In the quest for effective solutions to address Environ.Pollut.and meet the escalating energy demands,heterojunction photocatalysts have emerged as a captivating and versatile technology.These photocatalysts have garn...In the quest for effective solutions to address Environ.Pollut.and meet the escalating energy demands,heterojunction photocatalysts have emerged as a captivating and versatile technology.These photocatalysts have garnered significant interest due to their wideranging applications,including wastewater treatment,air purification,CO_(2) capture,and hydrogen generation via water splitting.This technique harnesses the power of semiconductors,which are activated under light illumination,providing the necessary energy for catalytic reactions.With visible light constituting a substantial portion(46%)of the solar spectrum,the development of visible-light-driven semiconductors has become imperative.Heterojunction photocatalysts offer a promising strategy to overcome the limitations associated with activating semiconductors under visible light.In this comprehensive review,we present the recent advancements in the field of photocatalytic degradation of contaminants across diverse media,as well as the remarkable progress made in renewable energy production.Moreover,we delve into the crucial role played by various operating parameters in influencing the photocatalytic performance of heterojunction systems.Finally,we address emerging challenges and propose novel perspectives to provide valuable insights for future advancements in this dynamic research domain.By unraveling the potential of heterojunction photocatalysts,this reviewcontributes to the broader understanding of their applications and paves the way for exciting avenues of exploration and innovation.展开更多
Electrocatalytic chemical oxidation(ECO)is an energy-efficient anodic reaction alternative to the oxygen evolution reaction(OER).ECO lowers the reaction potential and yields higher-value fine chemicals at the anode.Th...Electrocatalytic chemical oxidation(ECO)is an energy-efficient anodic reaction alternative to the oxygen evolution reaction(OER).ECO lowers the reaction potential and yields higher-value fine chemicals at the anode.The catalyst material plays a crucial role in influencing and determining ECO performance.Enhancing catalyst performance encompasses aspects such as activity,stability,selectivity and cost.Nickelbased electrocatalysts have garnered significant attention for their exceptional performance and widespread use in ECO applications.By modifying nickel-based electrocatalysts,the formation of NiOOH active centers can be encouraged.Strategies such as adjusting size and morphology,doping,introducing defects and constructing heterojunctions are advantageous for enhancing performance.Given the rapid advancements in related research fields,it is imperative to comprehend the mechanisms of nickel-based electrocatalysts in ECO and develop innovative catalysts.This article provides an overview of the modification strategies of nickel-based electrocatalysts,as well as their applications and mechanisms in ECO.展开更多
Natural enzymes are highly efficient catalysts with strong substrate specificity,making them ideal for biomedical applications.However,they often face issues such as variability,high costs,challenging preparation proc...Natural enzymes are highly efficient catalysts with strong substrate specificity,making them ideal for biomedical applications.However,they often face issues such as variability,high costs,challenging preparation processes,and difficulties in large-scale production.This has led to significant efforts in developing effective nanoenzymes and exploring their application potential.In recent years,carbon dots(CDs)have gained attention due to their strong fluorescence,excellent biocompatibility,and low cytotoxicity.Cationic CDs,which possess a positively charged surface,have shown the ability to mimic natural enzyme applications.The positive charge on the surfaces of these nanomaterials significantly influences their fluorescence,biological activity,and interactions with other biomolecules.Therefore,understanding how surface charge affects the performance of CDs is crucial for enhancing their usability.Considerable progress has been made in the design,synthesis,and mechanistic research of enzyme-like cationic CDs,as well as their advanced applications.This article reviews the latest research on the design structure,catalytic mechanisms,biosensing capabilities,and biomedical applications of enzyme-like cationic CDs.First,we review the synthesis strategies for cationic CDs and how surface charge influences their physical and chemical properties.Next,we highlight various applications of these cationic CDs,demonstrating their use in areas such as detection,biomedical applications(including antibacterial agents,gene carriers,and therapeutic agents),catalysis,and more.Finally,we discuss the challenges and obstacles faced in the development of cationic CDs and look forward to exploring new applications in the future.展开更多
