Phthalic acid esters(PAEs)are widely released into the environment due to industrial and agricultural activities.This poses significant risks,not only to crops grown on contaminated soil but also to humans.PAEs enter ...Phthalic acid esters(PAEs)are widely released into the environment due to industrial and agricultural activities.This poses significant risks,not only to crops grown on contaminated soil but also to humans.PAEs enter the human body through the food chain,causing potential health hazards.Endophytic bacteria have demonstrated a significant potential as effective bioremediation agents,with specialized mechanisms of PAEs degradation.Endophytic bacteria such as Rhodococcus,Pseudomonas and Sphingomona recognize root exudates,adhere to and penetrate root surfaces,and ultimately colonize crops.They form symbiotic relationships with crops,obtaining nutrients and habitats from crops,meanwhile,promoting plant growth and health through hormone production,nutrient regulation,and the suppression of pathogenic microorganisms.Furthermore,endophytic bacteria efficiently degrade PAEs in soil-crop systems through synergistic interactions with indigenous rhizosphere microflora and regulatory effects on enzyme activity in crops.Here,we review the role of endophytic bacteria in the bioremediation of PAEs-contaminated crops and soils.In addition,we discuss the scarcity of endophytic bacterial strains with a confirmed ability to degrade PAEs,and underscore the lack of the research on the mechanisms of PAEs degradation by these bacteria.This review also points out that future study should investigate the molecular mechanisms underlying the interaction between endophytic bacteria and PAEs to offer novel insights and solutions for environmental protection and sustainable agricultural development.展开更多
The hydrogen evolution reaction performance of semiconducting 2H-phase molybdenum disulfide(2H-MoS_(2))presents a significant hurdle in realizing its full potential applications.Here,we utilize theoretical calculation...The hydrogen evolution reaction performance of semiconducting 2H-phase molybdenum disulfide(2H-MoS_(2))presents a significant hurdle in realizing its full potential applications.Here,we utilize theoretical calculations to predict possible functionalized graphene quantum dots(GQDs),which can enhance HER activity of bulk MoS_(2).Subsequently,we design a functionalized GQD-induced in-situ bottom-up strategy to fabricate near atom-layer 2H-MoS_(2) nanosheets mediated with GQDs(ALQD)by modulating the concentration of electron withdrawing/donating functional groups.Experimental results reveal that the introduction of a series of functionalized GQDs during the synthesis of ALQD plays a crucial role.Notably,the higher the concentration and strength of electron-withdrawing functional groups on GQDs,the thinner and more active the resulting ALQD are.Remarkably,the synthesized near atom-layer ALQD-SO_(3)demonstrate significantly improved HER performance.Our GQD-induced strategy provides a simple and efficient approach for expanding the catalytic application of MoS_(2).Furthermore,it holds substantial potential for developing nanosheets in other transition-metal dichalcogenide materials.展开更多
High-efficiency electrochemical hydrogen evolution reaction(HER)offers a promising strategy to address energy and environmental crisis.Platinum is the most effective electrocatalyst for the HER.However,challenging sca...High-efficiency electrochemical hydrogen evolution reaction(HER)offers a promising strategy to address energy and environmental crisis.Platinum is the most effective electrocatalyst for the HER.However,challenging scarcity,valuableness,and poor electrochemical stability still hinder its wide application.Here,we designed an outstanding HER electrocatalyst,highly dispersed rhodium(Rh)nanoparticles with an average diameter of only 3 nm supported on boron(B)nanosheets.The HER catalytic activity is even comparable to that of commercial platinum catalysts,with an overpotential of only 66 mV in 0.5 M H_(2)SO_(4) and 101 mV in 1 M KOH to reach the current density of 10 mA cm−2.Meanwhile,the catalyst exhibited impressive electrochemical durability during long-term electrochemical processes in acidic and alkaline media,even the simu-lated seawater environment.Theoretical calculations unraveled that the structure-activity relationship between B(104)crystal plane and Rh(111)crystal plane is beneficial to the release of hydrogen,and surface O plays a vital role in the catalysis process.Our work may gain insights into the development of supported metal catalysts with robust catalytic performance through precise engineering of the strong metal-supported interaction effect.展开更多
