Theoretical exploration on the performance of single and dual-atom Cu catalysts on the CO2 electroreduction process: a DFT study.
Theoretical exploration on the performance of single and dual-atom Cu catalysts on the CO2 electroreduction process: a DFT study.
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单原子和双原子铜催化剂在 CO2 电还原过程中性能的理论探索：DFT 研究。
DOI：
10.1039/d3cp02403b
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发表时间：
2023
期刊：
影响因子：
--
通讯作者：
Bai Z
中科院分区：
文献类型：
--
作者：
Bai Z
金属氮掺杂碳(MNC)催化剂电还原二氧化碳(CO2)是一种通过将CO2分子转化为增值化学品来缓解全球变暖的有效方法。本研究采用密度泛函理论(DFT)方法对单原子和双原子铜催化剂在CO2电还原过程中的行为进行了系统的研究。CuNC-4-吡啶和CuCuNC-4a两种结构有利于C2的生成，具有较高的稳定性。随后，我们探索了在CuNC-4-吡啶和CuNC-4a上CO2电还原过程中关键产物(CO、HCOOH、CH3OH、CH4、C2H6O、C2H4和C2H6)的详细路径。本研究揭示了CuNC-4-吡啶和CuCuNC-4a在CO2电还原过程中关键产物的形成机理，为设计低极限电位和高产物选择性的MNC催化剂提供了重要的指导意义。
Carbon dioxide (CO2) electroreduction by metal–nitrogen-doped carbon (MNC) catalysts is a promising and efficient method to mitigate global warming by converting CO2 molecules to value-added chemicals. In this research, we systematically studied the behaviours of single and dual-atom Cu catalysts during the CO2 electroreduction process using density functional theory (DFT) calculations. Two structures, i.e., CuNC-4-pyridine and CuCuNC-4a, were found to be beneficial for C2 chemical generation with relatively high stabilities. Subsequently, we explored the detailed pathways of key products (CO, HCOOH, CH3OH, CH4, C2H6O, C2H4 and C2H6) during CO2 electroreduction on CuNC-4-pyridine and CuCuNC-4a. This research reveals the mechanisms of key product formation during CO2 electroreduction on CuNC-4-pyridine and CuCuNC-4a, which would provide important insights to guide the design of MNC catalysts with low limiting potentials and high product selectivity.