The intrinsic activity and durability of oxygen evolution reaction(OER)electrocatalysts are mainly dominated by the surface and interface properties of active materials.Herein,a core-shell heterogeneous structure(NF/N...The intrinsic activity and durability of oxygen evolution reaction(OER)electrocatalysts are mainly dominated by the surface and interface properties of active materials.Herein,a core-shell heterogeneous structure(NF/NiSe@Fe_(2)O_(3))is fabricated via two-step hydrothermal method,which exhibits a low overpotential of 220 mV(or 282 mV)at 10 mA/cm^(2)(or 200 mA/cm^(2)),a small Tafel slope of 36.9 mV/dec,and long-term stability(-230 h)in 1 mol/L KOH for OER.X-ray photoelectron spectroscopy and X-ray absorption spectroscopy reveal the(oxy)hydroxide-rich surface and strong coupling interface between NiSe and Fe_(2)O_(3)via the Fe-Se bond.Density functional theory calculation suggests that the d-band center and electronic state of NiSe@Fe_(2)O_(3)heterojunction are well optimized due to the formation of Fe-Se bond,which is favorable for the enhanced OER activity because of the easy adsorption of oxygen-containing intermediates and desorption of O^(2)in the OER process.In addition,the unique core-shell structure and robust bonding interface are responsible for the good stability for OER.This work provides fundamental insights on the bonding effect that determine the performance of OER electrocatalyst.展开更多
基金supported by the National Natural Science Foundation of China (21673105)the support received from NSF under the award numbers OIA-1539035 and CHE-1539035supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Award No. DE-AC02-06CH11357
文摘The intrinsic activity and durability of oxygen evolution reaction(OER)electrocatalysts are mainly dominated by the surface and interface properties of active materials.Herein,a core-shell heterogeneous structure(NF/NiSe@Fe_(2)O_(3))is fabricated via two-step hydrothermal method,which exhibits a low overpotential of 220 mV(or 282 mV)at 10 mA/cm^(2)(or 200 mA/cm^(2)),a small Tafel slope of 36.9 mV/dec,and long-term stability(-230 h)in 1 mol/L KOH for OER.X-ray photoelectron spectroscopy and X-ray absorption spectroscopy reveal the(oxy)hydroxide-rich surface and strong coupling interface between NiSe and Fe_(2)O_(3)via the Fe-Se bond.Density functional theory calculation suggests that the d-band center and electronic state of NiSe@Fe_(2)O_(3)heterojunction are well optimized due to the formation of Fe-Se bond,which is favorable for the enhanced OER activity because of the easy adsorption of oxygen-containing intermediates and desorption of O^(2)in the OER process.In addition,the unique core-shell structure and robust bonding interface are responsible for the good stability for OER.This work provides fundamental insights on the bonding effect that determine the performance of OER electrocatalyst.