Electrocatalytic nitrate reduction reaction(NitRR)is an efficient route for simultaneous wastewater treatment and ammonia production,but the conversion of NO_(3)–to NH_(3) involves multiple electron and proton transf...Electrocatalytic nitrate reduction reaction(NitRR)is an efficient route for simultaneous wastewater treatment and ammonia production,but the conversion of NO_(3)–to NH_(3) involves multiple electron and proton transfer processes and diverse by-products.Therefore,developing ammonia catalysts with superior catalytic activity and selectivity is an urgent task.The distinctive electronic structure of Cu enhances the adsorption of nitrogen-containing intermediates,but the insufficient activation capability of Cu for interfacial water restricts the generation of reactive hydrogen and inhibits the hydrogenation process.In this work,a Ce-doped CuO catalyst(Ce_(10)/CuO)was synthesized by in situ oxidative etching and annealing.The redox of Ce^(3+)/Ce^(4+)enables the optimization of the electronic structure of the catalyst,and the presence of Ce^(3+)as a defect indicator introduces more oxygen vacancies.The results demonstrate that Ce10/CuO provides an impressive ammonia yield of 3.88±0.14 mmol·cm^(–2)·h^(–1) at 0.4 V vs.reversible hydrogen electrode(RHE)with an increase of 1.04 mmol·cm^(–2)·h^(–1) compared to that of pure CuO,and the Faradaic efficiencies(FE)reaches 93.2%±3.4%.In situ characterization confirms the doping of Ce facilitates the activation and dissociation of interfacial water,which promotes the production of active hydrogen and thus enhances the ammonia production efficiency.展开更多
It is highly desired for the development of efficient bifunctional electrocatalyst for both oxygen reduction reaction （ORR） and oxygen evolution reaction （OER） in renewable energy technologies. In this work, cobal...It is highly desired for the development of efficient bifunctional electrocatalyst for both oxygen reduction reaction （ORR） and oxygen evolution reaction （OER） in renewable energy technologies. In this work, cobalt, nitrogen-codoped carbon was prepared by a facile one-step method and demonstrated to exhibit good elec- trocatalytic performance for ORR and OER via a complete four-electron process. Besides, the catalyst prepared at 900 ℃ also displayed excellent stability for both ORR and OER. Furthermore, the origin of catalytic activity was also explored, which was attributed to the synergistic effects of metallic Co and quaternary N.展开更多
Photocatalytic reduction of carbon dioxide into valuable chemicals is a sustainable and promising technology that alleviates the greenhouse effect and energy crisis.In this study,the Mn_(3)O_(4)/FeNbO_(4) type Ⅱ hete...Photocatalytic reduction of carbon dioxide into valuable chemicals is a sustainable and promising technology that alleviates the greenhouse effect and energy crisis.In this study,the Mn_(3)O_(4)/FeNbO_(4) type Ⅱ heterojunction photocatalyst with a core-satellite structure was synthesized by the facile soft chemical method.The formation of a nano-heterojunction is supposed to effectively improve light capture,charge transfer,and interfacial charge separation in the photochemical reaction.Meanwhile,the heterojunction has a good ability to capture and activate CO_(2).Our results show that the prepared Mn_(3)O_(4)/FeNbO_(4) photocatalyst exhibit obvious enhanced catalytic properties in the photocatalytic CO_(2) reduction reaction,where the CH_(4) yielding rate is 1.96 and 9.81 times those of FeNbO_(4) and Mn_(3)O_(4),respectively.The transient photovoltage test(TPV)shows that the low frequency electrons are crucial to the effective transfer of photogenerated electrons and holes in the Mn_(3)O_(4)/FeNbO_(4) nano heterojunctions.Analysis of in situ Fourier transform infrared spectroscopy(FTIR)verifies the effective CO_(2) adsorption on the Mn_(3)O_(4)/FeNbO_(4) surface and the high selectivity of CH_(4) products.These properties of the Mn_(3)O_(4)/FeNbO_(4) photocatalyst infer its broad prospects in the fields of carbon fixation and energy conservation.展开更多