Perfluorinated or polyfluorinated compounds(PFCs)continue entering to the environmental as individuals or mixtures,but their toxicological information remains largely unknown.Here,we investigated the toxic effects and...Perfluorinated or polyfluorinated compounds(PFCs)continue entering to the environmental as individuals or mixtures,but their toxicological information remains largely unknown.Here,we investigated the toxic effects and ecological risks of Perfluorooctane sulfonic acid(PFOS)and its substitutes on prokaryotes(Chlorella vulgaris)and eukaryotes(Microcystis aeruginosa).Based on the calculated EC50 values,the results showed that PFOS was significantly more toxic to both algae than its alternatives including Perfluorobutane sulfonic acid(PFBS)and 6:2 Fluoromodulated sulfonates(6:2 FTS),and the PFOS-PFBS mixture was more toxic to both algae than the other two PFC mixtures.The action mode of binary PFC mixtures on Chlorella vulgaris was mainly shown as antagonistic and on Microcystis aeruginosa as synergistic,by using Combination index(CI)model coupled with Monte Carlo simulation.The mean risk quotient(RQ)value of three individual PFCs and their mixtures were all below the threshold of 10^(−1),but the risk of those binary mixtures were higher than that of PFCs individually because of their synergistic effect.Our findings contribute to enhance the understanding of the toxicological information and ecological risks of emerging PFCs and provide a scientific basis for their pollution control.展开更多
Compared with the traditional heteroatom doping,employing heterostructure is a new modulating approach for carbon-based electrocatalysts.Herein,a facile ball milling-assisted route is proposed to synthesize porous car...Compared with the traditional heteroatom doping,employing heterostructure is a new modulating approach for carbon-based electrocatalysts.Herein,a facile ball milling-assisted route is proposed to synthesize porous carbon materials composed of abundant graphene/hexagonal boron nitride(G/h-BN)heterostructures.Metal Ni powder and nanoscale h-BN sheets are used as a catalytic substrate/hard template and“nucleation seed”for the formation of the heterostructure,respectively.As-prepared G/h-BN heterostructures exhibit enhanced electrocatalytic activity toward H_(2)O_(2) generation with 86%-95%selectivity at the range of 0.45-0.75 V versus reversible hydrogen electrode(RHE)and a positive onset potential of 0.79 versus RHE(defined at a ring current density of 0.3 mA cm^(-2))in the alkaline solution.In a flow cell,G/h-BN heterostructured electrocatalyst has a H_(2)O_(2) production rate of up to 762 mmol g_(catalyst)^(-1) h^(-1) and Faradaic efficiency of over 75%during 12 h testing,superior to the reported carbon-based electrocatalysts.The density functional theory simulation suggests that the B atoms at the interface of the G/h-BN heterostructure are the key active sites.This research provides a new route to activate carbon catalysts toward highly active and selective O_(2)-to-H_(2)O_(2) conversion.展开更多
Electrochemical reduction of CO_(2)(CO_(2)RR)to value-added chemicals is an attractive strategy for greenhouse gas mitigation and carbon recycle.Carbon material is one of most promising electrocatalysts but its produc...Electrochemical reduction of CO_(2)(CO_(2)RR)to value-added chemicals is an attractive strategy for greenhouse gas mitigation and carbon recycle.Carbon material is one of most promising electrocatalysts but its product selectivity is limited by few modulating approaches for active sites.Herein,the predominant pyridinic N-B sites(accounting for 80%to all N species)are fabricated in hierarchically porous structure of graphene nanoribbons/amorphous carbon.The graphene nanoribbons and porous structure can accelerate electron and ion/gas transport during CO_(2)RR,respectively.This carbon electrocatalyst exhibits excellent selectivity toward CO_(2)reduction to CH_(4)with the faradaic efficiency of 68%at−0.50 V vs.RHE.As demonstrated by density functional theory,a proper adsorbed energy of∗CO and∗CH_(2)O are generated on the pyridinic N-B site resulting into high CH_(4)selectivity.Therefore,this study provides a novel method to modulate active sites of carbon-based electrocatalyst to obtain high CH_(4)selectivity.展开更多
基金supported by the National Natural Science Foundation of China(No.22161132011)Jiangsu Provincial Special Fund for S&T Innovation in Carbon Emission Peak and Neutrality(No.20220013)+1 种基金the National Key Research and Development Program of China(Nos.2023YFE0110800 and 2023YFC3708100)the Fundamental Research Funds for the Central Universities(No.QTPY2024001).
