Rational design of dual-metal-site catalysts for electroreduction of carbon dioxide,Journal of Materials Chemistry A

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Rational design of dual-metal-site catalysts for electroreduction of carbon dioxide
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2020-03-09 , DOI: 10.1039/d0ta00033g
Gan Luo _{1,

2,

3,

4,

5} , Yu Jing _{6,

7,

8,

9} , Yafei Li _{1,

2,

3,

4,

5}

Affiliation

Electroreduction of carbon dioxide (CO₂) to useful chemical fuels represents an efficient and green strategy for solving the existing energy and environmental problems of human society. Developing efficient and inexpensive electrocatalysts for the CO₂ reduction reaction (CRR) has been a key scientific issue. Due to the robust scaling relationship that exists between CRR intermediates, it is difficult to improve the catalytic activity of commonly used transition metal catalysts. In this work, inspired by recent experimental progress in fabricating graphene-based dual-metal-site catalysts (DMSCs), we systematically studied the CRR activity of a series of DMSCs by means of density functional theory computations and micro-kinetics simulations. By using the adsorption strength of OH* and COOH* species as an indicator, three DMSCs, namely Cu/Mn, Ni/Mn and Ni/Fe, were identified as promising candidates after two-rounds of screening. Remarkably, it is found that the scaling relationship between the adsorption strength of COOH* and CO* species has been broken in these three DMSCs, leading to a superior CRR activity. Our work provides a useful guideline for further developing CRR electrocatalysts.

中文翻译：

二氧化碳电还原双金属位催化剂的合理设计

将二氧化碳（CO ₂）电还原为有用的化学燃料代表了解决人类社会现有的能源和环境问题的有效和绿色战略。开发用于CO _2的高效廉价的电催化剂还原反应（CRR）一直是关键的科学问题。由于CRR中间体之间存在牢固的结垢关系，因此难以提高常用过渡金属催化剂的催化活性。在这项工作中，受最近在制造基于石墨烯的双金属中心催化剂（DMSC）方面的实验进展的启发，我们通过密度泛函理论计算和微动力学模拟系统地研究了一系列DMSC的CRR活性。以OH *和COOH *种类的吸附强度为指标，经过两轮筛选，确定了Cu / Mn，Ni / Mn和Ni / Fe这三种DMSCs为有前途的候选物。值得注意的是，发现在这三个DMSC中，COOH *和CO *的吸附强度之间的比例关系已被破坏，导致卓越的CRR活性。我们的工作为进一步开发CRR电催化剂提供了有用的指导。

更新日期：2020-03-09

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