The keen interest in fuel cells and metal-air batteries stimulates a great deal of research on the development of a cost-efficient and high-performance catalyst as an alternative to traditional Pt to boost the sluggis...The keen interest in fuel cells and metal-air batteries stimulates a great deal of research on the development of a cost-efficient and high-performance catalyst as an alternative to traditional Pt to boost the sluggish oxygen reduction reaction(ORR)at the cathode.Herein,we report a facile and scalable strategy for the large-scale preparation of a free-standing and flexible porous atomically dispersed Fe-N-doped carbon microtube(FeSAC/PCMT)sponge.Benefiting from its unique structure that greatly facilitates the catalytic kinetics,mass transport,and electron transfer,our FeSAC/PCMT electrode exhibits excellent performance with an ORR potential of 0.942 V at^(-3) mA cm^(-2).When the FeSAC/PCMT sponge was directly used as an oxygen electrode for liquid-state and flexible solid-state zinc-air batteries,high peak power densities of 183.1 and 58.0 mW cm^(-2) were respectively achieved,better than its powdery counterpart and commercial Pt/C catalyst.Experimental and theoretical investigation results demonstrate that such ultrahigh ORR performance can be attributed to atomically dispersed Fe-N_(5) species in FeSAC/PCMT.This study presents a cost-effective and scalable strategy for the fabrication of highly efficient and flexible oxygen electrodes,provides a significant new insight into the catalytic mechanisms,and helps to realize significant advances in energy devices.展开更多
The North China Plain is one of the main grain producing areas in China. However, overexploitation has long been unsustainable since the water supply is mainly from groundwater. Since 2014,the South-to-North Water Div...The North China Plain is one of the main grain producing areas in China. However, overexploitation has long been unsustainable since the water supply is mainly from groundwater. Since 2014,the South-to-North Water Diversion Project's central route has been charted to the integrated management of water supply and over-exploitation, which has alleviated the problem to a certain extent. Although the Ministry of Water Resources has made many efforts on groundwater recharge since 2018 most of which have been successful, the recharge has not yet been sufficiently focused on the repair of shallow groundwater depression zones. It still needs further optimization. This paper discusses this particular issue,proposes optimized recharge plan and provides the following recommendations:(1) Seven priority target areas are selected for groundwater recharge in alluvial and proluvial fans in the piedmont plain, and the storage capacity is estimated to be 181.00×10~8 m~3;(2) A recharge of 31.18×10~8 m~3/a is required by 2035 to achieve the repair target;(3) It is proposed to increase the recharge of Hutuo River, Dasha River and Tanghe River to 19.00×10~8 m~3/a and to rehabilitate Gaoliqing-Ningbailong Depression Zone;increase the recharge of Fuyang River, Zhanghe River and Anyang River to 7.05×10~8 m~3/a and rehabilitate Handan Feixiang-Guangping Depression Zone;increase the recharge of Luanhe River by 0.56×10~8 m~3/a and restore Tanghai Depression Zone and Luanan-Leting Depression Zone;moderately reduce the amount of water recharged to North Canal and Yongding River to prevent excessive rebound of groundwater;(4) Recharge through well is implemented on a pilot basis in areas of severe urban ground subsidence and coastal saltwater intrusion;(5) An early warning mechanism for groundwater quality risks in recharge areas is established to ensure the safety. The numerical groundwater flow model also proves reasonable groundwater level restoration in the depression zones by 2035.展开更多
Single-atom catalyst(SAC)is one of the newest catalysts,and attracts people’s wide attention in cancer therapy based on their characteristics of maximum specific catalytic activity and high stability.We designed and ...Single-atom catalyst(SAC)is one of the newest catalysts,and attracts people’s wide attention in cancer therapy based on their characteristics of maximum specific catalytic activity and high stability.We designed and synthesized a Fe-N decorated graphene nanosheet(Fe-N5/GN SAC)with the coordination number of five.Through enzymology and theoretical calculations,the Fe-N5/GN SAC has outstanding intrinsic peroxidase-like catalytic activity due to single-atom Fe site with five-N-coordination structure.We explored its potential on lung cancer therapy,and found that it could kill human lung adenocarcinoma cells(A549)by decomposing hydrogen peroxide(H_(2)O_(2))into toxic reactive oxygen species(ROS)under acidic microenvironment in threedimensional(3D)lung cancer cell model.Our study demonstrates a promising application of SAC with highly efficient single-atom catalytic sites for cancer treatment.展开更多
