Anammox bacteria in constructed wetlands(CWs)play pivotal role in sustainable nitrogen transformation,yet existing studies lack comprehensive analysis of environmental gradients and microbial interactions,both key fac...Anammox bacteria in constructed wetlands(CWs)play pivotal role in sustainable nitrogen transformation,yet existing studies lack comprehensive analysis of environmental gradients and microbial interactions,both key factors in anammox bacteria enrichment.This study investigated the mechanisms driving anammox bacteria enrichment in lab-scale simulated CWs treating high-nitrogen wastewater,focusing on bacterial community re-sponses across wetland layers with various strategies,including continuous up-flow influent,nitrogen loading increase,effluent recirculation,intermittent influent,and anammox bacteria inoculation.Results showed that total relative and absolute abundances of anammox bacteria ranged from 0.77%to 12.50%and from 0.13 to 6.46×10^(7) copies/g,respectively.Dissolved oxygen and pH had significant positive correlations with the absolute abundance of anammox bacteria,while organic matter and nitrate negatively impacted their relative abundance.Permutational multivariate analysis of variance indicated that spatial heterogeneity explained more variation in anammox bacteria abundance(43.44%)compared to operational strategies(8.58%).In terms of microbial interactions,60 dominant species exhibited potential correlations with anammox bacteria,comprising 170 interactions(105 positive and 65 negative),which suggested that anammox bacteria generally foster cooperative relationships with dominant bacteria.Notably,significant interspecies interactions were observed between Candidatus Kuenenia(dominant anammox bacteria in CWs)and species within the genera Chitinivibrio-nia and Anaerolineaceae,suggesting that microbial interactions primarily manifest as indirect facilitative effects rather than direct mutualistic relationships.Given that the Normalized Stochasticity Ratio in CWs were<50%,this study inferred that environmental gradients have greater influence on anammox bacteria than microbial interactions.展开更多
Sustainable development for our life is important task,which is driven by key materials and technologies.In this roadmap,we discuss three main aspects in addressing environmental questions,green chemical processes and...Sustainable development for our life is important task,which is driven by key materials and technologies.In this roadmap,we discuss three main aspects in addressing environmental questions,green chemical processes and energy challenges.They are included,such as gas treatment and separation,wastewater treatment,waste gas treatment,solid waste treatment,lithium extraction,hydrogen production,water splitting,CO_(2) reduction,photocatalytic clean technologies,plastic degradation,fuel cells,lithium batteries,sodium batteries,aqueous batteries,solid state batteries,metal air batteries and supercapacitors.Their status,challenges,progress and future perspectives are also discussed.We hope that this paper can give clear views on sustainable development in materials and technologies.展开更多
Air pollution is a major challenge to the improvement of urban environmental quality.The control of air pollution still faces severe challenges,especially in developing countries,such as ozone pollution control.Ozone ...Air pollution is a major challenge to the improvement of urban environmental quality.The control of air pollution still faces severe challenges,especially in developing countries,such as ozone pollution control.Ozone is a typical secondary air pollutant,and its formation chemistry from its precursors(NOx and volatile organic compounds)is highly nonlinear,which caused the emission reduction of its precursors is not always effective and therefore new assisted approaches to control of ozone pollution are needed.Photocatalysis and ambient catalysis technology are expected to be applied in open atmosphere as a new booster to the direct purification of air pollutants in emission sources.In this perspective,we summarize the current knowledge about the photocatalysis and ambient catalysis technology for the removal of air pollutants under natural photothermal conditions.Based on these technologies,we propose the concept of“Environmental Catalytic City”,which refers to the spontaneous purification of low concentration urban air pollutants in the atmosphere by catalytic materials coating on the artificial surfaces,such as building surfaces in the city.In this way,the urban city with self-purification function can remove air pollution without additional energy consumption.The further improvement,development,and application of the“Environmental Catalytic City”is also discussed.展开更多
A novel hierarchical porous metal-organic framework(MOF)-based hollow carbon nanofiber mat(CNFM)was prepared through a facile electrospinning process followed by carbonization.Two immiscible polymers,polyacrylonitrile...A novel hierarchical porous metal-organic framework(MOF)-based hollow carbon nanofiber mat(CNFM)was prepared through a facile electrospinning process followed by carbonization.Two immiscible polymers,polyacrylonitrile/polymethyl methacrylate(PAN/PMMA),and porous zeolitic imidazolate framework-8(ZIF-8)particles were selected as components for the electrospinning suspension.The resulting PPZ-CNFM-1–2–2(PAN:PMMA:ZIF8=1:2:2,mass ratio)exhibited a hollow tubular structure with uniformly distributed dense hollow-spheres on the tube walls.The obtained CNFM possessed a high Brunauer-Emmett-Teller specific surface area(SBET)of 1696 m2/g and total pore volume of 2.74 cm^(3)/g,which are comparable to those achieved by traditional physical or chemical activation methods.This MOF-based CNFM demonstrated excellent adsorption performance towards ciprofloxacin(CIP),exhibiting a high static adsorption capacity of approximately 600 mg/g and achieving adsorption equilibrium withing only 1 h.The exceptional adsorption capacity can be attributed to its high SBET and abundant pores that accommodate CIP molecules,while the rapid adsorption rate is facilitated by the presence of hollow-sphere and hollow tubular structures in the carbon nanofibers.Furthermore,the study revealed the significant contributions of pore-filling effect during the adsorption process.Fixed-bed experiments confirmed that this MOF-based hollow CNFM holds great potential for large-scale applications in purifying CIP-contaminated water.展开更多
Conductive elastomers combining micromechanical sensitivity,lightweight adaptability,and environmental sustainability are critically needed for advanced flexible electronics requiring precise responsiveness and long-t...Conductive elastomers combining micromechanical sensitivity,lightweight adaptability,and environmental sustainability are critically needed for advanced flexible electronics requiring precise responsiveness and long-term wearability;however,the integration of these properties remains a significant challenge.Here,we present a biomass-derived conductive elastomer featuring a rationally engineered dynamic crosslinked network integrated with a tunable microporous architecture.This structural design imparts pronounced micromechanical sensitivity,an ultralow density(~0.25 g cm^(−3)),and superior mechanical compliance for adaptive deformation.Moreover,the unique micro-spring effect derived from the porous architecture ensures exceptional stretchability(>500%elongation at break)and superior resilience,delivering immediate and stable electrical response under both subtle(<1%)and large(>200%)mechanical stimuli.Intrinsic dynamic interactions endow the elastomer with efficient room temperature self-healing and complete recyclability without compromising performance.First-principles simulations clarify the mechanisms behind micropore formation and the resulting functionality.Beyond its facile and mild fabrication process,this work establishes a scalable route toward high-performance,sustainable conductive elastomers tailored for next-generation soft electronics.展开更多
Selective catalytic reduction with NH3(NH3-SCR)is an important means of NO_(x) abatement from stationary and mobile sources,and the key element is efficient and stable NH3-SCR catalysts.In this study,we propose a meth...Selective catalytic reduction with NH3(NH3-SCR)is an important means of NO_(x) abatement from stationary and mobile sources,and the key element is efficient and stable NH3-SCR catalysts.In this study,we propose a method to construct superior Fe-Beta catalysts based on Al-rich zeolites.This strategy successfully promotes the formation of NH3-SCR-active isolated Fe^(3+)species,thus effectively improving the low-temperature activity of the Fe-Beta catalysts.Thanks to the abundant Brønsted acid sites of the Al-rich zeolite,the Fe_(2)O_(3) particles are redispersed and anchored as isolated Fe^(3+)during hydrothermal aging.This dynamic evolution of Fe species makes up for the adverse effect of dealumination of the Al-rich zeolite framework and achieves high stability for the Al-rich Fe-Beta catalyst.This study may promote the understanding of highly efficient and stable catalyst design using Al-rich zeolites.展开更多
