材料科学
磷化物
密度泛函理论
双功能
分解水
X射线吸收光谱法
电化学
X射线光电子能谱
析氧
催化作用
物理化学
化学工程
吸收光谱法
计算化学
电极
化学
金属
生物化学
冶金
工程类
物理
光催化
量子力学
作者
Rui Zhang,Ziyu Wei,Gaoyang Ye,Guanjie Chen,Jiaojiao Miao,Xuehua Zhou,Xiangwei Zhu,Xiaoqun Cao,Xiangnan Sun
标识
DOI:10.1002/aenm.202101758
摘要
Abstract To generate “green hydrogen,” electrochemical water splitting is regarded as the most promising method, which requires highly efficient bifunctional electrocatalysts to accelerate the hydrogen and oxygen evolution reactions (HER and OER). Herein, a “d‐electron complementation” principle to develop such candidates is proposed. By taking advantage of the filling characteristics of 3d orbitals, vanadium‐cobalt phosphide (V‐CoP) is synthesized. According to X‐ray absorption fine structure and X‐ray photoelectron spectroscopy investigation, V can disorder the coordination environment of Co, leading to increased/decreased charge density in Co(P)/Co(O). As a result, V‐CoP shows impressive bifunctional activity, which only needs overpotentials of 46 and 267 mV to deliver 10 mA cm −2 for the HER and OER, respectively. Density functional theory calculations reveal that the accelerated H 2 O dissociation process on the VO x /CoO x /CoP surface and H conversion kinetics on the V‐neighboring CoCo bridge site result in promoted HER activity. Furthermore, the up‐shifted d‐band center of V‐CoOOH endows the V‐neighboring Co site with a lowered energy barrier for the OER. This work serves as a proof‐of‐concept for the application of the “d‐electron complementation” principle, which can be a generalized guideline to design and develop novel highly efficient catalysts.
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