Enhancing local K(+) adsorption by high-density cube corners for efficient electroreduction of CO(2) to C(2+) products

利用高密度立方角增强局部K(+)吸附,以实现CO(2)高效电还原为C(2+)产物

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Abstract

Reducing carbon dioxide (CO(2)) to high value-added chemicals using renewable electricity is a promising approach to reducing CO(2) levels in the air and mitigating the greenhouse effect, which depends on high-efficiency electrocatalysts. Copper-based catalysts can be used for electroreduction of CO(2) to produce C(2+) products with high added value, but suffer from poor stability and low selectivity. Herein, we propose a strategy to enhance the field effect by varying the cubic corner density on the surface of Cu(2)O microspheres for improving the electrocatalytic performance of CO(2) reduction to C(2+) products. Finite element method (FEM) simulation results show that the high density of cubic corners helps to enhance the local electric field, which increases the K(+) concentration on the catalyst surface. The results of CO(2) electroreduction tests show that the FE(C(2+)) of the Cu(2)O catalyst with high-density cubic corners is 71% at a partial current density of 497 mA cm(-2). Density functional theory (DFT) calculations reveal that Cu(2)O (111) and Cu(2)O (110) can effectively reduce the energy barrier of C-C coupling and improve the FE(C(2+)) at high K(+) concentrations relative to Cu(2)O (100). This study provides a new perspective for the design and development of efficient CO(2)RR catalysts.

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