Emerging contaminants in water sources present serious environmental and health risks,creating an urgent need for efficient and reliable treatment strategies.Photocatalytic advanced oxidation processes(AOPs)provide ra...Emerging contaminants in water sources present serious environmental and health risks,creating an urgent need for efficient and reliable treatment strategies.Photocatalytic advanced oxidation processes(AOPs)provide rapid reaction rates and strong oxidation capabilities,however,comprehensive evaluations of wastewater treatment,including degradation pathways,toxicity assessments and mechanistic insights,remain underexplored in the literature.This study presents novel S-scheme Mn_(0.5)Cd_(0.5)S/In_(2)S_(3)(MCS/IS)photocatalysts for efficient degradation of antibiotic pollutants,with a particular focus on tetracycline hydrochloride(TCH).The optimized MCS/IS photocatalyst demonstrates exceptional degradation efficiency and robust resistance to inorganic anions.Additionally,a continuous-flow wastewater treatment system,using an MCS/IS membrane,demonstrates outstanding stability in TCH photodegradation.Utilizing response surface methodology and Fukui function analysis,the effects of various parameters on photocatalytic degradation rates,along with the associated pathways and intermediate products,have been thoroughly investigated.Toxicity assessments confirm the environmental safety of the treated effluents.Mechanistic studies show that the S-scheme heterojunction in the MCS/IS photocatalyst improves electron-hole separation,thereby enhancing photocatalytic performance.It is expected that this study will serve as a model for advancing the removal of emerging contaminants,further enhancing photocatalytic AOPs as sustainable water purification technologies.展开更多
Electrochemical processes lie at the core of biological function,governing energy transduction,metabolic flux,and mo-lecular signaling.Recent advances in electrochemical science now allow these processes to be probed ...Electrochemical processes lie at the core of biological function,governing energy transduction,metabolic flux,and mo-lecular signaling.Recent advances in electrochemical science now allow these processes to be probed and controlled with unprecedented spatial,temporal,and chemical resolution.In this review,we present an integrated framework that pro-gresses from fundamental mechanisms to analytical technologies and functional modulation.We begin by outlining elec-tron transfer pathways in mitochondrial respiration,microbial extracellular electron transfer,and DNA-and protein-based charge conduction,followed by the principles of photon-electron conversion in photosynthesis and the central role of redox equilibrium in coordinating cellular responses.We then highlight electrochemical analytical strategies that enable multiscale biological characterization,including biosensing,electrochemical and scanning probe imaging,electrogenerated chemilu-minescence detection,and measurements of membrane potentials and neurotransmitter dynamics.Emerging platforms such as flexible biointerfaces,ultramicroelectrodes,and nanopore systems further extend these capabilities to in vivo and single-molecule contexts.Finally,we discuss how electrochemical inputs can be used to regulate metabolic pathways,mi-crobial and protein activities,and neural signaling,enabling precision therapeutic and bioengineering applications.Togeth-er,these developments establish electrochemistry as a powerful foundation for decoding and directing biological systems.展开更多
The anodic electrochemical ozone production(EOP)and the cathodic three-electron oxygen reduction reaction(3e^(-)ORR)are effective processes for generating active oxygen species(ROS).However,the activation of ozone(O_(...The anodic electrochemical ozone production(EOP)and the cathodic three-electron oxygen reduction reaction(3e^(-)ORR)are effective processes for generating active oxygen species(ROS).However,the activation of ozone(O_(3))by hydroxyl radical(OH)to form ROS poses significant challenges.The micelle balllike bimetallic La-Nb oxides(LNOx)have been developed as a bifunctional electrocatalyst for both the EOP and 3e^(-)ORR reactions.The LNO20 demonstrated a 9.8%of Faradaic efficiency(FE)in O_(3)production and a transfer number of 2.8 electrons in the 3e^(-)ORR.Theoretical calculations support the notion that the five-membered ring mechanism in LNO20 facilitates O_(3)production.Additionally,the incorporation of La provides active sites that enhance the activation of hydrogen peroxide(^(*)H_(2)O_(2))and the generation of OH.This innovative approach synergistically integrates EOP and 3e^(-)ORR,enhancing the activation of O_(3)to produce ROS,demonstrating exceptional efficacy in the degradation of organic pollutants and antimicrobial activity.The study paves the way for designing advanced electrocatalysts for EOP and 3e^(-)ORR and offers insights into utilizing electrochemical method to support other antibacterial strategies.展开更多
Dissolved organic matter(DOM)is ubiquitous in the environment and plays an important role in global ecosystems.However,our understanding of the evolution and molecular diversity of DOM from different biomass materials...Dissolved organic matter(DOM)is ubiquitous in the environment and plays an important role in global ecosystems.However,our understanding of the evolution and molecular diversity of DOM from different biomass materials and biochar is not enough.Herein,we investigated the changes in DOM from seven biomass and biochar samples over a bio-incubation of 28 days,and explored their contents,and optical,chemical,and molecular characteristics.The results indicated that dissolved organic carbon(DOC)from different sources all exhibited a gradually decreasing trends during the incubation,while the absorbance and aromaticity gradually increased.Biomass DOM was characterized by higher DOC concentrations and a higher degradation rate,whereas biochar DOM had high aromaticity and little variability.Parallel factor analysis results showed that the protein-like fluorescent groups were as only detected in biomass DOM,while the dominant humic-like components were identified in biochar DOM.Additionally,the molecular composition of DOM from different sources was different,and biomass DOM contained more carbohydrate-like and saturated compounds.More sulfur-containing compounds were detected in Ceratophyllum demersum(CD)DOM,which may indicate that the leaching of CD litter was an important source of sulfur-containing species in aquatic environments.Furthermore,biochar DOM had greater aromaticity and a higher degree of oxidation than the corresponding biomass DOM.This study provided a detailed understanding of the molecular diversity of DOM by considering its various sources,and the results are helpful for further understanding their chemical properties and structures.展开更多
In photocatalytic water treatment processes,the particulate photocatalysts are typically immobilized on membrane,through either chemical/physical loading onto the surface or directly embedding in the membrane matrix.H...In photocatalytic water treatment processes,the particulate photocatalysts are typically immobilized on membrane,through either chemical/physical loading onto the surface or directly embedding in the membrane matrix.However,these immobilization strategies inevitably compromise the interfacial mass diffusion and cause activity decline relative to the suspended catalyst.Here,we propose a binder-free surface immobilization strategy for fabrication of high-activity photocatalytic membrane.Through a simple dimethylformamide(DMF)treatment,the nanofibers of polyvinylidene fluoride membrane were softened and stretched,creating enlarged micropores to efficiently capture the photocatalyst.Subsequently,the nanofibers underwent shrinking during DMF evaporation,thus firmly strapping the photocatalyst microparticles on the membrane surface.This surface self-bounded photocatalytic membrane,with firmly bounded yet highly exposed photocatalyst,exhibited 4.2-fold higher efficiency in hydrogen peroxide(H_(2)O_(2))photosynthesis than the matrix-embedded control,due to improved O_(2)accessibility and H_(2)O_(2)diffusion.It even outperformed the suspension photocatalytic system attributed to alleviated H_(2)O_(2)decomposition at the hydrophobic surface.When adopted for UV-based water treatment,the photocatalytic system exhibited tenfold faster micropollutants photodegradation than the catalyst-free control and demonstrated superior robustness for treating contaminated tap water,lake water and secondary wastewater effluent.This immobilization strategy can also be extended to the fabrication of other photocatalytic membranes with diverse catalyst types and membrane substrate.Overall,our work opens a facile avenue for fabrication of high-performance photocatalytic membranes,which may benefit advanced oxidation water purification application and beyond.展开更多