The electrochemical nitrate reduction reaction(NO_(3)RR)to ammonia under ambient conditions is a promising approach for addressing elevated nitrate levels in water bodies,but the progress of this reaction is impeded b...The electrochemical nitrate reduction reaction(NO_(3)RR)to ammonia under ambient conditions is a promising approach for addressing elevated nitrate levels in water bodies,but the progress of this reaction is impeded by the complex series of chemical reactions involving electron and proton transfer and competing hydrogen evolution reaction.Therefore,it becomes imperative to develop an electro-catalyst that exhibits exceptional efficiency and remarkable selectivity for ammonia synthesis while maintaining long-term stability.Herein the magnetic biochar(Fe-C)has been synthesized by a two-step mechanochemical route after a pyrolysis treatment(450,700,and 1000℃),which not only significantly decreases the particle size,but also exposes more oxygen-rich functional groups on the surface,promoting the adsorption of nitrate and water and accelerating electron transfer to convert it into ammonia.Results showed that the catalyst(Fe-C-700)has an impressive NH_(3)production rate of 3.5 mol·h^(−1)·gcat^(−1),high Faradaic efficiency of 88%,and current density of 0.37 A·cm^(−2)at 0.8 V vs.reversible hydrogen electrode(RHE).In-situ Fourier transform infrared spectroscopy(FTIR)is used to investigate the reaction intermediate and to monitor the reaction.The oxygen functionalities on the catalyst surface activate nitrate ions to form various intermediates(NO_(2),NO,NH_(2)OH,and NH_(2))and reduce the rate determining step energy barrier(*NO_(3)→*NO_(2)).This study presents a novel approach for the use of magnetic biochar as an electro-catalyst in NO_(3)RR and opens the road for solving environmental and energy challenges.展开更多
Electrochemical carbon dioxide reduction reaction(CO_(2)RR)can produce value-added hydrocarbons from renewable electricity,providing a sustainable and promising approach to meet dual-carbon targets and alleviate the e...Electrochemical carbon dioxide reduction reaction(CO_(2)RR)can produce value-added hydrocarbons from renewable electricity,providing a sustainable and promising approach to meet dual-carbon targets and alleviate the energy crisis.However,it is still challenging to improve the selectivity and stability of the products,especially the C^(2+) products.Here we propose to modulate the electronic structure of copper oxide(CuO)through lattice strain construction by zinc(Zn)doping to improve the selectivity of the catalyst to ethylene.Combined performance and in situ characterization analyses show that the compressive strain generated within the CuO lattice and the electronic structure modulation by Zn doping enhances the adsorption of the key intermediate*CO,thereby increasing the intrinsic activity of CO_(2)RR and inhibiting the hydrogen precipitation reaction.Among the best catalysts had significantly improved ethylene selectivity of 60.5%and partial current density of 500 mA·cm^(–2),and the highest C^(2+) Faraday efficiency of 71.47%.This paper provides a simple idea to study the modulation of CO_(2)RR properties by heteroatom doped and lattice strain.展开更多
基金supported by the National Natural Science Foundation of China (Nos.52072152 and 51802126)Jiangsu University Jinshan Professor Fund,Jiangsu Specially-Appointed Professor Fund,the Open Fund from Guangxi Key Laboratory of Electrochemical Energy Materials,Zhenjiang“Jinshan Talents”Project 2021,China PostDoctoral Science Foundation (No.2022M721372)+1 种基金the“Doctor of Entrepreneurship and Innovation”in Jiangsu Province (No.JSSCBS20221197)the Postgraduate Research&Practice Innovation Program of Jiangsu Province (No.KYCX22_3645).
文摘In the quest for effective solutions to address Environ.Pollut.and meet the escalating energy demands,heterojunction photocatalysts have emerged as a captivating and versatile technology.These photocatalysts have garnered significant interest due to their wideranging applications,including wastewater treatment,air purification,CO_(2) capture,and hydrogen generation via water splitting.This technique harnesses the power of semiconductors,which are activated under light illumination,providing the necessary energy for catalytic reactions.With visible light constituting a substantial portion(46%)of the solar spectrum,the development of visible-light-driven semiconductors has become imperative.Heterojunction photocatalysts offer a promising strategy to overcome the limitations associated with activating semiconductors under visible light.In this comprehensive review,we present the recent advancements in the field of photocatalytic degradation of contaminants across diverse media,as well as the remarkable progress made in renewable energy production.Moreover,we delve into the crucial role played by various operating parameters in influencing the photocatalytic performance of heterojunction systems.Finally,we address emerging challenges and propose novel perspectives to provide valuable insights for future advancements in this dynamic research domain.By unraveling the potential of heterojunction photocatalysts,this reviewcontributes to the broader understanding of their applications and paves the way for exciting avenues of exploration and innovation.
