电催化剂
催化作用
析氧
纳米团簇
吸附
合金
材料科学
氧气
化学工程
活化能
碳纤维
动力学
化学
纳米技术
物理化学
电化学
复合材料
电极
冶金
有机化学
量子力学
工程类
物理
复合数
作者
Yangyang Tan,Zeyi Zhang,Lei Zhao,Liyue Yu,Wei Wu,Zichen Wang,Niancai Cheng
标识
DOI:10.1016/j.apcatb.2021.121006
摘要
Optimizing the electronic structure of the electrocatalyst to adjust the adsorption energies of oxygen intermediates to approach the equilibrium potential (U0RHE = 1.23 V) is of paramount importance to inhibit the sluggish reaction kinetics of the oxygen reduction/oxygen evolution reaction (ORR/OER), yet remains a huge challenge. Herein, a hierarchical 1D/3D hollow carbon nanopolyhedron with strong electron coupling between the encapsulated CoNi alloy and Co-Nx sites in N-CNTs was designed by a silicon protection-Ni infiltration strategy. Impressively, the optimized CoNi/Co-N@HNC catalyst exhibits high oxygen catalytic activity with a small potential gap of 0.73 V and superior ZABs durability over 350 h. DFT simulation results revealed that coupling with CoNi nanoclusters can effectively downshift the Ed energy levels of the Co adsorption site in CoN4, dramatically decreased the energy barrier of the rate-determining step (OH* to OH- in ORR; OH* to O* in OER), thereby promote the overall oxygen catalysis reaction kinetics.
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