Strain engineering of two-dimensional(2D)material interfaces represents a powerful strategy for enhanc-ing the electrocatalytic activity of water splitting.However,maintaining catalytic stability under various harsh c...Strain engineering of two-dimensional(2D)material interfaces represents a powerful strategy for enhanc-ing the electrocatalytic activity of water splitting.However,maintaining catalytic stability under various harsh conditions by introducing interface strain remains a great challenge.The catalyst developed and evaluated herein comprised Ir clusters dispersed on 2D NiO nanosheets(NSs)derived from metal organic frameworks(lr@NiO/C_(BDc)),which displays a high activity and stability under all pH conditions,and even a change of only 1%in the applied voltage is observed after continuous electrocatalytic operation for over 1800 h under alkaline conditions.Through combined experimental and computational studies,we found that the introduced interfacial strain contributes to the outstanding structural stability of the Ir@NiO/CBDC catalyst,arising from its increased Ir and Ni vacancy formation energies,and hence suppressing its leach-ing.Moreover,strain also enhances the kinetically sluggish electrocatalytic water splitting reaction by op-timizing its electronic structure and coordination environment.This work highlights the effects of strain on catalyst stability and provides new insights for designing widely applicable electrocatalysts.展开更多
As a half-reaction to obtain high-efficiency and stable water-splitting,oxygen evolution reaction(OER)is a slow-kinetics process involving a four-electron(4e^-)transfer process and therefore requires catalysts to fast...As a half-reaction to obtain high-efficiency and stable water-splitting,oxygen evolution reaction(OER)is a slow-kinetics process involving a four-electron(4e^-)transfer process and therefore requires catalysts to fasten electron transfer.Here,we rationally optimized an interface material of ceria nanoparticles and nickel hydroxide by adsorbing ethylene glycol(EG-Ni(OH)2@CeO2),which produced ultrasmall nanosheets uniformly attached onto carbon cloth substrate.According to the characterization and density functional theory(DFT),the ethylene glycol-induced nickel–cerium interface had strong electron interaction,generating numerous of Ni^(3-δ)+active sites,reducing the energy reaction barrier,and promoting the electron-transport kinetics in the catalytic system.EG-Ni(OH)2@CeO2 showed excellent OER performance,with a low overpotential(335 m V)at 50 m A cm^-2 and a small Tafel slope(67.4 m V dec^-1).And the EG-Ni(OH)2@CeO2 also maintained stable for up to 60 h at 10,20,and 30 m A cm^-2.Overall,this research shows the significance of the interface engineering of metal materials based on organic-solvent adsorption to improve the electrocatalytic OER process.展开更多
基金Hainan Province Science and Technology Special Fund(Nos.ZDYF2021SHFZ068 and ZDKJ2021029)National Natural Science Foundation of China(No.52262014)+1 种基金Hainan Provincial Natural Science Foundation of China(No.823CXTD376)Youth Foundation of Hainan Province(No.221QN0898).
文摘Strain engineering of two-dimensional(2D)material interfaces represents a powerful strategy for enhanc-ing the electrocatalytic activity of water splitting.However,maintaining catalytic stability under various harsh conditions by introducing interface strain remains a great challenge.The catalyst developed and evaluated herein comprised Ir clusters dispersed on 2D NiO nanosheets(NSs)derived from metal organic frameworks(lr@NiO/C_(BDc)),which displays a high activity and stability under all pH conditions,and even a change of only 1%in the applied voltage is observed after continuous electrocatalytic operation for over 1800 h under alkaline conditions.Through combined experimental and computational studies,we found that the introduced interfacial strain contributes to the outstanding structural stability of the Ir@NiO/CBDC catalyst,arising from its increased Ir and Ni vacancy formation energies,and hence suppressing its leach-ing.Moreover,strain also enhances the kinetically sluggish electrocatalytic water splitting reaction by op-timizing its electronic structure and coordination environment.This work highlights the effects of strain on catalyst stability and provides new insights for designing widely applicable electrocatalysts.
基金financially supported by the National Natural Science Foundation of China(51762012 and 51862006)the Key Research and Development Project of Hainan Province(ZDYF2018106)the Research Unit of Island Emergency Medicine of Chinese Academy of Medical Sciences(2019RU013)。
文摘As a half-reaction to obtain high-efficiency and stable water-splitting,oxygen evolution reaction(OER)is a slow-kinetics process involving a four-electron(4e^-)transfer process and therefore requires catalysts to fasten electron transfer.Here,we rationally optimized an interface material of ceria nanoparticles and nickel hydroxide by adsorbing ethylene glycol(EG-Ni(OH)2@CeO2),which produced ultrasmall nanosheets uniformly attached onto carbon cloth substrate.According to the characterization and density functional theory(DFT),the ethylene glycol-induced nickel–cerium interface had strong electron interaction,generating numerous of Ni^(3-δ)+active sites,reducing the energy reaction barrier,and promoting the electron-transport kinetics in the catalytic system.EG-Ni(OH)2@CeO2 showed excellent OER performance,with a low overpotential(335 m V)at 50 m A cm^-2 and a small Tafel slope(67.4 m V dec^-1).And the EG-Ni(OH)2@CeO2 also maintained stable for up to 60 h at 10,20,and 30 m A cm^-2.Overall,this research shows the significance of the interface engineering of metal materials based on organic-solvent adsorption to improve the electrocatalytic OER process.