Bisphenol A （BPA） is of global concern due to its disruption of endocrine systems and ubiquity in the aquatic environment. It is important, therefore, that efforts are made to remove it from the aqueous phase. A nov...Bisphenol A （BPA） is of global concern due to its disruption of endocrine systems and ubiquity in the aquatic environment. It is important, therefore, that efforts are made to remove it from the aqueous phase. A novel adsorbent, mesoporous carbon CMK-3, prepared from hexagonal SBA- 15 mesoporous silica was studied for BPA removal from aqueous phase, and compared with conventional powdered activated carbon （PAC）. Characterization of CMK-3 by transmission electron microscopy （TEM）, X-ray diffraction, and nitrogen adsorption indicated that prepared CMK-3 had an ordered mesoporous structure with a high specific surface area of 920 m^2/g and a pore-size of about 4.9 nm. The adsorption of BPA on CMK-3 followed a pseudo second-order kinetic model. The kinetic constant was 0.00049 g/（mg.min）, much higher than the adsorption of BPA on PAC. The adsorption isotherm fitted slightly better with the Freundlich model than the Langmuir model, and adsorption capacity decreased as temperature increased from 10 to 40℃. No significant influence of pH on adsorption was observed at pH 3 to 9; however, adsorption capacity decreased dramatically from pH 9 to 13.展开更多
Coal preparation solid waste,which is a major environmental issue for coal-producing areas in China,may be microbiologically digested and transformed into a product suitable as a soil amendment to increase soil organi...Coal preparation solid waste,which is a major environmental issue for coal-producing areas in China,may be microbiologically digested and transformed into a product suitable as a soil amendment to increase soil organic matter content and prevent and enhance plant/crop growth.Coal preparation waste collected from a coal sorting plant in Inner Mongolia,China was digested in bioreactors inoculated with microbial enrichments prepared from activated sludge and cow manure.The effluent solids from the coal preparation waste bioreactors were analyzed for their suitability as organic soil amendments,which complied with China standards.Plant growth tests were conducted in sandy soil from a semi-arid region in Colorado,which was amended with the effluent solids.Kentucky bluegrass(Poa pratensis L.)and chives(Allium schoenoprasum)were used as the representative plants for the growth tests,where results indicated substantially higher yields of Kentucky bluegrass and chives for the sandy soils amended with the effluent solids when compared to a commercial organic fertilizer.The number and average length of Kentucky bluegrass shoots were 10 and 5.1 times higher,respectively,in soils amended with the effluent solids.Similarly,the number and average length of chives shoots were 10 and 1.7 times higher,respectively,in soils amended with the effluent solids.Overall,the microbial digestion of coal preparation waste for application as an organic soil amendment is a viable alternative and beneficial use of coal preparation solid waste.展开更多
An environmental risk assessment was performed for pharmaceutical compounds present in the aquatic environment of China. Predicted environmental concentration （PEC） of the compounds were calculated according to Euro...An environmental risk assessment was performed for pharmaceutical compounds present in the aquatic environment of China. Predicted environmental concentration （PEC） of the compounds were calculated according to European Medicines Evaluation Agency （EMEA） guidelines. Available ecotoxicological data compromised by applying a very conservative assessment factor （AF） were employed to calculate the predicted noeffect concentration （PNEC）. The screening principle and the risk assessment were based on risk quotient （RQ）, which derived from the PEC and related PNEC values. PEC results indicated that all the compounds except sulfadimethoxine and levocamitine, should carry out phase II risk assessment in EMEA guideline. RQ values suggested that more than 36 pharmaceuticals may be imposed health threats to the aquatic environment; especially the antibiotic therapeutic class including amoxicillin, sulfasalazine, trimethoprim, oxytetracycline and erythromycin showed high RQ values. These substances with high RQ value （RQ≥ 1） were regarded as top- priority pharmaceuticals for control in the aquatic environment of China. However, the antibiotic substances which had low risk quotient （RQ 〈 1）, should be reassessed by its potentially induced resistance under low concentration in future.展开更多
Photocatalytic ammonia(NH_(3))decomposition is a key strategy for green hydrogen production and renewable energy conversion.Although conventional plasmonic metal/TiO_(2) composites exhibit some activity,their applicat...Photocatalytic ammonia(NH_(3))decomposition is a key strategy for green hydrogen production and renewable energy conversion.Although conventional plasmonic metal/TiO_(2) composites exhibit some activity,their applications are constrained by high carrier recombination rates and narrow light harvesting ranges.To address these challenges,this study innovatively introduces the plasmonic semiconductor MoO_(3-x),which is characterized by broad-spectrum absorption and abundant oxygen vacancies,to construct a Cu-MoO_(3-x)/TiO_(2) plasmon resonance coupling nanostructure.The construction of the Cu-MoO_(3-x) composite stabilizes Cu via MoO_(3-x) coating and facilitates electron transfer from Cu to MoO_(3-x),generating more oxygen vacancies for NH_(3) activation.The visible localized surface plasmon resonance(LSPR)response of Cu,coupled with the visible to near-infrared LSPR resonance of MoO_(3-x),broadens the spectral response and optimizes carrier dynamics,thereby reducing the recombination of photogenerated carriers.The use of hot carriers and plasmonic photothermal effects synergistically accelerate surface reaction kinetics and enhance photocatalytic efficiency.In particular,the optimal Cu-MoO_(3-x)/TiO_(2) catalyst results in an enhanced NH_(3) decomposition rate of 103.2 mmol·g^(-1)·h^(-1) under fullspectrum light irradiation,representing 29-fold and 94-fold enhancements over those of Cu/TiO_(2) and MoO_(3-x)/TiO_(2),respectively.This innovative design strategy transcends traditional plasmonic metal/semiconductor catalyst designs and opens new avenues for developing efficient solar-driven plasmon resonance coupling catalysts.展开更多
Overcoming the kinetic barrier of N-H bond activation in NH_(3)remains a central challenge in enabling efficient ammonia decomposition as well as thermocatalytic and electrocatalytic ammonia oxidation.Oxide-on-metal i...Overcoming the kinetic barrier of N-H bond activation in NH_(3)remains a central challenge in enabling efficient ammonia decomposition as well as thermocatalytic and electrocatalytic ammonia oxidation.Oxide-on-metal inverse catalysts offer promising opportunities to address this challenge;however,the role of oxide overlayer thickness in governing surface structures and reactivity is still poorly understood.Herein,we have elucidated the layer-dependent atomic structure of vanadium oxide overlayers on Cu(111)surfaces and its implications for NH_(3)adsorption,using a combination of high-resolution scanning tunneling microscopy(STM),X-ray photoelectron spectroscopy(XPS),and density functional theory(DFT)calculations.Despite sharing the same vanadium oxidation state(V^(3+)),VO_(x)overlayers on Cu(111)adopt distinct atomic structures depending on the overlayer thickness.A nonlinear correlation is observed between VO_(x)overlayer thickness and N-H activation capability.The surface-V_(2)O_(3)phase formed by 2-3 VO_(x)layers exhibits the highest activity,enabling both molecular and dissociative adsorption of NH_(3).In contrast,thicker bulk-V_(2)O_(3)(0001)(>3 VO_(x)layers)only shows molecular adsorption without dissociation,while the monolayer VO(111)surface exhibits negligible NH_(3)adsorption.These findings underscore the pivotal influence of oxide overlayer thickness in modulating oxide-on-metal inverse catalyst systems,providing atomic-level insights that can guide the rational design of high-performance catalytic materials for NH_(3)activation.展开更多