文摘Phthalic acid esters(PAEs)are widely released into the environment due to industrial and agricultural activities.This poses significant risks,not only to crops grown on contaminated soil but also to humans.PAEs enter the human body through the food chain,causing potential health hazards.Endophytic bacteria have demonstrated a significant potential as effective bioremediation agents,with specialized mechanisms of PAEs degradation.Endophytic bacteria such as Rhodococcus,Pseudomonas and Sphingomona recognize root exudates,adhere to and penetrate root surfaces,and ultimately colonize crops.They form symbiotic relationships with crops,obtaining nutrients and habitats from crops,meanwhile,promoting plant growth and health through hormone production,nutrient regulation,and the suppression of pathogenic microorganisms.Furthermore,endophytic bacteria efficiently degrade PAEs in soil-crop systems through synergistic interactions with indigenous rhizosphere microflora and regulatory effects on enzyme activity in crops.Here,we review the role of endophytic bacteria in the bioremediation of PAEs-contaminated crops and soils.In addition,we discuss the scarcity of endophytic bacterial strains with a confirmed ability to degrade PAEs,and underscore the lack of the research on the mechanisms of PAEs degradation by these bacteria.This review also points out that future study should investigate the molecular mechanisms underlying the interaction between endophytic bacteria and PAEs to offer novel insights and solutions for environmental protection and sustainable agricultural development.
基金This research was supported by Shanghai Pujiang Program(21PJD022)National Natural Science Foundation of China(21901154).
文摘The hydrogen evolution reaction performance of semiconducting 2H-phase molybdenum disulfide(2H-MoS_(2))presents a significant hurdle in realizing its full potential applications.Here,we utilize theoretical calculations to predict possible functionalized graphene quantum dots(GQDs),which can enhance HER activity of bulk MoS_(2).Subsequently,we design a functionalized GQD-induced in-situ bottom-up strategy to fabricate near atom-layer 2H-MoS_(2) nanosheets mediated with GQDs(ALQD)by modulating the concentration of electron withdrawing/donating functional groups.Experimental results reveal that the introduction of a series of functionalized GQDs during the synthesis of ALQD plays a crucial role.Notably,the higher the concentration and strength of electron-withdrawing functional groups on GQDs,the thinner and more active the resulting ALQD are.Remarkably,the synthesized near atom-layer ALQD-SO_(3)demonstrate significantly improved HER performance.Our GQD-induced strategy provides a simple and efficient approach for expanding the catalytic application of MoS_(2).Furthermore,it holds substantial potential for developing nanosheets in other transition-metal dichalcogenide materials.
基金project was funded by National Natural Science Foundation of China(Nos.21901154,21671129)the Program for Changjiang Scholars and Innovative Research Team in University(No.IRT17R71)。
文摘High-efficiency electrochemical hydrogen evolution reaction(HER)offers a promising strategy to address energy and environmental crisis.Platinum is the most effective electrocatalyst for the HER.However,challenging scarcity,valuableness,and poor electrochemical stability still hinder its wide application.Here,we designed an outstanding HER electrocatalyst,highly dispersed rhodium(Rh)nanoparticles with an average diameter of only 3 nm supported on boron(B)nanosheets.The HER catalytic activity is even comparable to that of commercial platinum catalysts,with an overpotential of only 66 mV in 0.5 M H_(2)SO_(4) and 101 mV in 1 M KOH to reach the current density of 10 mA cm−2.Meanwhile,the catalyst exhibited impressive electrochemical durability during long-term electrochemical processes in acidic and alkaline media,even the simu-lated seawater environment.Theoretical calculations unraveled that the structure-activity relationship between B(104)crystal plane and Rh(111)crystal plane is beneficial to the release of hydrogen,and surface O plays a vital role in the catalysis process.Our work may gain insights into the development of supported metal catalysts with robust catalytic performance through precise engineering of the strong metal-supported interaction effect.
基金supported by the National Key Research and Development Program of China(No.2018YFC1407501)the Key Laboratory Open Fund of Fishery Ecology Environment,Ministry of Agriculture,China.
