Oxygen evolution reaction(OER)is widely recognized as a bottleneck of water electrolysis.To determine the underlying reaction mechanisms,particularly the relative contribution of the adsorbate evolution mechanism(AEM)...Oxygen evolution reaction(OER)is widely recognized as a bottleneck of water electrolysis.To determine the underlying reaction mechanisms,particularly the relative contribution of the adsorbate evolution mechanism(AEM)and lattice-oxygen participation mechanism(LOM),we conduct a comprehensive investigation combining Density Functional Theory(DFT)calculations and experimental validation.Our theoretical analysis of doped RuO_(2)catalysts reveals that heteroatom doping(Ni,Cu,and Zn)induces significant local charge transfer,leading to the increased charge state of Ru and the downshifted d-band center.This,in turn,enables the mechanism switching from the conventional AEM to the more efficient LOM,and finally improves OER activity.We also establish a simple yet powerful descriptor,Ne of Ru(representing charge density of Ru sites),which enables accurate prediction of both catalytic activity and stability.Guided by these theoretical predictions,we successfully synthesize a Ni-doped RuO_(2)catalyst,which exhibits excellent OER activity and stability in acidic media,achieving an overpotential of just 156 mV and maintaining stability for 4000 h at 10 mA cm^(−2),significantly surpassing the performance of the commercial RuO_(2).These findings not only provide fundamental insights into the mechanism-switching behavior in OER catalysis but also offer a practical strategy for designing high-performance,stable electrocatalysts for acidic water electrolysis.展开更多
Derivatives of metal-organic frameworks(MOFs)are a promising bifunctional electrocatalysts in electrochemical advanced oxidation processes(EAOPs).These metal/carbon materials overcome the limitations of individual com...Derivatives of metal-organic frameworks(MOFs)are a promising bifunctional electrocatalysts in electrochemical advanced oxidation processes(EAOPs).These metal/carbon materials overcome the limitations of individual components by creating synergistic effects.EAOPs is primarily constrained by the generation and activation of H_(2)O_(2).This article examines the regulatory strategies employed in MOFs derivatives to enhance the production of H_(2)O_(2)via 2e^(-)pathways and its activation to·OH,focusing on preparation techniques,structures,and compositions.The design of these derivatives involves methods such as metal dispersion on the surface of nanocarbons,embedding in carbon shells,and atomic dispersion of metals anchored in porous carbon.MOFs derivatives promote·OH production and enhance wastewater purification through mechanisms such as boosting the Fe(Ⅱ)/Fe(Ⅲ)cycle,facilitating direct 3e^(-)reactions of O_(2),and interacting of O_(2)^(·-).Moreover,the performance and durability of MOFs derivatives in wastewater treatment,particularly in influencing·OH generation within EAOPs,were investigated.This review addresses current challenges and future prospects,offering valuable insights for the development of MOFs derivatives as 3e^(-)ORR electrocatalysts and the advancement of sustainable water treatment technologies.展开更多
OER Commons项目是由美国教育领域的知识管理研究协会(ISKME)创建的共享开放教育资源的知识库与联接门户,旨在支持开放教育资源应用和重用。文章介绍了OER Commons项目的发展及其特色,并分析了该项目的开放机制,提出了对我国开放教育资...OER Commons项目是由美国教育领域的知识管理研究协会(ISKME)创建的共享开放教育资源的知识库与联接门户,旨在支持开放教育资源应用和重用。文章介绍了OER Commons项目的发展及其特色,并分析了该项目的开放机制,提出了对我国开放教育资源建设的启示。展开更多
基金supported by the National Natural Science Foundation of China(22472104)Guangdong Basic and Applied Basic Research Foundation(2024A1515012075,2024A1515010028)the Postdoctoral Fellowship Program of CPS Funder(GZC20241083,2025M771117)。
文摘Oxygen evolution reaction(OER)is widely recognized as a bottleneck of water electrolysis.To determine the underlying reaction mechanisms,particularly the relative contribution of the adsorbate evolution mechanism(AEM)and lattice-oxygen participation mechanism(LOM),we conduct a comprehensive investigation combining Density Functional Theory(DFT)calculations and experimental validation.Our theoretical analysis of doped RuO_(2)catalysts reveals that heteroatom doping(Ni,Cu,and Zn)induces significant local charge transfer,leading to the increased charge state of Ru and the downshifted d-band center.This,in turn,enables the mechanism switching from the conventional AEM to the more efficient LOM,and finally improves OER activity.We also establish a simple yet powerful descriptor,Ne of Ru(representing charge density of Ru sites),which enables accurate prediction of both catalytic activity and stability.Guided by these theoretical predictions,we successfully synthesize a Ni-doped RuO_(2)catalyst,which exhibits excellent OER activity and stability in acidic media,achieving an overpotential of just 156 mV and maintaining stability for 4000 h at 10 mA cm^(−2),significantly surpassing the performance of the commercial RuO_(2).These findings not only provide fundamental insights into the mechanism-switching behavior in OER catalysis but also offer a practical strategy for designing high-performance,stable electrocatalysts for acidic water electrolysis.
基金financially supported by National Natural Science Foundation of China(No.22302170)Science Research Project of Hebei Education Department(No.QN2024256)。
文摘Derivatives of metal-organic frameworks(MOFs)are a promising bifunctional electrocatalysts in electrochemical advanced oxidation processes(EAOPs).These metal/carbon materials overcome the limitations of individual components by creating synergistic effects.EAOPs is primarily constrained by the generation and activation of H_(2)O_(2).This article examines the regulatory strategies employed in MOFs derivatives to enhance the production of H_(2)O_(2)via 2e^(-)pathways and its activation to·OH,focusing on preparation techniques,structures,and compositions.The design of these derivatives involves methods such as metal dispersion on the surface of nanocarbons,embedding in carbon shells,and atomic dispersion of metals anchored in porous carbon.MOFs derivatives promote·OH production and enhance wastewater purification through mechanisms such as boosting the Fe(Ⅱ)/Fe(Ⅲ)cycle,facilitating direct 3e^(-)reactions of O_(2),and interacting of O_(2)^(·-).Moreover,the performance and durability of MOFs derivatives in wastewater treatment,particularly in influencing·OH generation within EAOPs,were investigated.This review addresses current challenges and future prospects,offering valuable insights for the development of MOFs derivatives as 3e^(-)ORR electrocatalysts and the advancement of sustainable water treatment technologies.