CONSPECTUS:Electrochemical water purification and pollutant monitoring have garnered significant attention due to their unique technical advantages.The pursuit of safe,efficient,and economically viable catalysts remai...CONSPECTUS:Electrochemical water purification and pollutant monitoring have garnered significant attention due to their unique technical advantages.The pursuit of safe,efficient,and economically viable catalysts remains a critical priority.Titanium dioxide(TiO_(2)),a prototypical transition-metal oxide with substantial industrial importance,is widely recognized as a benchmark catalyst for photochemical reactions.However,its practical application is limited by restricted light absorption and rapid photocarrier recombination.Recently,TiO_(2) has emerged as a promising candidate in electrochemical catalysis,particularly in the fields of energy and environmental science.Its atomic and electronic structures can be precisely engineered through advanced techniques such as nanoscale morphology control,polar-facet engineering,vip-metal doping,and structural-defect modulation.This review examines recent advancements in TiO_(2)-based electrochemical applications,with a focus on water purification and pollutant monitoring.In this Account,we present our efforts to harness facet-and defect-engineered TiO_(2) as electrochemical catalysts for water purification,addressing critical challenges such as low conductivity and poor reactivity.Initially,we demonstrate that facetengineered TiO_(2),specifically designed to expose the high-energy{001}polar facet,facilitates the dissociation of both pollutant and water molecules.This significantly lowers energy barriers and enhances anodic reactions through both direct and indirect pathways,thereby markedly improving water purification efficiency.Furthermore,the dual photochemical and electrochemical functionalities of a single{001}-tailored TiO_(2) electrode enable synergistic UV-light-assisted electrochemical catalysis under low bias conditions,achieving superior energy efficiency and resistance to electrode fouling.Next,we explore the catalytic potential of defect-engineered TiO_(2)(TiO_(2−x)),highlighting the role of titanium(Ti^(3+))and oxygen vacancies(O_(v))in boosting electrochemical water purification.Surface and subsurface defects,characterized by localized atomic disorder and structural distortions,serve as active sites that drive beneficial structural transformations,enriched electronic distribution,enhanced spin−spin correlations,and polaron hopping mechanisms,all of which contribute to improved cathodic reduction.To stabilize these reactive sites under anodic polarization,we propose a practical visible-light-assisted electrochemical catalysis strategy.This approach leverages mild non-band-gap excitation pathways mediated by defect sub-bands,providing enhanced stability and catalytic efficiency.Finally,we identify the challenges associated with the application of self-engineered TiO_(2) in electrochemical water purification and outline directions for future research.Our studies deepen the fundamental understanding of structure−catalysis relationships and exemplify a self-tailoring strategy to advance oxide catalysis without reliance on noble or toxic-metal cocatalysts.By elucidating catalytic mechanisms and adopting innovative synthesis techniques,our insights provide a foundation for designing advanced electrocatalysts.Self-engineered TiO_(2) holds the potential to establish a new paradigm in electrochemical catalysis,opening pathways for transformative solutions in environmental remediation.展开更多
Electron paramagnetic resonance(EPR)is a spectroscopic approach that can directly and non-destructively detect and char-acterize species with unpaired electrons,such as radicals,transi-tion metal ions,defects in mater...Electron paramagnetic resonance(EPR)is a spectroscopic approach that can directly and non-destructively detect and char-acterize species with unpaired electrons,such as radicals,transi-tion metal ions,defects in materials,and the excited triplet state of molecules[1].To date,the EPR technique has become an indis-pensable component in the toolbox of environmental studies.Using various diamagnetic probes(e.g.,5,5-dimethyl-1-pyrroline-N-oxide(DMPO))as the spin traps,transient reactive species can be transformed to EPR-detectable(meta)stable spin adducts,which enables radical identification and mechanism interpretation.Therefore,EPR constitutes a versatile platform for the mechanistic investigation of advanced oxidation processes(AOPs)in the field of water purification and contaminated groundwater remediation[2].展开更多
Conductive additive such as biochar have been extensively employed to enhance anaerobic digestion(AD)performance for over a decade.Among the proposed mechanisms,conductive additive-facilitated direct interspecies elec...Conductive additive such as biochar have been extensively employed to enhance anaerobic digestion(AD)performance for over a decade.Among the proposed mechanisms,conductive additive-facilitated direct interspecies electron transfer(DIET)is frequently cited as a key contributor to these performance improvements.Because this process is believed to bypass traditional diffusible intermediates(e.g.,H_(2) or formate),it can enable more efficient energy transfer between syntrophic partners and accelerate substrate degradation,potentially leading to higher methane yields and improved overall stability of the anaerobic digestion process.However,benefits regarding conductive additivefacilitated DIET often rely on indirect indicators rather than direct experimental evidence.Here,we advocate for a critical reassessment on the benefits of conductive additive for DIET in AD.Specifically,we emphasize the importance of establishing standardized experimental protocols and obtaining direct evidence to confirm the occurrence and significance of DIET in conductive additive-amended AD system.Furthermore,it is essential to distinguish DIET from other enhancement mechanisms such as pH buffering and toxin adsorption that may independently contribute to improved AD performance,with the goal of advancing its practical implementation.展开更多
Electroactive microorganisms are integral to biogeochemical cycles through extracellular electron transfer and have potential applications in environmental remediation.However,their long-term competitive interactions ...Electroactive microorganisms are integral to biogeochemical cycles through extracellular electron transfer and have potential applications in environmental remediation.However,their long-term competitive interactions and evolutionary dynamics with non-electroactive microorganisms remain poorly understood.In this study,we conducted a 320-day cultivation experiment in which monocultures of the electroactive Shewanella oneidensis MR-1,the non-electroactive Citrobacter freundii An1,and their cocultures were compared under three single electron acceptor conditions:anaerobic(no exogenous electron acceptor),ferrihydrite,or oxygen.After 320 d,S.oneidensis MR-1 presented the highest relative abundance of 30.94%±0.74%in the ferrihydrite cocultures.S.oneidensis MR-1 maintained ferrihydrite reduction capacity after cultivation under all three conditions,indicating the long-term stability of its extracellular electron transfer.Moreover,no other phenotypic evolution was observed in S.oneidensis MR-1 after ferrihydrite or anaerobic cultivation.In contrast,both monocultured and cocultured S.oneidensis MR-1 exhibited enhanced adaptation to oxygen,characterized by increased growth rates,metabolic activity,and reduced cell aggregation.Notably,substrate consumption increased in monocultures but decreased in cocultures,suggesting an optimization of metabolic efficiency in the latter.Genome sequencing revealed mutations in genes associated with cell division,adenosine triphosphate synthesis,lactate metabolism,and flagellar/pilus expression in S.oneidensis MR-1.Interestingly,the ferrihydrite-adapted groups also exhibited enhanced adaptation to oxygen.83.96%of mutations were shared across all culture systems and enriched in environmental signal-sensing pathways,indicating that parallel genomic evolution facilitated cross-environmental adaptation.Our findings reveal the ecological evolution of electroactive microorganisms in diverse redox environments and establish a foundation for engineering electroactive communities.展开更多
基金supported by Natural Science Foundation of Xiamen,China(No.3502Z20227232)the STS Project of Fujian-CAS(No.2023T3018)Bureau of International Cooperation,Chinese Academy of Sciences(No.322GJHZ2022035MI).
文摘Anammox bacteria in constructed wetlands(CWs)play pivotal role in sustainable nitrogen transformation,yet existing studies lack comprehensive analysis of environmental gradients and microbial interactions,both key factors in anammox bacteria enrichment.This study investigated the mechanisms driving anammox bacteria enrichment in lab-scale simulated CWs treating high-nitrogen wastewater,focusing on bacterial community re-sponses across wetland layers with various strategies,including continuous up-flow influent,nitrogen loading increase,effluent recirculation,intermittent influent,and anammox bacteria inoculation.Results showed that total relative and absolute abundances of anammox bacteria ranged from 0.77%to 12.50%and from 0.13 to 6.46×10^(7) copies/g,respectively.Dissolved oxygen and pH had significant positive correlations with the absolute abundance of anammox bacteria,while organic matter and nitrate negatively impacted their relative abundance.Permutational multivariate analysis of variance indicated that spatial heterogeneity explained more variation in anammox bacteria abundance(43.44%)compared to operational strategies(8.58%).In terms of microbial interactions,60 dominant species exhibited potential correlations with anammox bacteria,comprising 170 interactions(105 positive and 65 negative),which suggested that anammox bacteria generally foster cooperative relationships with dominant bacteria.Notably,significant interspecies interactions were observed between Candidatus Kuenenia(dominant anammox bacteria in CWs)and species within the genera Chitinivibrio-nia and Anaerolineaceae,suggesting that microbial interactions primarily manifest as indirect facilitative effects rather than direct mutualistic relationships.Given that the Normalized Stochasticity Ratio in CWs were<50%,this study inferred that environmental gradients have greater influence on anammox bacteria than microbial interactions.