Although zinc-air batteries(ZABs)are regarded as one of the most prospective energy storage devices,their practical application has been restricted by poor air electrode performance.Herein,we developed a free-standing...Although zinc-air batteries(ZABs)are regarded as one of the most prospective energy storage devices,their practical application has been restricted by poor air electrode performance.Herein,we developed a free-standing air electrode that is fabricated on the basis of a multifunctional three-dimensional interconnected graphene network.Specifically,a three-dimensional interconnected graphene network with fast mass and electron transport ability,prepared by catalyzing growth of graphene foam on nickel foam and then filling reduced graphene oxide into the pores of graphene foam,is used to anchor iron phthalocyanine molecules with atomic Fe-N_(4)sites for boosting the oxygen reduction during discharging and nanosized FeNi hydroxides for accelerating the oxygen evolution during charging.As a result,the obtained air electrode exhibited an ultra-small electrocatalytic overpotential of 0.603 V for oxygen reactions,a high peak power density of 220.2mWcm^(-2),and a small and stable charge-discharge voltage gap of 0.70 V at 10mA cm^(-2)after 1136 cycles.Furthermore,in situ Raman spectroscopy together with theoretical calculations confirmed that phase transformation of FeNi hydroxides takes place fromα-Ni(OH)_(x)toβ-Ni(OH)_(x)toγ-Ni^((3+δ)+)OOH for the oxygen evolution reaction and Ni is the active center while Fe enhances the activity of Ni active sites.展开更多
Non-precious metal single-atom catalysts(NPM-SACs)with unique electronic structures and coordination environments have gained much attention in electrocatalysis owing to their low cost,high atomic utilization,and high...Non-precious metal single-atom catalysts(NPM-SACs)with unique electronic structures and coordination environments have gained much attention in electrocatalysis owing to their low cost,high atomic utilization,and high performance.NPM-SACs on carbon support(NPM-SACs/CS)are promising because of the carbon substrate with a large surface area,excellent electrical conductivity,and high chemical stability.This review provides an overview of recent developments in NPM-SACs/CS for the electrocatalytic field.First,the state-of-the-art synthesis methods and advanced characterization techniques of NPM-SACs/CS are discussed in detail.Then,the structural adjustment strategy of NPM-SACs/CS for optimizing electrocatalytic performance is introduced concisely.Furthermore,we provide a comprehensive summary of recent advances in developing NPM-SACs/CS for important electrochemical reactions,including carbon dioxide reduction reaction,hydrogen evolution reaction,oxygen evolution reaction,oxygen reduction reaction,and nitrogen reduction reaction.In the end,the existing challenges and future opportunities of NPM-SACs/CS in the electrocatalytic field are highlighted.展开更多
The enzyme-mimicking catalytic activity of single-atom nanozymes has been widely used in tumor treatment.However,research on alleviating metabolic diseases,such as hyperglycemia,has not been reported.Herein,we found t...The enzyme-mimicking catalytic activity of single-atom nanozymes has been widely used in tumor treatment.However,research on alleviating metabolic diseases,such as hyperglycemia,has not been reported.Herein,we found that the single-atom Ce-N_(4)-C-(OH)_(2)(SACe-N_(4)-C-(OH)_(2))nanozyme promoted glucose absorption in lysosomes,resulting in increased reactive oxygen species production in HepG2 cells.Furthermore,the SACe-N_(4)-C-(OH)_(2)nanozyme initiated a cascade reaction involving superoxide dismutase-,oxidase-,catalase-,and peroxidase-like activity to overcome the limitations associated with the substrate and produce•OH,thus improving glucose intolerance and insulin resistance by increasing the phosphorylation of protein kinase B and glycogen synthase kinase 3β,and the expression of glycogen synthase,promoting glycogen synthesis to improve glucose intolerance and insulin resistance in high-fat diet-induced hyperglycemic mice.Altogether,these results demonstrated that the novel nanozyme SACeN_(4)-C-(OH)_(2)alleviated the effects of hyperglycemia without evident toxicity,demonstrating its excellent clinical application potential.展开更多
The Fe–N–C material is a promising non-noblemetal electrocatalyst for oxygen reduction reaction(ORR).Further improvement on the ORR activity is highly desired in order to replace Pt/C in acidic media.Herein,we devel...The Fe–N–C material is a promising non-noblemetal electrocatalyst for oxygen reduction reaction(ORR).Further improvement on the ORR activity is highly desired in order to replace Pt/C in acidic media.Herein,we developed a new-type of single-atom Fe–N–C electrocatalyst,in which Fe–Nxactive sites were modified by P atoms.The half-wave potential of the optimized material reached 0.858 V,which is 23 mV higher than that of the pristine one in a 0.1 mol L-1 HClO4 solution.Density functional theory(DFT)calculations revealed that P-doping can reduce the thermodynamic overpotential of the rate determining step and consequently improve the ORR activity.展开更多
