带CN空位的冷等离子体活化Cu-Co催化剂促进CO2电还原制备低碳醇

IF 14 1区 化学 Q1 CHEMISTRY, APPLIED 能源化学 Pub Date : 2023-10-01 DOI:10.1016/j.jechem.2023.06.004
Junyi Peng , Qiang Zhang , Yang Zhou , Xiaohui Yang , Fang Guo , Junqiang Xu
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引用次数: 3

摘要

电催化CO2还原反应制备低碳醇是一项具有挑战性的任务,尤其是对乙醇的高选择性,这主要受到反应中间体和随后的C–C偶联的调节。利用H2冷等离子体成功地制备了一种具有CN空位的Cu-Co双金属催化剂,将CO2RR高效转化为低碳醇。Cu-Co-PBA-VCN(具有CN空位的普鲁士蓝类似物)电催化剂产生甲醇和乙醇作为主要产物,在−0.9 V vs.RHE下,总低碳醇FE为83.8%(甲醇:39.2%,乙醇:44.6%),优异的耐久性(100小时)和−0.21 V的小起始电位。ATR-SIRAS(衰减全内反射表面增强红外吸收光谱)和DFT(密度泛函理论)表明,VCN的空间位阻可以增强*COOH产生的CO,并且CO在均匀分散的Cu原子上的溢出也可以增加C–C耦合。这项工作为CO2RR转化为低碳醇产品的电催化剂的设计和制备提供了一种策略,并强调了催化剂空间位阻对催化性能的影响。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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Cold plasma-activated Cu-Co catalysts with CN vacancies for enhancing CO2 electroreduction to low-carbon alcohol

Electrocatalytic CO2 reduction reaction to low-carbon alcohol is a challenging task, especially high selectivity for ethanol, which is mainly limited by the regulation of reaction intermediates and subsequent C–C coupling. A Cu-Co bimetallic catalyst with CN vacancies is successfully developed by H2 cold plasma toward a high-efficiency CO2RR into low-carbon alcohol. The Cu-Co PBA-VCN (Prussian blue analogues with CN vacancies) electrocatalyst yields methanol and ethanol as major products with a total low-carbon alcohol FE of 83.8% (methanol: 39.2%, ethanol: 44.6%) at −0.9 V vs. RHE, excellent durability (100 h) and a small onset potential of −0.21 V. ATR-SEIRAS (attenuated total internal reflection surface enhanced infrared absorption spectroscopy) and DFT (density functional theory) reveal that the steric hindrance of VCN can enhance the CO generation from *COOH, and the C–C coupling can also be increased by CO spillover on uniformly dispersed Cu atoms. This work provides a strategy for the design and preparation of electrocatalysts for CO2RR into low-carbon alcohol products and highlights the impact of catalyst steric hindrance to catalytic performance.

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CiteScore
23.60
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