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

doi:10.3866/PKU.WHXB202308027

物理化学学报 >> 2024, Vol. 40 >> Issue (8): 2308027.doi: 10.3866/PKU.WHXB202308027

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

项东¹, 李坤振¹, 苗康华¹, 龙冉², 熊宇杰²^,*(), 康雄武¹^,*()

¹ 华南理工大学新能源研究所, 环境与能源学院, 广州 510006
² 中国科学技术大学合肥微尺度物质科学国家研究中心, 化学与材料科学学院, 合肥 230026

收稿日期:2023-08-15 修回日期:2023-09-20 录用日期:2023-09-28 发布日期:2023-10-09
通讯作者: esxkang@scut.edu.cn (康雄武)Email: yjxiong@ustc.edu.cn (熊宇杰)
基金资助:
国家自然科学基金(U2032151); 国家自然科学基金(21725102); 国家自然科学基金(91961106)

Amine-Functionalized Copper Catalysts: Hydrogen Bonding Mediated Electrochemical CO₂ Reduction to C₂ Products and Superior Rechargeable Zn-CO₂ Battery Performance

Dong Xiang¹, Kunzhen Li¹, Kanghua Miao¹, Ran Long², Yujie Xiong²^,*(), Xiongwu Kang¹^,*()

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

Received:2023-08-15 Revised:2023-09-20 Accepted:2023-09-28 Published:2023-10-09
Contact: esxkang@scut.edu.cn (Xiongwu Kang)Email: yjxiong@ustc.edu.cn (Yujie Xiong)
Supported by:
the National Natural Science Foundation of China(U2032151); the National Natural Science Foundation of China(21725102); the National Natural Science Foundation of China(91961106)

1. 附件.pdf(3651KB)

摘要/Abstract

摘要：

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。

关键词: 二氧化碳还原, CO―CHO耦合, 有机分子功能化, 原位拉曼, C₂产物, Zn-CO₂电池

Abstract:

The electrochemical carbon dioxide reduction reaction (eCO₂RR) can convert CO₂ into valuable chemicals, achieving a carbon cycle. Copper-based catalysts have demonstrated a unique ability to produce C₂₊ products in eCO₂RR, which is often limited by the scaling relationship of the reaction intermediates, complex reaction mechanism and competitive H₂ evolution. Organic functionalization is a promising strategy for regulating the activity and selectivity of eCO₂RR toward C₂₊ products. However, the mechanism behind such regulation of eCO₂RR, especially at the molecular level, remains elusive. In this study, Cu nanoparticles were prepared and functionalized with a set of amine derivatives, including hexadecylamine (HDA), N-methylhexadecylamine (N-MHDA), hexadecyldimethylamine (HDDMA), and palmitamide (PMM). The impact of the molecular structure of the amine surfactants on the selectivity and activity toward eCO₂RR was systematically explored through both experiments and theoretical calculations. X-ray photoelectron spectroscopy and density functional theory calculations revealed that HDA functionalization of the Cu catalyst surface resulted in negative charge transfer from amine molecules to Cu. ECO₂RR was examined in a 1.0 mol∙L⁻¹ KOH aqueous electrolyte. HDA functionalization of the Cu catalyst achieved the highest Faradaic efficiency (FE) of 73.5% for C₂ products and 46.4% for C₂H₄, respectively. It also provided the highest C₂ partial current density of 131.4 mA∙cm⁻² at −0.9 Ⅴ vs. reversible hydrogen electrode (RHE) among these amine derivatives functionalized Cu catalysts. In contrast, the highest FE and partial current density for C₂ products achieved with pristine Cu catalysts were only 27.0% and 50.5 mA·cm⁻², respectively. Theoretical studies demonstrated that hydrogen bonding interactions of HDA with CO₂ and eCO₂RR intermediates enriched CO₂, CO, and other intermediates, lowered the kinetic energy barrier of CO―CHO coupling and thereby promoted eCO₂RR to C₂ products. Replacing the H atoms of the amine group with methyl groups in N-MHDA and HDDMA resulted in dominant hydrogen evolution reaction (HER) in eCO₂RR. PMM bonding with the Cu surface through a Cu―O bond, instead of Cu―N bonding as in HDA, N-MHDA and HDDMA, resulted in preferred ethanol production. In situ Raman spectroscopy indicated CO adsorption on Cu at atop sites for HDA-capped Cu catalysts, instead of bridge site CO adsorption on clean Cu surfaces, possibly due to the enriched CO in the former case. HDA also increased the local pH relative to pristine Cu catalysts. The Cu-HDA-based rechargeable Zn-CO₂ battery exhibited a superior maximum power density of 6.48 mW∙cm^–2 at a discharge current density of 16 mA∙cm^–2 and remarkable rechargeable durability for 60 h, outperforming most of the reported catalysts in the literature. This work enhances CO₂-C₂ conversion by tuning the eCO₂RR activity and selectivity of Cu-based materials, unravels the reaction mechanism at the molecular level, and provides new insights for promoting C₂ products in eCO₂RR through surface functionalization with organic molecules.

Key words: CO₂ reduction, CO―CHO coupling, Organic functionalization, In situ Raman, C₂ product, Zn-CO₂ battery

项东, 李坤振, 苗康华, 龙冉, 熊宇杰, 康雄武. 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]. 物理化学学报, 2024, 40(8), 2308027. doi: 10.3866/PKU.WHXB202308027

Dong Xiang, Kunzhen Li, Kanghua Miao, Ran Long, Yujie Xiong, Xiongwu Kang. Amine-Functionalized Copper Catalysts: Hydrogen Bonding Mediated Electrochemical CO₂ Reduction to C₂ Products and Superior Rechargeable Zn-CO₂ Battery Performance[J]. Acta Phys. -Chim. Sin. 2024, 40(8), 2308027. doi: 10.3866/PKU.WHXB202308027

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202308027

https://www.whxb.pku.edu.cn/CN/Y2024/V40/I8/2308027

图/表 5

参考文献 57

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