Novel two-dimensional MOF as a promising single-atom electrocatalyst for CO2 reduction: A theoretical study
Novel two-dimensional MOF as a promising single-atom electrocatalyst for CO2 reduction: A theoretical study
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新型二维 MOF 作为一种有前景的 CO2 还原单原子电催化剂：理论研究
DOI：
10.1016/j.apsusc.2019.143993
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发表时间：
2020-01-15
影响因子：
6.7
通讯作者：
Sun, Qiao
中科院分区：
文献类型：
--
作者：
Cui, Qianyi;Qin, Gangqiang;Sun, Qiao
CO2的转化对于缓解环境和资源危机非常重要。在这里，我们利用密度泛函理论（DFT）计算系统地研究了一系列新兴的二维金属有机框架（MOF）。二维MOFs具有单原子催化剂（SAC）的特性，比掺杂单金属原子改性材料具有更高的可操作性和实用性。我们的结果表明，钼基 MOF 在环境条件下具有良好的 CO2 活化和还原能力。 CO2选择性还原为甲烷的能量成本值较低，仅为0.42 eV。此外，基于MoO的MOF可以将能量输入进一步降低至0.27 eV。这些能量输入远低于传统的纯金属催化剂和一些基于贵金属的新型 SAC。这项研究在原子水平上提供了见解，即新型钼基 MOF（其中钼是一种地球上储量丰富的金属）可以用作一种经济高效的单原子电催化剂，用于在温和条件下还原二氧化碳。
The conversion of CO2 is very important for alleviating environmental and resource crisis. Herein, we have systemically investigated a family of emerging 2D metal-organic frameworks (MOFs) utilizing density functional theory (DFT) calculations. The 2D MOFs possess characteristics of single-atom catalysts (SACs), and present higher maneuverability and practicability than modifying materials by doped single metal atoms. Our results show that the Mo-based MOF presents the promising capability of CO2 activation and reduction under ambient conditions. The value of energy cost for CO2 selectively reduced to methane is low with a value of only 0.42 eV. Moreover, the energy input can be further decreased to 0.27 eV with MoO based MOF. These energy inputs are substantially lower than classical pure metal catalysts and some novel SACs based on noble metals. This study provides insights at the atomic level that novel Mo-based MOF, in which molybdenum is an earth-abundant metal, can be used as a cost-effective single-atom electrocatalyst for CO2 reduction at mild conditions.