基金supported by the National Natural Science Foundation of China(Nos.52072152 and 51802126)the Jiangsu University Jinshan Professor Fund,the Jiangsu Specially-Appointed Professor Fund,Open Fund from Guangxi Key Laboratory of Electrochemical Energy Materials,Zhenjiang“Jinshan Talents”Project 2021,China PostDoctoral Science Foundation(No.2022M721372)+2 种基金“Doctor of Entrepreneurship and Innovation”in Jiangsu Province(No.JSSCBS20221197)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(Nos.KYCX22_3645 and KYCX24_3964)Student Research Project of Jiangsu University(No.23A586).
文摘Electrocatalytic chemical oxidation(ECO)is an energy-efficient anodic reaction alternative to the oxygen evolution reaction(OER).ECO lowers the reaction potential and yields higher-value fine chemicals at the anode.The catalyst material plays a crucial role in influencing and determining ECO performance.Enhancing catalyst performance encompasses aspects such as activity,stability,selectivity and cost.Nickelbased electrocatalysts have garnered significant attention for their exceptional performance and widespread use in ECO applications.By modifying nickel-based electrocatalysts,the formation of NiOOH active centers can be encouraged.Strategies such as adjusting size and morphology,doping,introducing defects and constructing heterojunctions are advantageous for enhancing performance.Given the rapid advancements in related research fields,it is imperative to comprehend the mechanisms of nickel-based electrocatalysts in ECO and develop innovative catalysts.This article provides an overview of the modification strategies of nickel-based electrocatalysts,as well as their applications and mechanisms in ECO.
基金supported by the National Natural Science Foundation of China(Nos.52072152,and 51802126)the Jiangsu University Jinshan Professor Fund+4 种基金the Jiangsu Specially-Appointed Professor FundOpen Fund from Guangxi Key Laboratory of Electrochemical Energy Materials,Zhenjiang“Jinshan Talents”Project 2021China PostDoctoral Science Foundation(No.2022M721372)“Doctor of Entrepreneurship and Innovation”in Jiangsu Province(No.JSSCBS20221197)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(Nos.KYCX22_3645 and KYCX24_3964).
文摘Natural enzymes are highly efficient catalysts with strong substrate specificity,making them ideal for biomedical applications.However,they often face issues such as variability,high costs,challenging preparation processes,and difficulties in large-scale production.This has led to significant efforts in developing effective nanoenzymes and exploring their application potential.In recent years,carbon dots(CDs)have gained attention due to their strong fluorescence,excellent biocompatibility,and low cytotoxicity.Cationic CDs,which possess a positively charged surface,have shown the ability to mimic natural enzyme applications.The positive charge on the surfaces of these nanomaterials significantly influences their fluorescence,biological activity,and interactions with other biomolecules.Therefore,understanding how surface charge affects the performance of CDs is crucial for enhancing their usability.Considerable progress has been made in the design,synthesis,and mechanistic research of enzyme-like cationic CDs,as well as their advanced applications.This article reviews the latest research on the design structure,catalytic mechanisms,biosensing capabilities,and biomedical applications of enzyme-like cationic CDs.First,we review the synthesis strategies for cationic CDs and how surface charge influences their physical and chemical properties.Next,we highlight various applications of these cationic CDs,demonstrating their use in areas such as detection,biomedical applications(including antibacterial agents,gene carriers,and therapeutic agents),catalysis,and more.Finally,we discuss the challenges and obstacles faced in the development of cationic CDs and look forward to exploring new applications in the future.
基金This work was supported by the National Natural Science Foundation of China(Nos.52072152 and 51802126)the Jiangsu University Jinshan Professor Fund,the Jiangsu Specially-Appointed Professor Fund,Open Fund from Guangxi Key Laboratory of Electrochemical Energy Materials,Zhenjiang“Jinshan Talents”Project 2021,China Post Doctoral Science Foundation(No.2022M721372)+2 种基金“Doctor of Entrepreneurship and Innovation”in Jiangsu Province(No.JSSCBS20221197)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(Nos.KYCX22_3645 and KYCX24_3964)Student Research Project of Jiangsu University(Nos.23A586 and 23A804).