基金supported by the Russian Science Foundation(No.22-13-00035)the National Outstanding Young Scientists Fund(No.52125002)+14 种基金the National Key Research and Development Program of China(Nos.2023YFC3904800 and 2022YFB4002501)the National Natural Science Foundation of China(Nos.52400228,52300139,22308063,52103340,U22A20418,22578302,52202208,52400163,52205054,22075171,52177214,22405201,52371072,52171078,52377218)the Key Research and Development Project of Science and Technology Department of Zhejiang Province(No.2024C03284(SD2))the Research Development Fund of Zhejiang A&F University(No.2024LFR042)the President Research Funds from Xiamen University(No.ZK1111)Nanqiang Youth Scholar program of Xiamen University,the Young Elite Scientists Sponsorship Program by CAST(No.2023QNRC001)Natural Science Foundation of Xiamen(No.3502z202471037)Open Fund of the State Environmental Protection Key Laboratory of Urban Air Particulate Matter Pollution Prevention and Control,College of Environmental Science and Engineering,Nankai University(No.NKPMLF202409)the Key Project of Research and Development Plan of Jiangxi Province(No.20243BBI91001)Natural Science Foundation of Shanghai(No.23ZR1423400)the Postdoctoral Science Research Program of Shaanxi(No.2023BSHEDzZ159)Xidian University Specially Funded Project for Interdisciplinary Exploration(No.TZJH2024062)the Open Project of Yunnan Precious Metals Laboratory Co.,Ltd.(No.YPML-20240502058)the Fundamental Research Program of Shanxi Province(No.202303021212159)the Natural Science Foundation of Shanxi Normal University(No.JCYJ2024017).
文摘Sustainable development for our life is important task,which is driven by key materials and technologies.In this roadmap,we discuss three main aspects in addressing environmental questions,green chemical processes and energy challenges.They are included,such as gas treatment and separation,wastewater treatment,waste gas treatment,solid waste treatment,lithium extraction,hydrogen production,water splitting,CO_(2) reduction,photocatalytic clean technologies,plastic degradation,fuel cells,lithium batteries,sodium batteries,aqueous batteries,solid state batteries,metal air batteries and supercapacitors.Their status,challenges,progress and future perspectives are also discussed.We hope that this paper can give clear views on sustainable development in materials and technologies.
基金the support of the National Natural Science Foundation of China(NSFC)(Nos.52425003,22188102,and 52400144)the Project funded by China Postdoctoral Science Foundation(Nos.BX20220325 and 2023M743707)the Youth Innovation Promotion Association,CAS(Nos.Y2021020 and Y2022023).
文摘Air pollution is a major challenge to the improvement of urban environmental quality.The control of air pollution still faces severe challenges,especially in developing countries,such as ozone pollution control.Ozone is a typical secondary air pollutant,and its formation chemistry from its precursors(NOx and volatile organic compounds)is highly nonlinear,which caused the emission reduction of its precursors is not always effective and therefore new assisted approaches to control of ozone pollution are needed.Photocatalysis and ambient catalysis technology are expected to be applied in open atmosphere as a new booster to the direct purification of air pollutants in emission sources.In this perspective,we summarize the current knowledge about the photocatalysis and ambient catalysis technology for the removal of air pollutants under natural photothermal conditions.Based on these technologies,we propose the concept of“Environmental Catalytic City”,which refers to the spontaneous purification of low concentration urban air pollutants in the atmosphere by catalytic materials coating on the artificial surfaces,such as building surfaces in the city.In this way,the urban city with self-purification function can remove air pollution without additional energy consumption.The further improvement,development,and application of the“Environmental Catalytic City”is also discussed.
基金supported by the Natural Science Foundation of Xiamen,China(No.3502Z20227238)the National Natural Science Foundation of China(Nos.22276181 and 52300143)+3 种基金the Science and Technology Planning project of Fujian Province,China(Nos.2022H0045 and 2023I0035)the Youth Innovation Promotion Associ-ation CAS(No.2019307)China Postdoctoral Science Foundation(No.2022M723082)the Youth Science and Technology Innovation Pro-gram of Xiamen Ocean and Fisheries Development Special Funds(No.23ZHZB032QCA20).
文摘A novel hierarchical porous metal-organic framework(MOF)-based hollow carbon nanofiber mat(CNFM)was prepared through a facile electrospinning process followed by carbonization.Two immiscible polymers,polyacrylonitrile/polymethyl methacrylate(PAN/PMMA),and porous zeolitic imidazolate framework-8(ZIF-8)particles were selected as components for the electrospinning suspension.The resulting PPZ-CNFM-1–2–2(PAN:PMMA:ZIF8=1:2:2,mass ratio)exhibited a hollow tubular structure with uniformly distributed dense hollow-spheres on the tube walls.The obtained CNFM possessed a high Brunauer-Emmett-Teller specific surface area(SBET)of 1696 m2/g and total pore volume of 2.74 cm^(3)/g,which are comparable to those achieved by traditional physical or chemical activation methods.This MOF-based CNFM demonstrated excellent adsorption performance towards ciprofloxacin(CIP),exhibiting a high static adsorption capacity of approximately 600 mg/g and achieving adsorption equilibrium withing only 1 h.The exceptional adsorption capacity can be attributed to its high SBET and abundant pores that accommodate CIP molecules,while the rapid adsorption rate is facilitated by the presence of hollow-sphere and hollow tubular structures in the carbon nanofibers.Furthermore,the study revealed the significant contributions of pore-filling effect during the adsorption process.Fixed-bed experiments confirmed that this MOF-based hollow CNFM holds great potential for large-scale applications in purifying CIP-contaminated water.
基金supported by National Natural Science Foundation of China(No.52103044)Double First-Class Initiative University of Science and Technology of China(KY2400000037)the Young Talent Programme(GG2400007009).
文摘Conductive elastomers combining micromechanical sensitivity,lightweight adaptability,and environmental sustainability are critically needed for advanced flexible electronics requiring precise responsiveness and long-term wearability;however,the integration of these properties remains a significant challenge.Here,we present a biomass-derived conductive elastomer featuring a rationally engineered dynamic crosslinked network integrated with a tunable microporous architecture.This structural design imparts pronounced micromechanical sensitivity,an ultralow density(~0.25 g cm^(−3)),and superior mechanical compliance for adaptive deformation.Moreover,the unique micro-spring effect derived from the porous architecture ensures exceptional stretchability(>500%elongation at break)and superior resilience,delivering immediate and stable electrical response under both subtle(<1%)and large(>200%)mechanical stimuli.Intrinsic dynamic interactions endow the elastomer with efficient room temperature self-healing and complete recyclability without compromising performance.First-principles simulations clarify the mechanisms behind micropore formation and the resulting functionality.Beyond its facile and mild fabrication process,this work establishes a scalable route toward high-performance,sustainable conductive elastomers tailored for next-generation soft electronics.
基金supported by the National Key R&D Program of China(No.2023YFC3707200)the National Natural Science Foundation of China(Nos.22306191 and 52270112).