文摘Perfluorinated or polyfluorinated compounds(PFCs)continue entering to the environmental as individuals or mixtures,but their toxicological information remains largely unknown.Here,we investigated the toxic effects and ecological risks of Perfluorooctane sulfonic acid(PFOS)and its substitutes on prokaryotes(Chlorella vulgaris)and eukaryotes(Microcystis aeruginosa).Based on the calculated EC50 values,the results showed that PFOS was significantly more toxic to both algae than its alternatives including Perfluorobutane sulfonic acid(PFBS)and 6:2 Fluoromodulated sulfonates(6:2 FTS),and the PFOS-PFBS mixture was more toxic to both algae than the other two PFC mixtures.The action mode of binary PFC mixtures on Chlorella vulgaris was mainly shown as antagonistic and on Microcystis aeruginosa as synergistic,by using Combination index(CI)model coupled with Monte Carlo simulation.The mean risk quotient(RQ)value of three individual PFCs and their mixtures were all below the threshold of 10^(−1),but the risk of those binary mixtures were higher than that of PFCs individually because of their synergistic effect.Our findings contribute to enhance the understanding of the toxicological information and ecological risks of emerging PFCs and provide a scientific basis for their pollution control.
基金supported by the“National Natural Science Foundation of China (Nos.51902162,21901154)”the FoundationResearch Project of Jiangsu Province (BK20221338)+1 种基金Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources,International Innovation Center for Forest Chemicals and Materials,Nanjing Forestry University,merit-based funding for Nanjing innovation and technology projects,Shanghai Pujiang Program (21PJD022)the Foundation of Jiangsu Key Lab of Biomass Energy and Material (JSBEM-S-202101).
文摘Compared with the traditional heteroatom doping,employing heterostructure is a new modulating approach for carbon-based electrocatalysts.Herein,a facile ball milling-assisted route is proposed to synthesize porous carbon materials composed of abundant graphene/hexagonal boron nitride(G/h-BN)heterostructures.Metal Ni powder and nanoscale h-BN sheets are used as a catalytic substrate/hard template and“nucleation seed”for the formation of the heterostructure,respectively.As-prepared G/h-BN heterostructures exhibit enhanced electrocatalytic activity toward H_(2)O_(2) generation with 86%-95%selectivity at the range of 0.45-0.75 V versus reversible hydrogen electrode(RHE)and a positive onset potential of 0.79 versus RHE(defined at a ring current density of 0.3 mA cm^(-2))in the alkaline solution.In a flow cell,G/h-BN heterostructured electrocatalyst has a H_(2)O_(2) production rate of up to 762 mmol g_(catalyst)^(-1) h^(-1) and Faradaic efficiency of over 75%during 12 h testing,superior to the reported carbon-based electrocatalysts.The density functional theory simulation suggests that the B atoms at the interface of the G/h-BN heterostructure are the key active sites.This research provides a new route to activate carbon catalysts toward highly active and selective O_(2)-to-H_(2)O_(2) conversion.
基金supported by the Foundation of Jiangsu Key Lab of Biomass Energy and Material(No.JSBEM-S-202101)National Natural Science Foundation of China(No.51902162)+1 种基金the Foundation Research Project of Jiangsu Province(No.BK20221338)Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources,International Innovation Center for Forest Chemicals and Materials,Nanjing Forestry University,merit-based funding for Nanjing innovation and technology projects.
文摘Electrochemical reduction of CO_(2)(CO_(2)RR)to value-added chemicals is an attractive strategy for greenhouse gas mitigation and carbon recycle.Carbon material is one of most promising electrocatalysts but its product selectivity is limited by few modulating approaches for active sites.Herein,the predominant pyridinic N-B sites(accounting for 80%to all N species)are fabricated in hierarchically porous structure of graphene nanoribbons/amorphous carbon.The graphene nanoribbons and porous structure can accelerate electron and ion/gas transport during CO_(2)RR,respectively.This carbon electrocatalyst exhibits excellent selectivity toward CO_(2)reduction to CH_(4)with the faradaic efficiency of 68%at−0.50 V vs.RHE.As demonstrated by density functional theory,a proper adsorbed energy of∗CO and∗CH_(2)O are generated on the pyridinic N-B site resulting into high CH_(4)selectivity.Therefore,this study provides a novel method to modulate active sites of carbon-based electrocatalyst to obtain high CH_(4)selectivity.
