双功能
过电位
电负性
密度泛函理论
材料科学
电催化剂
析氧
催化作用
吉布斯自由能
单层
物理化学
化学物理
计算化学
纳米技术
化学
热力学
电化学
物理
有机化学
电极
作者
Xuefei Liu,Yuefei Zhang,Wentao Wang,Yuanzheng Chen,Wenjun Xiao,Tianyun Liu,Zhen Zhong,Zijiang Luo,Zhao Ding,Zhaofu Zhang
标识
DOI:10.1021/acsami.1c22309
摘要
It is vital to search for highly efficient bifunctional oxygen evolution/reduction reaction (OER/ORR) electrocatalysts for sustainable and renewable clean energy. Herein, we propose a single transition-metal (TM)-based defective AlP system to validate bifunctional oxygen electrocatalysis by using the density functional theory (DFT) method. We found that the catalytic activity is enhanced by substituting two P atoms with two N atoms in the Al vacancy of the TM-anchored AlP monolayer. Specifically, the overpotential of OER(ORR) in Co- and Ni-based defective AlP systems is found to be 0.38 (0.25 V) and 0.23 V (0.39 V), respectively, showing excellent bifunctional catalytic performance. The results are further presented by establishing the volcano plots and contour maps according to the scaling relation of the Gibbs free-energy change of *OH, *O, and *OOH intermediates. The d-band center and the product of the number of d-orbital electrons and electronegativity of the TM atom are the ideal descriptors for this system. To investigate the activity origin of the OER/ORR process, we performed the machine learning (ML) algorithm. The result indicates that the number of TM-d electrons (Ne), the radius of TM atoms (rd), and the charge transfer of TM atoms (Qe) are the three primary descriptors characterizing the adsorption behavior. Our results can provide a theoretical guidance for designing highly efficient bifunctional electrocatalysts and pave a way for the DFT-ML hybrid method in catalysis research.
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