005 and 2016YFE0112200).
文摘Iron and oxalic acids are widely distributed in the atmosphere and easily form ferric oxalate complex(Fe(III)-Ox).The tropospheric aqueous-phase could provide a medium to enable the photo-Fenton reaction with Fe(III)-Ox under solar irradiation.Although the photolysis mechanisms of Fe(III)-Ox have been investigated extensively,information about the oxidation of volatile organic compounds(VOC),specifically the potential for Secondary Organic Aerosol(SOA)formation in the Fe(III)-Ox system,is lacking.In this study,a ubiquitous VOC methacrolein(MACR)is chosen as a model VOC,and the oxidation of MACR with Fe(III)-Ox is investigated under typical atmospheric water conditions.The effects of oxalate concentration,Fe(III)concentration,MACR concentration,and pH on the oxidation of MACR are studied in detail.Results show that the oxidation rate of MACR greatly accelerates in the presence of oxalate when compared with only Fe(III).The oxidation rate of MACR also accelerates with increasing concentration of oxalate.The effect of Fe(III)is found to be more complicated.The oxidation rate of MACR first increases and then decreases with increasing Fe(III)concentration.The oxidation rate of MACR increases monotonically with decreasing pH in the common atmospheric water pH range or with decreasing MACR concentration.The production of ferrous and hydrogen peroxide,pH,and aqueous absorbance are monitored throughout the reaction process.The quenching experiments verify that·OH and O_(2)^(+)are both responsible for the oxidation of MACR.MACR is found to rapidly oxidize into small organic acids with higher boiling points and oligomers with higher molecular weight,which contributes to the yield of SOA.These results suggest that Fe(III)-Ox plays an important role in atmospheric oxidation.
基金National Natural Science Foundation of China(No.52070040,No.51878136,and No.51878135)Shanghai Rising-Star Program,China(No.19QC1400300)the Fundamental Research Funds for the Central Universities,China(DHU Distinguished Young Professor Program)。
文摘Nitrogen is the most important component for living beings while the excessive discharge of organic and inorganic nitrogen may create severe environmental problems.In this study,a continuous anoxic/oxic(A/O)reactor adopting activated sludge and sludge biofilms in the anoxic and oxic zones was applied for total nitrogen(TN)and chemical oxygen demand(COD)removal,and the efficiencies of nitrification and denitrification were compared as well.Results showed that when using activated sludge,the effluent concentrations of NH_(4)^(+)-N,NO_(3)^(-)-N,NO_(2)^(-)-N,TN and COD were inconsistent and fluctuated greatly,and the removal efficiencies of corresponding nitrification,denitrification and TN were also unstable;the obtained average COD removal efficiency was 85%.While using sludge biofilms,the acquired effluent concentrations of NH^(+)_(4)-N,NO^(-)_(3)-N,NO_(2)^(-)-N,TN and COD became stable and constant.The nitrification,denitrification,TN and COD removal efficiencies were 96%,84%and 65%and 94%,respectively.Bacterial community analysis of sludge biofilms indicated that the genus Arcobacter was the major denitrifiers in the anoxic zone with relative abundance of 76.1%,and in the oxic zone the abundances of Acinetobacter,Hydrogenophaga and Nitrospira responsible for complete nitrification were 20.05%,7.6%and 3.7%respectively.The high abundance of nitrifying bacteria and denitrifiers were related with the high and stable nitrogen and COD removal.
基金supported by the National Key R&D Program of China(2019YFC1905400)the Fundamental Research Funds for the Central Universities(2022-4-ZD-08).
文摘Electrocatalytic reduction of ethylenediamine tetraacetic acid copper(CuEDTA),a typical refractory heavy metal complexation pollutant,is an environmental benign method that operates at mild condition.Unfortunately,the selective reduction of CuEDTA is still a big challenge in cathodic process.In this work,we report a MoS_(2) nanosheet/graphite felt(GF)cathode,which achieves an average Faraday efficiency of 29.6%and specific removal rate(SRR)of 0.042 mol/cm^(2)/h for CuEDTA at−0.65 V vs SCE(saturated calomel electrode),both of which are much higher than those of the commonly reported electrooxidation technology-based removal systems.Moreover,a proofof-concept CuEDTA/Zn battery with Zn anode and MoS_(2)/GF cathode is demonstrated,which has bifunctions of simultaneous CuEDTA removal and energy output.This is one of the pioneer studies on the electrocatalytic reduction of heavy metal complex and CuEDTA/Zn battery,which brings new insights in developing efficient electrocatalytic reduction system for pollution control and energy output.