With the improvement of people’s requirements for food quality,food safety has become the focus of society.More and more researchers continue to develop specific and convenient biochemical sensors for the detection o...With the improvement of people’s requirements for food quality,food safety has become the focus of society.More and more researchers continue to develop specific and convenient biochemical sensors for the detection of certain components in food,which also imposes higher requirements for the structure and performance of nanomaterials.Biochemical sensors based on carbon nanotubes,metal nanowires,nanofibers,metal-organic framework(MOF)compounds and other functional composite materials have the advantages of high sensitivity,great detection speed and reliable results,and have been continuously developed and widely used in medical,environmental and food safety fields.This paper reviews the progress of research on the application of the sensors based on the above functional nanomaterials in food detection in recent years,demonstrates the advantages brought by the functional composite materials,and discusses the challenges faced by the functional nanomaterials in the field of food safety testing,to provide an effective reference for developing functional composite material sensors for food safety testing.展开更多
基金supported by the start-up fund from Kunming University of Science and Technology,the National Natural Science Foundation of China (Grants 52102046,51872293,52130209,52072375)Liaoning Revitalization Talents Program (XLYC2002037)Basic Research Project of Natural Science Foundation of Shandong Province,China (ZR2019ZD49).
文摘The keen interest in fuel cells and metal-air batteries stimulates a great deal of research on the development of a cost-efficient and high-performance catalyst as an alternative to traditional Pt to boost the sluggish oxygen reduction reaction(ORR)at the cathode.Herein,we report a facile and scalable strategy for the large-scale preparation of a free-standing and flexible porous atomically dispersed Fe-N-doped carbon microtube(FeSAC/PCMT)sponge.Benefiting from its unique structure that greatly facilitates the catalytic kinetics,mass transport,and electron transfer,our FeSAC/PCMT electrode exhibits excellent performance with an ORR potential of 0.942 V at^(-3) mA cm^(-2).When the FeSAC/PCMT sponge was directly used as an oxygen electrode for liquid-state and flexible solid-state zinc-air batteries,high peak power densities of 183.1 and 58.0 mW cm^(-2) were respectively achieved,better than its powdery counterpart and commercial Pt/C catalyst.Experimental and theoretical investigation results demonstrate that such ultrahigh ORR performance can be attributed to atomically dispersed Fe-N_(5) species in FeSAC/PCMT.This study presents a cost-effective and scalable strategy for the fabrication of highly efficient and flexible oxygen electrodes,provides a significant new insight into the catalytic mechanisms,and helps to realize significant advances in energy devices.
基金funded by Geological Joint Fund of the National Natural Science Foundation of China (U2244214)China Geological Survey Program (DD20190336, DD20221752, DD20230078)+1 种基金Chinese Academy of Geological Sciences Basic Research Fund Program (SK202118, SK202216)Hebei Provincial Innovation Capacity Enhancement Program for High-level Talent Team Building (225A4204D)。
文摘The North China Plain is one of the main grain producing areas in China. However, overexploitation has long been unsustainable since the water supply is mainly from groundwater. Since 2014,the South-to-North Water Diversion Project's central route has been charted to the integrated management of water supply and over-exploitation, which has alleviated the problem to a certain extent. Although the Ministry of Water Resources has made many efforts on groundwater recharge since 2018 most of which have been successful, the recharge has not yet been sufficiently focused on the repair of shallow groundwater depression zones. It still needs further optimization. This paper discusses this particular issue,proposes optimized recharge plan and provides the following recommendations:(1) Seven priority target areas are selected for groundwater recharge in alluvial and proluvial fans in the piedmont plain, and the storage capacity is estimated to be 181.00×10~8 m~3;(2) A recharge of 31.18×10~8 m~3/a is required by 2035 to achieve the repair target;(3) It is proposed to increase the recharge of Hutuo River, Dasha River and Tanghe River to 19.00×10~8 m~3/a and to rehabilitate Gaoliqing-Ningbailong Depression Zone;increase the recharge of Fuyang River, Zhanghe River and Anyang River to 7.05×10~8 m~3/a and rehabilitate Handan Feixiang-Guangping Depression Zone;increase the recharge of Luanhe River by 0.56×10~8 m~3/a and restore Tanghai Depression Zone and Luanan-Leting Depression Zone;moderately reduce the amount of water recharged to North Canal and Yongding River to prevent excessive rebound of groundwater;(4) Recharge through well is implemented on a pilot basis in areas of severe urban ground subsidence and coastal saltwater intrusion;(5) An early warning mechanism for groundwater quality risks in recharge areas is established to ensure the safety. The numerical groundwater flow model also proves reasonable groundwater level restoration in the depression zones by 2035.
