电催化剂
过电位
塔菲尔方程
密度泛函理论
介电谱
X射线光电子能谱
离解(化学)
循环伏安法
化学
分析化学(期刊)
过渡金属
催化作用
计算化学
物理化学
电化学
化学工程
电极
生物化学
色谱法
工程类
作者
Hua‐Jie Niu,Chuanxue Huang,Tong Sun,Zhen Fang,Xiaoxing Ke,Ruimin Zhang,Nian Ran,Jianbo Wu,Jianjun Li,Wei Zhou
标识
DOI:10.1002/anie.202401819
摘要
Density functional theory (DFT) calculations demonstrate neighboring Pt atoms can enhance the metal activity of NiCoP for hydrogen evolution reaction (HER). However, it remains a great challenge to link Pt and NiCoP. Herein, we introduced curvature of bowl‐like structure to construct Pt/NiCoP interface by adding a minimal 1‰‐molar‐ratio Pt. The as‐prepared sample only requires an overpotential of 26.5 and 181.6 mV to accordingly achieve the current density of 10 and 500 mA cm−2 in 1M KOH. The water dissociation energy barrier (Ea) has a ~43% decrease compared with NiCoP counterpart. It also shows an ultrahigh stability with a small degradation rate of 10.6 μV h−1 at harsh conditions (500 mA cm−2 and 50 °C) after 3000 hrs. X‐ray photoelectron spectroscopy (XPS), soft X‐ray absorption spectroscopy (sXAS), and X‐ray absorption fine structure (XAFS) verify the interface electron transfer lowers the valence state of Co/Ni and activates them. DFT calculations also confirm the catalytic transition step of NiCoP can change from Heyrovsky (2.71 eV) to Tafel step (0.51 eV) in the neighborhood of Pt, in accord with the result of the improved Hads at the interface disclosed by in‐situ electrochemical impedance spectroscopy (EIS) and scanning electrochemical microscopy (SECM) tests.
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