文摘Electrocatalytic nitrate reduction reaction(NitRR)is an efficient route for simultaneous wastewater treatment and ammonia production,but the conversion of NO_(3)–to NH_(3) involves multiple electron and proton transfer processes and diverse by-products.Therefore,developing ammonia catalysts with superior catalytic activity and selectivity is an urgent task.The distinctive electronic structure of Cu enhances the adsorption of nitrogen-containing intermediates,but the insufficient activation capability of Cu for interfacial water restricts the generation of reactive hydrogen and inhibits the hydrogenation process.In this work,a Ce-doped CuO catalyst(Ce_(10)/CuO)was synthesized by in situ oxidative etching and annealing.The redox of Ce^(3+)/Ce^(4+)enables the optimization of the electronic structure of the catalyst,and the presence of Ce^(3+)as a defect indicator introduces more oxygen vacancies.The results demonstrate that Ce10/CuO provides an impressive ammonia yield of 3.88±0.14 mmol·cm^(–2)·h^(–1) at 0.4 V vs.reversible hydrogen electrode(RHE)with an increase of 1.04 mmol·cm^(–2)·h^(–1) compared to that of pure CuO,and the Faradaic efficiencies(FE)reaches 93.2%±3.4%.In situ characterization confirms the doping of Ce facilitates the activation and dissociation of interfacial water,which promotes the production of active hydrogen and thus enhances the ammonia production efficiency.
基金supported by the National Basic Research Program of China (2012CB825803, 2013CB932702)the National Natural Science Foundation of China (51422207, 51132006,51572179, 21471106, and 21501126)+2 种基金the Specialized Research Fund for the Doctoral Program of Higher Education (20123201110018)a Suzhou Planning Project of Science and Technology (ZXG2012028)the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
文摘It is highly desired for the development of efficient bifunctional electrocatalyst for both oxygen reduction reaction （ORR） and oxygen evolution reaction （OER） in renewable energy technologies. In this work, cobalt, nitrogen-codoped carbon was prepared by a facile one-step method and demonstrated to exhibit good elec- trocatalytic performance for ORR and OER via a complete four-electron process. Besides, the catalyst prepared at 900 ℃ also displayed excellent stability for both ORR and OER. Furthermore, the origin of catalytic activity was also explored, which was attributed to the synergistic effects of metallic Co and quaternary N.
基金supported by the National Natural Science Foundation of China(Nos.52072152 and 51802126)the Jiangsu University Jinshan Professor Fund,the Jiangsu SpeciallyAppointed Professor Fund(No.17TPJS-003)Open Fund from Guangxi Key Laboratory of Electrochemical Energy Materials.
文摘Photocatalytic reduction of carbon dioxide into valuable chemicals is a sustainable and promising technology that alleviates the greenhouse effect and energy crisis.In this study,the Mn_(3)O_(4)/FeNbO_(4) type Ⅱ heterojunction photocatalyst with a core-satellite structure was synthesized by the facile soft chemical method.The formation of a nano-heterojunction is supposed to effectively improve light capture,charge transfer,and interfacial charge separation in the photochemical reaction.Meanwhile,the heterojunction has a good ability to capture and activate CO_(2).Our results show that the prepared Mn_(3)O_(4)/FeNbO_(4) photocatalyst exhibit obvious enhanced catalytic properties in the photocatalytic CO_(2) reduction reaction,where the CH_(4) yielding rate is 1.96 and 9.81 times those of FeNbO_(4) and Mn_(3)O_(4),respectively.The transient photovoltage test(TPV)shows that the low frequency electrons are crucial to the effective transfer of photogenerated electrons and holes in the Mn_(3)O_(4)/FeNbO_(4) nano heterojunctions.Analysis of in situ Fourier transform infrared spectroscopy(FTIR)verifies the effective CO_(2) adsorption on the Mn_(3)O_(4)/FeNbO_(4) surface and the high selectivity of CH_(4) products.These properties of the Mn_(3)O_(4)/FeNbO_(4) photocatalyst infer its broad prospects in the fields of carbon fixation and energy conservation.
