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Atomically Dispersed Ni/Cu Dual Sites for Boosting the CO2 Reduction Reaction
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-10-01 , DOI: 10.1021/acscatal.1c02319
Huiyuan Cheng 1 , Xuemei Wu 1 , Manman Feng 1 , Xiangcun Li 1 , Guangping Lei 2 , Zihao Fan 1 , Dongwei Pan 1 , Fujun Cui 3 , Gaohong He 1, 3
Affiliation  

Developing diatomic catalysts (DACs) for the CO2 reduction reaction (CO2RR) has emerged as a promising leading-edge research area owing to their maximum atomic utility and more sophisticated functionalities. However, the proper design of DACs at an atomic level and an understanding of the synergistic mechanism of binary sites remain challenging. Herein, an N-rich carbon matrix with precisely controlled Ni/Cu dual sites is synthesized through the assistance of metal–organic frameworks. The as-prepared catalyst presents high CO Faradaic efficiency of over 95% from −0.39 to −1.09 V vs reversible hydrogen electrode (RHE) with the maximum value of 99.2% at −0.79 V vs RHE and long-term durability of 60 h electrolysis. Density functional theory studies reveal that the electronic redistribution and band gap narrowing induced by the adjacent NiN4 and CuN4 moieties enhance the electron conductivity and strengthen the bonding interactions between *COOH intermediates and Ni centers, thus lowering the overall reaction barriers and promoting CO generation.

中文翻译:

用于促进 CO2 还原反应的原子分散 Ni/Cu 双位点

开发用于 CO 2还原反应 (CO 2RR)因其最大的原子效用和更复杂的功能而成为一个有前途的前沿研究领域。然而,在原子水平上正确设计 DAC 和理解二元位点的协同机制仍然具有挑战性。在此,通过金属-有机骨架的辅助合成了具有精确控制的 Ni/Cu 双位点的富氮碳基体。所制备的催化剂在 -0.39 至 -1.09 V vs 可逆氢电极 (RHE) 范围内具有超过 95% 的高 CO 法拉第效率,在 -0.79 V vs RHE 时的最大值为 99.2%,并且具有 60 小时电解的长期耐久性. 密度泛函理论研究表明,相邻的 NiN 4和 CuN 4引起的电子重分布和带隙变窄 部分增强了电子传导性并加强了 *COOH 中间体和 Ni 中心之间的键合相互作用,从而降低了整体反应势垒并促进了 CO 的生成。
更新日期:2021-10-15
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