文摘Selective catalytic reduction with NH3(NH3-SCR)is an important means of NO_(x) abatement from stationary and mobile sources,and the key element is efficient and stable NH3-SCR catalysts.In this study,we propose a method to construct superior Fe-Beta catalysts based on Al-rich zeolites.This strategy successfully promotes the formation of NH3-SCR-active isolated Fe^(3+)species,thus effectively improving the low-temperature activity of the Fe-Beta catalysts.Thanks to the abundant Brønsted acid sites of the Al-rich zeolite,the Fe_(2)O_(3) particles are redispersed and anchored as isolated Fe^(3+)during hydrothermal aging.This dynamic evolution of Fe species makes up for the adverse effect of dealumination of the Al-rich zeolite framework and achieves high stability for the Al-rich Fe-Beta catalyst.This study may promote the understanding of highly efficient and stable catalyst design using Al-rich zeolites.
文摘Emerging contaminants in water sources present serious environmental and health risks,creating an urgent need for efficient and reliable treatment strategies.Photocatalytic advanced oxidation processes(AOPs)provide rapid reaction rates and strong oxidation capabilities,however,comprehensive evaluations of wastewater treatment,including degradation pathways,toxicity assessments and mechanistic insights,remain underexplored in the literature.This study presents novel S-scheme Mn_(0.5)Cd_(0.5)S/In_(2)S_(3)(MCS/IS)photocatalysts for efficient degradation of antibiotic pollutants,with a particular focus on tetracycline hydrochloride(TCH).The optimized MCS/IS photocatalyst demonstrates exceptional degradation efficiency and robust resistance to inorganic anions.Additionally,a continuous-flow wastewater treatment system,using an MCS/IS membrane,demonstrates outstanding stability in TCH photodegradation.Utilizing response surface methodology and Fukui function analysis,the effects of various parameters on photocatalytic degradation rates,along with the associated pathways and intermediate products,have been thoroughly investigated.Toxicity assessments confirm the environmental safety of the treated effluents.Mechanistic studies show that the S-scheme heterojunction in the MCS/IS photocatalyst improves electron-hole separation,thereby enhancing photocatalytic performance.It is expected that this study will serve as a model for advancing the removal of emerging contaminants,further enhancing photocatalytic AOPs as sustainable water purification technologies.
基金supported by the National Key Research and Development Program of China(Nos.2021YFA1200101 and 2021YFA1200104)the National Natural Science Foundation of China(Nos.21635005,21890741,22174134,and 22474133)the CAS Project for Young Scientists in Basic Research(YSBR-054).
文摘Electrochemical processes lie at the core of biological function,governing energy transduction,metabolic flux,and mo-lecular signaling.Recent advances in electrochemical science now allow these processes to be probed and controlled with unprecedented spatial,temporal,and chemical resolution.In this review,we present an integrated framework that pro-gresses from fundamental mechanisms to analytical technologies and functional modulation.We begin by outlining elec-tron transfer pathways in mitochondrial respiration,microbial extracellular electron transfer,and DNA-and protein-based charge conduction,followed by the principles of photon-electron conversion in photosynthesis and the central role of redox equilibrium in coordinating cellular responses.We then highlight electrochemical analytical strategies that enable multiscale biological characterization,including biosensing,electrochemical and scanning probe imaging,electrogenerated chemilu-minescence detection,and measurements of membrane potentials and neurotransmitter dynamics.Emerging platforms such as flexible biointerfaces,ultramicroelectrodes,and nanopore systems further extend these capabilities to in vivo and single-molecule contexts.Finally,we discuss how electrochemical inputs can be used to regulate metabolic pathways,mi-crobial and protein activities,and neural signaling,enabling precision therapeutic and bioengineering applications.Togeth-er,these developments establish electrochemistry as a powerful foundation for decoding and directing biological systems.
基金the financial support from the National Key R&D Program of China(2022YFA1504200)the Zhejiang Provincial Natural Science Foundation(No.LR22B060003)+2 种基金the National Natural Science Foundation of China(22322810,22078293,22141001,and 22008211)the Fundamental Research Funds for the Provincial Universities of Zhejiang(RF-C2023004)the Midea Group-Zhejiang University of Technology Joint Development Funding(KYY-HX-20240263)。
文摘The anodic electrochemical ozone production(EOP)and the cathodic three-electron oxygen reduction reaction(3e^(-)ORR)are effective processes for generating active oxygen species(ROS).However,the activation of ozone(O_(3))by hydroxyl radical(OH)to form ROS poses significant challenges.The micelle balllike bimetallic La-Nb oxides(LNOx)have been developed as a bifunctional electrocatalyst for both the EOP and 3e^(-)ORR reactions.The LNO20 demonstrated a 9.8%of Faradaic efficiency(FE)in O_(3)production and a transfer number of 2.8 electrons in the 3e^(-)ORR.Theoretical calculations support the notion that the five-membered ring mechanism in LNO20 facilitates O_(3)production.Additionally,the incorporation of La provides active sites that enhance the activation of hydrogen peroxide(^(*)H_(2)O_(2))and the generation of OH.This innovative approach synergistically integrates EOP and 3e^(-)ORR,enhancing the activation of O_(3)to produce ROS,demonstrating exceptional efficacy in the degradation of organic pollutants and antimicrobial activity.The study paves the way for designing advanced electrocatalysts for EOP and 3e^(-)ORR and offers insights into utilizing electrochemical method to support other antibacterial strategies.
基金supported by the National Natural Science Foundation of China(No.42192514)Guangdong Major Project of Basic and Applied Basic Research(No.2023B0303000007)and Guangdong Foundation for Program of Science and Technology Research(No.2023B1212060049)。
文摘Dissolved organic matter(DOM)is ubiquitous in the environment and plays an important role in global ecosystems.However,our understanding of the evolution and molecular diversity of DOM from different biomass materials and biochar is not enough.Herein,we investigated the changes in DOM from seven biomass and biochar samples over a bio-incubation of 28 days,and explored their contents,and optical,chemical,and molecular characteristics.The results indicated that dissolved organic carbon(DOC)from different sources all exhibited a gradually decreasing trends during the incubation,while the absorbance and aromaticity gradually increased.Biomass DOM was characterized by higher DOC concentrations and a higher degradation rate,whereas biochar DOM had high aromaticity and little variability.Parallel factor analysis results showed that the protein-like fluorescent groups were as only detected in biomass DOM,while the dominant humic-like components were identified in biochar DOM.Additionally,the molecular composition of DOM from different sources was different,and biomass DOM contained more carbohydrate-like and saturated compounds.More sulfur-containing compounds were detected in Ceratophyllum demersum(CD)DOM,which may indicate that the leaching of CD litter was an important source of sulfur-containing species in aquatic environments.Furthermore,biochar DOM had greater aromaticity and a higher degree of oxidation than the corresponding biomass DOM.This study provided a detailed understanding of the molecular diversity of DOM by considering its various sources,and the results are helpful for further understanding their chemical properties and structures.
基金supported by the National Key R&D Program of China(2024YFA1211004)the National Natural Science Foundation of China(52300069,52192681,U21A20160)+1 种基金the Natural Science Foundation of Jiangsu Province(BK20230276)Science and Technology Program of Suzhou,China(SWY20222003,2022SS19).
文摘In photocatalytic water treatment processes,the particulate photocatalysts are typically immobilized on membrane,through either chemical/physical loading onto the surface or directly embedding in the membrane matrix.However,these immobilization strategies inevitably compromise the interfacial mass diffusion and cause activity decline relative to the suspended catalyst.Here,we propose a binder-free surface immobilization strategy for fabrication of high-activity photocatalytic membrane.Through a simple dimethylformamide(DMF)treatment,the nanofibers of polyvinylidene fluoride membrane were softened and stretched,creating enlarged micropores to efficiently capture the photocatalyst.Subsequently,the nanofibers underwent shrinking during DMF evaporation,thus firmly strapping the photocatalyst microparticles on the membrane surface.This surface self-bounded photocatalytic membrane,with firmly bounded yet highly exposed photocatalyst,exhibited 4.2-fold higher efficiency in hydrogen peroxide(H_(2)O_(2))photosynthesis than the matrix-embedded control,due to improved O_(2)accessibility and H_(2)O_(2)diffusion.It even outperformed the suspension photocatalytic system attributed to alleviated H_(2)O_(2)decomposition at the hydrophobic surface.When adopted for UV-based water treatment,the photocatalytic system exhibited tenfold faster micropollutants photodegradation than the catalyst-free control and demonstrated superior robustness for treating contaminated tap water,lake water and secondary wastewater effluent.This immobilization strategy can also be extended to the fabrication of other photocatalytic membranes with diverse catalyst types and membrane substrate.Overall,our work opens a facile avenue for fabrication of high-performance photocatalytic membranes,which may benefit advanced oxidation water purification application and beyond.