基金National Natural Science Foundation of China(22176125,52200103 and22178220)China Postdoctoral Science Foundation(2022 M722081 and 2021 M692064)+1 种基金the Fundamental Research Funds for the Central Universitiesthe Center for Advanced Electronic Materials and Devices and the instrumental Analysis Center,School of Environmental Science and Engineering,Shanghai Jiao Tong University for support。
文摘Hydrogen peroxide(H_(2)O_(2))in situ electrosynthesis by O_(2)reduction reaction is a promising alternative to the conventional Fenton treatment of refractory wastewater.However,O_(2)mass transfer limitation,cathodic catalyst selectivity,and electron transfer in O_(2)reduction remain major engineering obstacles.Here,we have proposed a systematic solution for efficient H_(2)O_(2)generation and its electro-Fenton(EF)application for refractory organic degradation based on the fabrication of a novel ZrO_(2)/CMK-3/PTFE cathode,in which polytetrafluoroethylene(PTFE)acted as a hydrophobic modifier to strengthen the O_(2)mass transfer,ZrO_(2)was adopted as a hydrophilic modifier to enhance the electron transfer of O_(2)reduction,and mesoporous carbon CMK-3 was utilized as a catalyst substrate to provide catalytic active sites.Moreover,feasible mass transfer of O_(2)from the hydrophobic to the hydrophilic layer was designed to increase the contact between O_(2)and the reaction interface.The H_(2)O_(2)yield of the ZrO_(2)/CMK-3/PTFE cathode was significantly improved by approximately 7.56 times compared to that of the co nventional gas diffusion cathode under the same conditions.The H_(2)O_(2)generation rate and Faraday efficiency reached125.98 mg·cm^(-2)·h^(-1)(normalized to 5674.04 mmol·g^(-1)·h^(-1)by catalyst loading)and 78.24%at-1.3 V versus standard hydrogen electrode(current density of-252 mA·cm^(-2)),respectively.The high H_(2)O_(2)yield ensured that sufficient OH was produced for excellent EF performance,resulting in a degradation efficiency of over 96%for refractory organics.This study offers a novel engineering solution for the efficient treatment of refractory wastewater using EF technology based on in situ high-yield H_(2)O_(2)electrosynthesis.
基金supported by the National Natural Science Foundation of China(21876030)the International Cooperation Project of Science and Technology Commission of Shanghai Municipality(18230710700)。
文摘Recalcitrance and the inherent heterogeneity of lignin structure are the major bottlenecks to impede the popularization of lignin-based chemicals production processes.Recent works suggested a promising pathway for lignin depolymerization and lignin-derived bio-oil upgrading via an electrochemical biorefinery(a process in which lignin valorization is performed via electrochemical oxidation or reduction).This review presents the progress on chemicals synthesis and bio-oil upgrading from lignin by an electrochemical biorefinery,relating to the lignin biosynthesis pathway,reaction pathway of lignin electrochemical conversion,inner-sphere and outer-sphere electron transfer mechanism,basic kinetics and thermodynamics in electrochemistry,and the recent embodiments analysis with the emphasis on the respective feature and limitation for lignin electrochemical oxidative and reductive conversion.Lastly,the challenge and perspective associated with lignin electrochemical biorefinery are discussed.Present-day results indicate that more work should be performed to promote efficiency,selectivity,and stability in pursuing a lignin electrochemical biorefinery.One of the most promising developing directions appears to be integrating various types of lignin electrochemical conversion strategies and other existing or evolving lignin valorization technologies.This review aims to provide more references and discussion on the development for lignin electrochemical biorefinery.
基金supported by the“Scientific and Technical Innovation Action Plan”Basic Research Field of Shanghai Science and Technology Committee(19JC1410500)financial support from the National Natural Science Foundation of China(91645110)。
文摘The electrocatalytic carbon dioxide reduction reaction(eCO_(2)RR)into high-value-added chemicals and fuels is a promising strategy to mitigate global warming.However,it remains a significant stumbling block to the rationally tuning lattice plane of the catalyst with high activity to produce the target product in the eCO_(2)RR process.To attempt to solve this problem,the Culn bimetallic alloy nanocatalyst with specifically exposed lattice planes is modulated and electrodeposited on the nitrogen-doped porous carbon cloth by a simple two-step electrodeposition method,which induces high Faraday efficiency of 80%towards HCOO-(FEHCOO-)with a partial current density of 13.84 mA cm-2at-1.05 V(vs.RHE).Systematic characterizations and theoretical modeling reveal that the specific coexposed Culn(200)and In(101)lattice facets selectively adsorbed the key intermediate of OCHO*,reducing the overpotential of HCOOH and boosting the FEHCOO-in a wide potential window(-0.65--1.25 V).Moreover,a homogeneous distribution of Culn nanoparticles with an average diameter of merely~3.19 nm affords exposure to abundant active sites,meanwhile prohibiting detachment and agglomeration of nanoparticles during eCO_(2)RR for enhanced stability attributing to the self-assembly electrode strategy.This study highlights the synergistic effect between catalytic activity and facet effect,which opens a new route in surface engineering to tune their electrocatalytic performance.