基金N.C.would like to acknowledge the support the 2115 Talent Development Program of China Agricultural UniversityThis research used resources of the Advanced Photon Source,a U.S.Department of Energy(DOE)Office of Science User Facility,operated for the DOE Office of Science by Argonne National Laboratory under Contract No.DE-AC02-06CH11357.
文摘Single-atom catalyst(SAC)is one of the newest catalysts,and attracts people’s wide attention in cancer therapy based on their characteristics of maximum specific catalytic activity and high stability.We designed and synthesized a Fe-N decorated graphene nanosheet(Fe-N5/GN SAC)with the coordination number of five.Through enzymology and theoretical calculations,the Fe-N5/GN SAC has outstanding intrinsic peroxidase-like catalytic activity due to single-atom Fe site with five-N-coordination structure.We explored its potential on lung cancer therapy,and found that it could kill human lung adenocarcinoma cells(A549)by decomposing hydrogen peroxide(H_(2)O_(2))into toxic reactive oxygen species(ROS)under acidic microenvironment in threedimensional(3D)lung cancer cell model.Our study demonstrates a promising application of SAC with highly efficient single-atom catalytic sites for cancer treatment.
基金supported by the National Natural Science Foundation of China(52102046)the Yunnan Fundamental Research Projects(202301AW070016).
文摘Although zinc-air batteries(ZABs)are regarded as one of the most prospective energy storage devices,their practical application has been restricted by poor air electrode performance.Herein,we developed a free-standing air electrode that is fabricated on the basis of a multifunctional three-dimensional interconnected graphene network.Specifically,a three-dimensional interconnected graphene network with fast mass and electron transport ability,prepared by catalyzing growth of graphene foam on nickel foam and then filling reduced graphene oxide into the pores of graphene foam,is used to anchor iron phthalocyanine molecules with atomic Fe-N_(4)sites for boosting the oxygen reduction during discharging and nanosized FeNi hydroxides for accelerating the oxygen evolution during charging.As a result,the obtained air electrode exhibited an ultra-small electrocatalytic overpotential of 0.603 V for oxygen reactions,a high peak power density of 220.2mWcm^(-2),and a small and stable charge-discharge voltage gap of 0.70 V at 10mA cm^(-2)after 1136 cycles.Furthermore,in situ Raman spectroscopy together with theoretical calculations confirmed that phase transformation of FeNi hydroxides takes place fromα-Ni(OH)_(x)toβ-Ni(OH)_(x)toγ-Ni^((3+δ)+)OOH for the oxygen evolution reaction and Ni is the active center while Fe enhances the activity of Ni active sites.
基金support from the China Postdoctoral Science Foundation(2022M711553).Y.W.would like to acknowledge the support from the National Natural Science Foundation of China(22171132)the Innovation Fund from Nanjing University(020514913419)+5 种基金the Program for Innovative Talents and Entrepreneurs in Jiangsu(020513006012 and 020513006014),and the National Key R&D Program of China(2002YFB3607000).W.Z.would like to acknowledge the support from the National Natural Science Foundation of China(22176086)Natural Science Foundation of Jiangsu Province(BK20210189)State Key Laboratory of Pollution Control and Resource Reuse(PCRR-ZZ-202106)the Fundamental Research Funds for the Central Universities(021114380183,021114380189 and 021114380199)the Research Funds from the Nanjing Science and Technology Innovation Project for Chinese Scholars Studying Abroad(13006003)the Research Funds from Frontiers Science Center for Critical Earth Material Cycling of Nanjing University,and Research Funds for Jiangsu Distinguished Professor.Y.L.would like to thank the support from the Washington State University startup fund.