基金supported by the National Science Fund for Distinguished Young Scholars(No. 50625823)the Program of Research on Key Technology of Environmental Pollution Control and Quality Improvement(No. 2007DFC90170)
文摘Bisphenol A （BPA） is of global concern due to its disruption of endocrine systems and ubiquity in the aquatic environment. It is important, therefore, that efforts are made to remove it from the aqueous phase. A novel adsorbent, mesoporous carbon CMK-3, prepared from hexagonal SBA- 15 mesoporous silica was studied for BPA removal from aqueous phase, and compared with conventional powdered activated carbon （PAC）. Characterization of CMK-3 by transmission electron microscopy （TEM）, X-ray diffraction, and nitrogen adsorption indicated that prepared CMK-3 had an ordered mesoporous structure with a high specific surface area of 920 m^2/g and a pore-size of about 4.9 nm. The adsorption of BPA on CMK-3 followed a pseudo second-order kinetic model. The kinetic constant was 0.00049 g/（mg.min）, much higher than the adsorption of BPA on PAC. The adsorption isotherm fitted slightly better with the Freundlich model than the Langmuir model, and adsorption capacity decreased as temperature increased from 10 to 40℃. No significant influence of pH on adsorption was observed at pH 3 to 9; however, adsorption capacity decreased dramatically from pH 9 to 13.
基金The authors declare that the work of Co-author Dr.Liang Chen was partially supported by the National Key R&D Program of China(2016YFC0401405)the National Natural Science Foundation of China(No.41772245).
文摘Coal preparation solid waste,which is a major environmental issue for coal-producing areas in China,may be microbiologically digested and transformed into a product suitable as a soil amendment to increase soil organic matter content and prevent and enhance plant/crop growth.Coal preparation waste collected from a coal sorting plant in Inner Mongolia,China was digested in bioreactors inoculated with microbial enrichments prepared from activated sludge and cow manure.The effluent solids from the coal preparation waste bioreactors were analyzed for their suitability as organic soil amendments,which complied with China standards.Plant growth tests were conducted in sandy soil from a semi-arid region in Colorado,which was amended with the effluent solids.Kentucky bluegrass(Poa pratensis L.)and chives(Allium schoenoprasum)were used as the representative plants for the growth tests,where results indicated substantially higher yields of Kentucky bluegrass and chives for the sandy soils amended with the effluent solids when compared to a commercial organic fertilizer.The number and average length of Kentucky bluegrass shoots were 10 and 5.1 times higher,respectively,in soils amended with the effluent solids.Similarly,the number and average length of chives shoots were 10 and 1.7 times higher,respectively,in soils amended with the effluent solids.Overall,the microbial digestion of coal preparation waste for application as an organic soil amendment is a viable alternative and beneficial use of coal preparation solid waste.
基金This work was supported by the National Natural Science Foundation of China （Grant No. 41301572） Tsinghua Univcrsity- Vcolia Environnmcnt Joint Research Center for Advanced Environmental Technology.
文摘An environmental risk assessment was performed for pharmaceutical compounds present in the aquatic environment of China. Predicted environmental concentration （PEC） of the compounds were calculated according to European Medicines Evaluation Agency （EMEA） guidelines. Available ecotoxicological data compromised by applying a very conservative assessment factor （AF） were employed to calculate the predicted noeffect concentration （PNEC）. The screening principle and the risk assessment were based on risk quotient （RQ）, which derived from the PEC and related PNEC values. PEC results indicated that all the compounds except sulfadimethoxine and levocamitine, should carry out phase II risk assessment in EMEA guideline. RQ values suggested that more than 36 pharmaceuticals may be imposed health threats to the aquatic environment; especially the antibiotic therapeutic class including amoxicillin, sulfasalazine, trimethoprim, oxytetracycline and erythromycin showed high RQ values. These substances with high RQ value （RQ≥ 1） were regarded as top- priority pharmaceuticals for control in the aquatic environment of China. However, the antibiotic substances which had low risk quotient （RQ 〈 1）, should be reassessed by its potentially induced resistance under low concentration in future.
基金financially supported in part by the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB0450401)the National Natural Science Foundation of China(U23A2091,22122506,22479140,22479139,22232003,22075267,22109152)+3 种基金Anhui Provincial Natural Science Foundation(2408085JX001)Youth Innovation Promotion Association of CAS(Y2023129)Fundamental Research Funds for the Central Universities(20720220007,WK2060000039,KY2140000031)West Light Foundation of the Chinese Academy of Sciences(xbzg-zdsys-202209).
文摘Photocatalytic ammonia(NH_(3))decomposition is a key strategy for green hydrogen production and renewable energy conversion.Although conventional plasmonic metal/TiO_(2) composites exhibit some activity,their applications are constrained by high carrier recombination rates and narrow light harvesting ranges.To address these challenges,this study innovatively introduces the plasmonic semiconductor MoO_(3-x),which is characterized by broad-spectrum absorption and abundant oxygen vacancies,to construct a Cu-MoO_(3-x)/TiO_(2) plasmon resonance coupling nanostructure.The construction of the Cu-MoO_(3-x) composite stabilizes Cu via MoO_(3-x) coating and facilitates electron transfer from Cu to MoO_(3-x),generating more oxygen vacancies for NH_(3) activation.The visible localized surface plasmon resonance(LSPR)response of Cu,coupled with the visible to near-infrared LSPR resonance of MoO_(3-x),broadens the spectral response and optimizes carrier dynamics,thereby reducing the recombination of photogenerated carriers.The use of hot carriers and plasmonic photothermal effects synergistically accelerate surface reaction kinetics and enhance photocatalytic efficiency.In particular,the optimal Cu-MoO_(3-x)/TiO_(2) catalyst results in an enhanced NH_(3) decomposition rate of 103.2 mmol·g^(-1)·h^(-1) under fullspectrum light irradiation,representing 29-fold and 94-fold enhancements over those of Cu/TiO_(2) and MoO_(3-x)/TiO_(2),respectively.This innovative design strategy transcends traditional plasmonic metal/semiconductor catalyst designs and opens new avenues for developing efficient solar-driven plasmon resonance coupling catalysts.
基金National Key Research and Development Program(2022YFA1505500)National Natural Science Foundation of China(92477132,22376194)+4 种基金Talent Plan of Shanghai Branch,Chinese Academy of Sciences(CASSHBQNPD-2023-023)Youth Innovation Promotion Association of Chinese Academy of Sciences(2022309)Ningbo Key Technology Breakthrough Scheme Projects under Yongjiang Science and Innovation 2035(2024Z237)Natural Science Foundation of Fujian Province,China(2023J02030)National Science Foundation of China(22203012)(G.S.)。
文摘Overcoming the kinetic barrier of N-H bond activation in NH_(3)remains a central challenge in enabling efficient ammonia decomposition as well as thermocatalytic and electrocatalytic ammonia oxidation.Oxide-on-metal inverse catalysts offer promising opportunities to address this challenge;however,the role of oxide overlayer thickness in governing surface structures and reactivity is still poorly understood.Herein,we have elucidated the layer-dependent atomic structure of vanadium oxide overlayers on Cu(111)surfaces and its implications for NH_(3)adsorption,using a combination of high-resolution scanning tunneling microscopy(STM),X-ray photoelectron spectroscopy(XPS),and density functional theory(DFT)calculations.Despite sharing the same vanadium oxidation state(V^(3+)),VO_(x)overlayers on Cu(111)adopt distinct atomic structures depending on the overlayer thickness.A nonlinear correlation is observed between VO_(x)overlayer thickness and N-H activation capability.The surface-V_(2)O_(3)phase formed by 2-3 VO_(x)layers exhibits the highest activity,enabling both molecular and dissociative adsorption of NH_(3).In contrast,thicker bulk-V_(2)O_(3)(0001)(>3 VO_(x)layers)only shows molecular adsorption without dissociation,while the monolayer VO(111)surface exhibits negligible NH_(3)adsorption.These findings underscore the pivotal influence of oxide overlayer thickness in modulating oxide-on-metal inverse catalyst systems,providing atomic-level insights that can guide the rational design of high-performance catalytic materials for NH_(3)activation.