基金the National Natural Science Foundation of China(Nos.52072152 and 51802126)the Jiangsu University Jinshan Professor Fund,the Jiangsu Specially-Appointed Professor Fund,Open Fund from Guangxi Key Laboratory of Electrochemical Energy Materials,Zhenjiang“Jinshan Talents”Project 2021,China PostDoctoral Science Foundation(No.2022M721372)+3 种基金“Doctor of Entrepreneurship and Innovation”in Jiangsu Province(No.JSSCBS20221197)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX22_3645)the National Natural Science Foundation of China(No.22208134)Jiangsu Agricultural Science and Technology Innovation Fund(No.CX(21)1010).
文摘The electrochemical nitrate reduction reaction(NO_(3)RR)to ammonia under ambient conditions is a promising approach for addressing elevated nitrate levels in water bodies,but the progress of this reaction is impeded by the complex series of chemical reactions involving electron and proton transfer and competing hydrogen evolution reaction.Therefore,it becomes imperative to develop an electro-catalyst that exhibits exceptional efficiency and remarkable selectivity for ammonia synthesis while maintaining long-term stability.Herein the magnetic biochar(Fe-C)has been synthesized by a two-step mechanochemical route after a pyrolysis treatment(450,700,and 1000℃),which not only significantly decreases the particle size,but also exposes more oxygen-rich functional groups on the surface,promoting the adsorption of nitrate and water and accelerating electron transfer to convert it into ammonia.Results showed that the catalyst(Fe-C-700)has an impressive NH_(3)production rate of 3.5 mol·h^(−1)·gcat^(−1),high Faradaic efficiency of 88%,and current density of 0.37 A·cm^(−2)at 0.8 V vs.reversible hydrogen electrode(RHE).In-situ Fourier transform infrared spectroscopy(FTIR)is used to investigate the reaction intermediate and to monitor the reaction.The oxygen functionalities on the catalyst surface activate nitrate ions to form various intermediates(NO_(2),NO,NH_(2)OH,and NH_(2))and reduce the rate determining step energy barrier(*NO_(3)→*NO_(2)).This study presents a novel approach for the use of magnetic biochar as an electro-catalyst in NO_(3)RR and opens the road for solving environmental and energy challenges.
基金financially supported by the National Key Research and Development Program of China(2019YFE0118100)the National Natural Science Foundation of China(U1902218)the Major Basic Research Projects of the Shandong Province Natural Science Foundation(ZR2021ZD25)。
基金supported by the National Natural Science Foundation of China(Nos.52072152 and 51802126)the Jiangsu University Jinshan Professor Fund,the Jiangsu Specially-Appointed Professor Fund,Open Fund from Guangxi Key Laboratory of Electrochemical Energy Materials,Zhenjiang“Jinshan Talents”Project 2021,China PostDoctoral Science Foundation(No.2022M721372)+2 种基金“Doctor of Entrepreneurship and Innovation”in Jiangsu Province(No.JSSCBS20221197)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX22_3645)Key Research and Development Program of Zhenjiang City(No.CG2023004).
文摘Electrochemical carbon dioxide reduction reaction(CO_(2)RR)can produce value-added hydrocarbons from renewable electricity,providing a sustainable and promising approach to meet dual-carbon targets and alleviate the energy crisis.However,it is still challenging to improve the selectivity and stability of the products,especially the C^(2+) products.Here we propose to modulate the electronic structure of copper oxide(CuO)through lattice strain construction by zinc(Zn)doping to improve the selectivity of the catalyst to ethylene.Combined performance and in situ characterization analyses show that the compressive strain generated within the CuO lattice and the electronic structure modulation by Zn doping enhances the adsorption of the key intermediate*CO,thereby increasing the intrinsic activity of CO_(2)RR and inhibiting the hydrogen precipitation reaction.Among the best catalysts had significantly improved ethylene selectivity of 60.5%and partial current density of 500 mA·cm^(–2),and the highest C^(2+) Faraday efficiency of 71.47%.This paper provides a simple idea to study the modulation of CO_(2)RR properties by heteroatom doped and lattice strain.
