材料科学
纳米片
锥面
选择性
电子转移
有限元法
电化学
化学工程
催化作用
化学物理
纳米技术
光化学
物理化学
电极
复合材料
热力学
有机化学
化学
物理
工程类
作者
Chunzhong Li,Tingting Zhang,Heng Liu,Zhongyuan Guo,Zhongliang Liu,Huancong Shi,Jialin Cui,Hao Li,Huihui Li,Chunzhong Li
标识
DOI:10.1002/adma.202312204
摘要
The electrochemical carbon dioxide (CO2 ) reduction reaction (CO2 RR) involves a multistep proton-coupled electron transfer (PCET) process that generates a variety of intermediates, making it challenging to transform them into target products with high activity and selectivity. Here, a catalyst featuring a nanosheet-stacked sphere structure with numerous open and deep conical cavities (OD-CCs) is reported. Under the guidance of the finite-element method (FEM) simulations and theoretical analysis, it is shown that exerting control over the confinement space results in diffusion limitation of the carbon intermediates, thereby increasing local pressure and subsequently enhancing localized *CO coverage for dimerization. The nanocavities exhibit a structure-driven shift in selectivity of multicarbon (C2+ ) product from 41.8% to 81.7% during the CO2 RR process.
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