基金the financial support for this work provided by the National Natural Science Point Foundation of China(No.52131002)the International Exchange Program for Graduate Students,Tongji University(China)(No.2023020014).
文摘Anaerobic digestion(AD)of organic fraction of municipal solid waste(OFMSW)is prone to system breakdown under high organic loading rates(OLRs)condition,which subsequently reduces the efficiency of digestion process and results in substantial economic losses.In this perspective paper,the substances metabolisms,electrons flow,as well as microbial interaction mechanisms within AD process are comprehensively discussed,and the underlying bottleneck that causes inefficient methane production is identified,which is“electrons surplus”.Systems encountering severe electron surplus are at risk of process failure,making it crucial to proactively prevent this phenomenon through appropriate approaches.On this basis,the present perspective proposes three potential electronic regulation strategies to prevent electrons surplus,namely,electron shunt,accelerating electron transfer and regulating methanogenic metabolism pathway,and presents specific methodologies for each strategy.Furthermore,the potential solutions to challenges that may occur during the electronic regulation process are also presented in this paper.This perspective aims to provide innovative approaches to achieve the efficient and stable operation of OFMSW anaerobic digestion,especially under high OLRs condition.
基金Financial support from the National Natural Science Foundation of China(Grant Nos.52225001 and 51978485)the State Key Laboratory for Pollution Control(China)is acknowledged.
文摘The deep-learning protein structure prediction method AlphaFold2 has garnered enormous attention beyond the realm of structural biology,for its groundbreaking contribution to solving the"protein foiding problem"In this perspective,we explore the connection between protein structure studies and environmental research,delving into the potential for addressing specific environmental challenges.Proteins are promising for environmental applications because of the functional diversity endowed by their structural complexity.However,structural studies on proteins with environmental significance remain scarce.Here,we present the opportunity to study proteins by advancing experimental determination and deep-learning prediction methods.Specifically,the latest progress in environmental research via cryogenic electron microscopy is highlighted.It allows us to determine the structure of protein complexes in their native state within cells at molecular resolution,revealing environmentally-associated structural dynamics.With the remarkable advancements in computational power and experimental resolution,the study of protein structure and dynamics has reached unprecedented depth and accuracy.These advancements will undoubtedly accelerate the establishment of comprehensive environmental protein structural and functional databases.Tremendous opportunities for protein engineering exist to enable innovative solutions for environmental applications,such as the degradation of persistent contaminants,and the recovery of valuable metals as well as rare earth elements.
基金supported by the National Key Research and Development Program of China(No.2019YFC0408203)。
文摘Tetramethylammonium hydroxide(TMAH)is an important compound that utilized and released by the rapidly expanding semiconductor industry,which could hardly be removed by the conventional wastewater treatment techniques.As a cholinergic agonist,the tetramethylammonium ion(TMA^(+))has been reported to induce toxicity to muscular and respiratory systems of mammals and human,however the toxicity on aquatic biota remains poorly known.We investigated the neurotoxic effects of TMA^(+)exposure on zebrafish,based on neurobehavior tests and a series of biomarkers.Significant inhibitions on the swimming distance of zebrafish larvae were observed when the exposure level exceeded 50 mg/L,and significant alterations on swimming path angles(straight and deflective movements)occurred even at 10 mg/L.The tested neurobehavioral endpoints of zebrafish larvae were significantly positively correlated with reactive oxygen species(ROS)and malondialdehyde(MDA),significantly negatively related with the activities of antioxidant enzymes,but not significantly correlated with the level of acetylcholinesterase(AChE).Such relationship indicates that the observed neurotoxic effects on swimming behavior of zebrafish larvae is mainly driven by oxidative stress,rather than the alterations of neurotransmitter.At the highest exposure concentration(200 mg/L),TMA^(+)evoked more severe toxicity on zebrafish juveniles,showing significantly stronger elevation on the MDA activity,and greater inhibitions on the activities of antioxidant enzymes and ACh E,suggesting juveniles were more susceptible to TMA^(+)exposure than larval zebrafish.