文摘Non-precious metal single-atom catalysts(NPM-SACs)with unique electronic structures and coordination environments have gained much attention in electrocatalysis owing to their low cost,high atomic utilization,and high performance.NPM-SACs on carbon support(NPM-SACs/CS)are promising because of the carbon substrate with a large surface area,excellent electrical conductivity,and high chemical stability.This review provides an overview of recent developments in NPM-SACs/CS for the electrocatalytic field.First,the state-of-the-art synthesis methods and advanced characterization techniques of NPM-SACs/CS are discussed in detail.Then,the structural adjustment strategy of NPM-SACs/CS for optimizing electrocatalytic performance is introduced concisely.Furthermore,we provide a comprehensive summary of recent advances in developing NPM-SACs/CS for important electrochemical reactions,including carbon dioxide reduction reaction,hydrogen evolution reaction,oxygen evolution reaction,oxygen reduction reaction,and nitrogen reduction reaction.In the end,the existing challenges and future opportunities of NPM-SACs/CS in the electrocatalytic field are highlighted.
基金This work was supported by the Natural Science Foundation of China(Grant No.32001787)the 2115 Talent Development Program of China Agricultural University。
文摘The enzyme-mimicking catalytic activity of single-atom nanozymes has been widely used in tumor treatment.However,research on alleviating metabolic diseases,such as hyperglycemia,has not been reported.Herein,we found that the single-atom Ce-N_(4)-C-(OH)_(2)(SACe-N_(4)-C-(OH)_(2))nanozyme promoted glucose absorption in lysosomes,resulting in increased reactive oxygen species production in HepG2 cells.Furthermore,the SACe-N_(4)-C-(OH)_(2)nanozyme initiated a cascade reaction involving superoxide dismutase-,oxidase-,catalase-,and peroxidase-like activity to overcome the limitations associated with the substrate and produce•OH,thus improving glucose intolerance and insulin resistance by increasing the phosphorylation of protein kinase B and glycogen synthase kinase 3β,and the expression of glycogen synthase,promoting glycogen synthesis to improve glucose intolerance and insulin resistance in high-fat diet-induced hyperglycemic mice.Altogether,these results demonstrated that the novel nanozyme SACeN_(4)-C-(OH)_(2)alleviated the effects of hyperglycemia without evident toxicity,demonstrating its excellent clinical application potential.
基金This work was supported by the National Key R&D Program of China(2017YFB0102900)the Research Grant Council(N一HKUST610/17)of Hong Kong Special Administrative Region.It used resources of the Advanced Photon Source,Office of Science user facilities,supported by the U.S.Department of Energy,Office of Science,Office of Basic Energy Sciences(DE-AC02-06CH11357).
文摘The Fe–N–C material is a promising non-noblemetal electrocatalyst for oxygen reduction reaction(ORR).Further improvement on the ORR activity is highly desired in order to replace Pt/C in acidic media.Herein,we developed a new-type of single-atom Fe–N–C electrocatalyst,in which Fe–Nxactive sites were modified by P atoms.The half-wave potential of the optimized material reached 0.858 V,which is 23 mV higher than that of the pristine one in a 0.1 mol L-1 HClO4 solution.Density functional theory(DFT)calculations revealed that P-doping can reduce the thermodynamic overpotential of the rate determining step and consequently improve the ORR activity.
基金This work was supported by the National Natural Science Foundation of China(22176221)the Special Scientific Research Funds for Central Non-profit Institutes,CAFS(2022A004 and 2020TD75)the Open foundation,Key laboratory of forensic marks,ministry of public security of China(2021FMKFKT04).
文摘With the improvement of people’s requirements for food quality,food safety has become the focus of society.More and more researchers continue to develop specific and convenient biochemical sensors for the detection of certain components in food,which also imposes higher requirements for the structure and performance of nanomaterials.Biochemical sensors based on carbon nanotubes,metal nanowires,nanofibers,metal-organic framework(MOF)compounds and other functional composite materials have the advantages of high sensitivity,great detection speed and reliable results,and have been continuously developed and widely used in medical,environmental and food safety fields.This paper reviews the progress of research on the application of the sensors based on the above functional nanomaterials in food detection in recent years,demonstrates the advantages brought by the functional composite materials,and discusses the challenges faced by the functional nanomaterials in the field of food safety testing,to provide an effective reference for developing functional composite material sensors for food safety testing.