基金supported by the National Natural Science Foundation of China(22076036,52192684 and 52027815)the Anhui Provincial Natural Science Foundation(2308085J23 and 2408055US005).
文摘CONSPECTUS:Electrochemical water purification and pollutant monitoring have garnered significant attention due to their unique technical advantages.The pursuit of safe,efficient,and economically viable catalysts remains a critical priority.Titanium dioxide(TiO_(2)),a prototypical transition-metal oxide with substantial industrial importance,is widely recognized as a benchmark catalyst for photochemical reactions.However,its practical application is limited by restricted light absorption and rapid photocarrier recombination.Recently,TiO_(2) has emerged as a promising candidate in electrochemical catalysis,particularly in the fields of energy and environmental science.Its atomic and electronic structures can be precisely engineered through advanced techniques such as nanoscale morphology control,polar-facet engineering,vip-metal doping,and structural-defect modulation.This review examines recent advancements in TiO_(2)-based electrochemical applications,with a focus on water purification and pollutant monitoring.In this Account,we present our efforts to harness facet-and defect-engineered TiO_(2) as electrochemical catalysts for water purification,addressing critical challenges such as low conductivity and poor reactivity.Initially,we demonstrate that facetengineered TiO_(2),specifically designed to expose the high-energy{001}polar facet,facilitates the dissociation of both pollutant and water molecules.This significantly lowers energy barriers and enhances anodic reactions through both direct and indirect pathways,thereby markedly improving water purification efficiency.Furthermore,the dual photochemical and electrochemical functionalities of a single{001}-tailored TiO_(2) electrode enable synergistic UV-light-assisted electrochemical catalysis under low bias conditions,achieving superior energy efficiency and resistance to electrode fouling.Next,we explore the catalytic potential of defect-engineered TiO_(2)(TiO_(2−x)),highlighting the role of titanium(Ti^(3+))and oxygen vacancies(O_(v))in boosting electrochemical water purification.Surface and subsurface defects,characterized by localized atomic disorder and structural distortions,serve as active sites that drive beneficial structural transformations,enriched electronic distribution,enhanced spin−spin correlations,and polaron hopping mechanisms,all of which contribute to improved cathodic reduction.To stabilize these reactive sites under anodic polarization,we propose a practical visible-light-assisted electrochemical catalysis strategy.This approach leverages mild non-band-gap excitation pathways mediated by defect sub-bands,providing enhanced stability and catalytic efficiency.Finally,we identify the challenges associated with the application of self-engineered TiO_(2) in electrochemical water purification and outline directions for future research.Our studies deepen the fundamental understanding of structure−catalysis relationships and exemplify a self-tailoring strategy to advance oxide catalysis without reliance on noble or toxic-metal cocatalysts.By elucidating catalytic mechanisms and adopting innovative synthesis techniques,our insights provide a foundation for designing advanced electrocatalysts.Self-engineered TiO_(2) holds the potential to establish a new paradigm in electrochemical catalysis,opening pathways for transformative solutions in environmental remediation.
文摘Electron paramagnetic resonance(EPR)is a spectroscopic approach that can directly and non-destructively detect and char-acterize species with unpaired electrons,such as radicals,transi-tion metal ions,defects in materials,and the excited triplet state of molecules[1].To date,the EPR technique has become an indis-pensable component in the toolbox of environmental studies.Using various diamagnetic probes(e.g.,5,5-dimethyl-1-pyrroline-N-oxide(DMPO))as the spin traps,transient reactive species can be transformed to EPR-detectable(meta)stable spin adducts,which enables radical identification and mechanism interpretation.Therefore,EPR constitutes a versatile platform for the mechanistic investigation of advanced oxidation processes(AOPs)in the field of water purification and contaminated groundwater remediation[2].
基金National Natural Science Foundation of China(Nos.52200074 and 52192684)the Fundamental Research Funds for the Central Universities(No.21625309)for supporting this work.
文摘Conductive additive such as biochar have been extensively employed to enhance anaerobic digestion(AD)performance for over a decade.Among the proposed mechanisms,conductive additive-facilitated direct interspecies electron transfer(DIET)is frequently cited as a key contributor to these performance improvements.Because this process is believed to bypass traditional diffusible intermediates(e.g.,H_(2) or formate),it can enable more efficient energy transfer between syntrophic partners and accelerate substrate degradation,potentially leading to higher methane yields and improved overall stability of the anaerobic digestion process.However,benefits regarding conductive additivefacilitated DIET often rely on indirect indicators rather than direct experimental evidence.Here,we advocate for a critical reassessment on the benefits of conductive additive for DIET in AD.Specifically,we emphasize the importance of establishing standardized experimental protocols and obtaining direct evidence to confirm the occurrence and significance of DIET in conductive additive-amended AD system.Furthermore,it is essential to distinguish DIET from other enhancement mechanisms such as pH buffering and toxin adsorption that may independently contribute to improved AD performance,with the goal of advancing its practical implementation.
基金supported by the National Natural Science Foundation of China(No.22276183)the Institute of Urban Environment,Chinese Academy of Sciences(No.IUE-JBGS-202212)the Youth Innovation Promotion Association,Chinese Academy of Sciences(No.Y2022082).
文摘Electroactive microorganisms are integral to biogeochemical cycles through extracellular electron transfer and have potential applications in environmental remediation.However,their long-term competitive interactions and evolutionary dynamics with non-electroactive microorganisms remain poorly understood.In this study,we conducted a 320-day cultivation experiment in which monocultures of the electroactive Shewanella oneidensis MR-1,the non-electroactive Citrobacter freundii An1,and their cocultures were compared under three single electron acceptor conditions:anaerobic(no exogenous electron acceptor),ferrihydrite,or oxygen.After 320 d,S.oneidensis MR-1 presented the highest relative abundance of 30.94%±0.74%in the ferrihydrite cocultures.S.oneidensis MR-1 maintained ferrihydrite reduction capacity after cultivation under all three conditions,indicating the long-term stability of its extracellular electron transfer.Moreover,no other phenotypic evolution was observed in S.oneidensis MR-1 after ferrihydrite or anaerobic cultivation.In contrast,both monocultured and cocultured S.oneidensis MR-1 exhibited enhanced adaptation to oxygen,characterized by increased growth rates,metabolic activity,and reduced cell aggregation.Notably,substrate consumption increased in monocultures but decreased in cocultures,suggesting an optimization of metabolic efficiency in the latter.Genome sequencing revealed mutations in genes associated with cell division,adenosine triphosphate synthesis,lactate metabolism,and flagellar/pilus expression in S.oneidensis MR-1.Interestingly,the ferrihydrite-adapted groups also exhibited enhanced adaptation to oxygen.83.96%of mutations were shared across all culture systems and enriched in environmental signal-sensing pathways,indicating that parallel genomic evolution facilitated cross-environmental adaptation.Our findings reveal the ecological evolution of electroactive microorganisms in diverse redox environments and establish a foundation for engineering electroactive communities.
