Abstract

With the development of the economy, the greenhouse effect is becoming more and more serious, and the culprit is elected as carbon dioxide, so it is urgent to find an effective way to alleviate the greenhouse effect. The carbon dioxide electrochemical reduction reaction (CO₂RR) can realize the resource conversion of carbon dioxide, which is the key technology to realize the natural “carbon cycle” and alleviate many environmental problems caused by excessive carbon dioxide emissions. Due to the excellent performance of metal nitrogen-doped carbon catalysts (M-N-C catalysts), in this letter, we choose M-N-C catalysts (M = a series of transition metals) to conduct a series of studies. We used the PBE method of density functional theory (DFT) to conduct a detailed study on the changes of the electroreduction of CO₂ on M-N-C (M = Fe/Ni/Cu/Zn/Ru/Rh/Pd/Ag/Cd/Os/Ir/Pt/Au) catalysts, compare the catalytic performance of the selected nitrogen-doped metal carbon catalyst, and focus on simulating the mechanism of various CO₂ electrochemical reduction reactions. The research points out that M-N-C (M = Ir) catalysts have good performance in catalyzing the reduction of carbon dioxide into carbon products with economic value, especially methane and methanol, and multicarbon products such as ethanol.

Graphical abstract

中文翻译：

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单原子分散催化剂（金属-氮-碳）高效电催化CO 2还原反应的理论见解

摘要

随着经济的发展，温室效应越来越严重，罪魁祸首被选为二氧化碳，因此迫切需要找到一种减轻温室效应的有效途径。二氧化碳电化学还原反应（CO ₂ RR）可以实现二氧化碳的资源转化，这是实现自然“碳循环”并缓解二氧化碳排放过多引起的许多环境问题的关键技术。由于金属氮掺杂碳催化剂（MNC催化剂）的优异性能，在本文中，我们选择MNC催化剂（M =一系列过渡金属）进行一系列研究。我们使用密度泛函理论（DFT）的PBE方法对CO的电还原变化进行了详细的研究₂在MNC（M = Fe / Ni / Cu / Zn / Ru / Rh / Pd / Ag / Cd / Os / Ir / Pt / Au）催化剂上，比较所选氮掺杂金属碳催化剂的催化性能，并重点关注模拟各种CO ₂电化学还原反应的机理。研究指出，MNC（M = Ir）催化剂具有良好的催化性能，可将二氧化碳还原为具有经济价值的碳产品，特别是甲烷和甲醇，以及乙醇等多碳产品。

图形概要