Citation: Dong Xiang, Kunzhen Li, Kanghua Miao, Ran Long, Yujie Xiong, Xiongwu Kang. 胺功能化的铜催化剂：氢键介导的电化学CO₂还原为C₂产物以及优越的可充电Zn-CO₂电池性能[J]. Acta Physico-Chimica Sinica, ;2024, 40(8): 230802. doi: 10.3866/PKU.WHXB202308027 shu

胺功能化的铜催化剂：氢键介导的电化学CO₂还原为C₂产物以及优越的可充电Zn-CO₂电池性能

Dong Xiang ¹ ,
Kunzhen Li ¹ ,
Kanghua Miao ¹ ,
Ran Long ² ,
Yujie Xiong ^2,, ,
Xiongwu Kang ^1,,

1.
New Energy Research Institute, School of Environment and Energy, South China University of Technology, Guangzhou 510006, China;
2.
Hefei National Laboratory for Physical Sciences at the Microscale, School of Chemistry and Materials Science, University of Science and Technology of China, Hefei 230026, China

Corresponding author: Yujie Xiong, Xiongwu Kang,
Received Date: 15 August 2023
Revised Date: 20 September 2023
Accepted Date: 28 September 2023

Fund Project: The project was supported by the National Natural Science Foundation of China (U2032151, 21725102, 91961106).

有机分子功能化是一种有前景的策略，用于调控电化学CO₂还原反应(eCO₂RR)的C₂₊产物选择性和活性。然而，我们对于电化学CO₂还原调控机制的分子水平理解仍然不够清晰。在本文中，我们成功制备了铜纳米颗粒，并使用一系列胺类衍生物(如十六胺(HAD)、N-甲基十六胺(N-MHDA)、十六烷基二甲胺(HDDMA)和十六酰胺(PMM))对其进行功能化，以系统地研究胺表面活性剂分子结构对eCO₂RR选择性和活性的影响。结果表明，HDA的功能化可以将C₂产物和C₂H₄的法拉第效率(FE)提高至73.5%和46.4%，并且在−0.9 V vs. RHE (可逆氢电极)电位下，C₂产物的分电流密度为131.4 mA·cm⁻²。理论研究发现，HDA通过与CO₂和eCO₂RR中间体之间的氢键相互作用，富集了*CO₂、*CO和其他反应中间体，降低了CO―CHO耦合反应的动力学能垒，从而促进了eCO₂RR向C₂产物的转化。当胺基的H原子被甲基取代后，氢键相互作用减弱，竞争的析氢反应加剧。PMM通过Cu―O键与Cu表面发生键合，而不是通过Cu―N键，导致Cu-PMM更倾向于产乙醇。原位拉曼光谱显示，在Cu-HDA表面，CO主要吸附在Cu的顶位吸附位点上，与在Cu表面上的桥式吸附不同，这可能是因为前者表面对CO的富集引发了CO的吸附构型变化。HDA功能化还提高了Cu催化剂的表面pH。基于Cu-HDA组装的可充电Zn-CO₂电池在放电电流密度为16 mA∙cm^–2时，最大功率密度为6.48 mW∙cm^–2，并具有长达60 h的良好充放电稳定性。本研究的重点在于通过在分子水平上调节Cu基材料的CO₂RR活性和选择性，促进CO₂-C₂的转化，这可能为提高C₂产物的产率提供新的见解。
- CO₂ reduction,
- CO―CHO coupling,
- Organic functionalization,
- In situ Raman,
- C₂ product,
- Zn-CO₂ battery
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胺功能化的铜催化剂：氢键介导的电化学CO2还原为C2产物以及优越的可充电Zn-CO2电池性能

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胺功能化的铜催化剂：氢键介导的电化学CO₂还原为C₂产物以及优越的可充电Zn-CO₂电池性能