Ni-Fe-based catalysts are considered to be among the most active catalysts for the oxygen evolution reaction(OER)under alkaline conditions,with Fe playing a crucial role.However,Fe leaching occurs during the reaction ...Ni-Fe-based catalysts are considered to be among the most active catalysts for the oxygen evolution reaction(OER)under alkaline conditions,with Fe playing a crucial role.However,Fe leaching occurs during the reaction due to thermodynamic instability,which has resulted in conflicting reports within the literature regarding its role.To clarify this point,we propose a strategy consisting of modulating the electronic orbital occupancy to suppress the extensive loss of Fe atoms during the OER process.Theoretical calculations,in-situ X-ray photoelectron spectroscopy,molecular dynamics simulations,and a series of characterization showed that the stable presence of Fe not only accelerates the electron transfer process but also optimizes the reaction barriers of the oxygen evolution intermediates,promoting the phase transition of Fe_(5)Ni_(4)S_(8)to highly active catalytic species.The modulated Fe_(5)Ni_(4)S_(8)-based pre-catalysts exhibit improved OER activity and long-term durability.This study provides a novel perspective for understanding the role of Fe in the OER process.展开更多
The development of 3D structural composites with electromagnetic(EM)wave absorption could attenuate EM waves.Herein,magnetized flower-like Cu_(9)S_(5)/ZnFe_(2)O_(4)composites were fabricated through a multistep hydrot...The development of 3D structural composites with electromagnetic(EM)wave absorption could attenuate EM waves.Herein,magnetized flower-like Cu_(9)S_(5)/ZnFe_(2)O_(4)composites were fabricated through a multistep hydrothermal method.The crystallographic and surface phase chemical information,morphological structure,and magnetic and EM parameters of the composites were analyzed.The prepared Cu_(9)S_(5)/ZnFe_(2)O_(4)composites have multiple loss paths for EM waves and present an overall 3D flower-like structure.The Cu_(9)S_(5)/ZnFe_(2)O_(4)composites exhibit a minimum reflection loss of-54.38 dB and a broad effective absorption bandwidth of 5.92 GHz.Through magnetization,ZnFe_(2)O_(4)particles are self-assembled and grown on the surfaces of Cu_(9)S_(5).Such a modification is conducive to the generation of additional cross-linking contact sites and the effective introduction of a large number of phase interfaces,crystalline defects,special three-dimensional flower-like structures,and magneto-electrical coupling loss effects.Moreover,the synergistic effect of multiple loss strategies effectively improves EM wave absorption by the material.This work can provide a strategy for the use of magnetizationmodified sulfide composite functional materials in EM wave absorption.展开更多
基金financially supported by the Scientific and Technological Development Program of Jilin Province(20220201138GX)the support of the National Key R&D Program of China(No.2022YFA1503801)+1 种基金CAS Project for Young Scientists in Basic Research(No.YSBR-022)the Young Cross Team Project of CAS(No.JCTD-2021-14)。
文摘Ni-Fe-based catalysts are considered to be among the most active catalysts for the oxygen evolution reaction(OER)under alkaline conditions,with Fe playing a crucial role.However,Fe leaching occurs during the reaction due to thermodynamic instability,which has resulted in conflicting reports within the literature regarding its role.To clarify this point,we propose a strategy consisting of modulating the electronic orbital occupancy to suppress the extensive loss of Fe atoms during the OER process.Theoretical calculations,in-situ X-ray photoelectron spectroscopy,molecular dynamics simulations,and a series of characterization showed that the stable presence of Fe not only accelerates the electron transfer process but also optimizes the reaction barriers of the oxygen evolution intermediates,promoting the phase transition of Fe_(5)Ni_(4)S_(8)to highly active catalytic species.The modulated Fe_(5)Ni_(4)S_(8)-based pre-catalysts exhibit improved OER activity and long-term durability.This study provides a novel perspective for understanding the role of Fe in the OER process.
基金This work was supported by the National Natural Science Foundation of China(No.51477002)the University Synergy Innovation Program of Anhui Province,China(No.GXXT-2019-028).
文摘The development of 3D structural composites with electromagnetic(EM)wave absorption could attenuate EM waves.Herein,magnetized flower-like Cu_(9)S_(5)/ZnFe_(2)O_(4)composites were fabricated through a multistep hydrothermal method.The crystallographic and surface phase chemical information,morphological structure,and magnetic and EM parameters of the composites were analyzed.The prepared Cu_(9)S_(5)/ZnFe_(2)O_(4)composites have multiple loss paths for EM waves and present an overall 3D flower-like structure.The Cu_(9)S_(5)/ZnFe_(2)O_(4)composites exhibit a minimum reflection loss of-54.38 dB and a broad effective absorption bandwidth of 5.92 GHz.Through magnetization,ZnFe_(2)O_(4)particles are self-assembled and grown on the surfaces of Cu_(9)S_(5).Such a modification is conducive to the generation of additional cross-linking contact sites and the effective introduction of a large number of phase interfaces,crystalline defects,special three-dimensional flower-like structures,and magneto-electrical coupling loss effects.Moreover,the synergistic effect of multiple loss strategies effectively improves EM wave absorption by the material.This work can provide a strategy for the use of magnetizationmodified sulfide composite functional materials in EM wave absorption.
