铜基催化剂电还原二氧化碳选择性的调控策略

doi:10.16085/j.issn.1000-6613.2023-0397

化工进展 ›› 2023, Vol. 42 ›› Issue (8): 4043-4057.DOI: 10.16085/j.issn.1000-6613.2023-0397

铜基催化剂电还原二氧化碳选择性的调控策略

王耀刚¹^,²^,³^,⁴(), 韩子姗¹^,²^,³^,⁴, 高嘉辰¹^,²^,³^,⁴, 王新宇¹^,²^,³^,⁴, 李思琪¹^,²^,³^,⁴, 杨全红¹^,²^,³^,⁴, 翁哲¹^,²^,³^,⁴()

^1.天津市先进碳与电化学储能重点实验室，天津 300072
^2.国家储能技术产教融合创新平台，天津 300072
^3.物质绿色创造与制造海河实验室，天津 300192
^4.天津化学化工协同创新中心，天津 300072

收稿日期:2023-03-15 修回日期:2023-07-27 出版日期:2023-08-15 发布日期:2023-09-19
通讯作者: 翁哲
作者简介:王耀刚（1996—），男，硕士研究生，研究方向为电催化二氧化碳还原催化剂的设计。E-mail：e158263980@163.com。
基金资助:
国家自然科学基金(51972223);天津市自然科学基金(20JCYBJC01550)

Strategies for regulating product selectivity of copper-based catalysts in electrochemical CO₂ reduction

WANG Yaogang¹^,²^,³^,⁴(), HAN Zishan¹^,²^,³^,⁴, GAO Jiachen¹^,²^,³^,⁴, WANG Xinyu¹^,²^,³^,⁴, LI Siqi¹^,²^,³^,⁴, YANG Quanhong¹^,²^,³^,⁴, WENG Zhe¹^,²^,³^,⁴()

^1.Nanoyang Group, Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage, Tianjin 30072, China
^2.National Industry-Education Integration Platform of Energy Storage, Tianjin 300072, China
^3.Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300192, China
^4.Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin 300072, China

Received:2023-03-15 Revised:2023-07-27 Online:2023-08-15 Published:2023-09-19
Contact: WENG Zhe

摘要/Abstract

摘要：

在水系电解液中利用电能直接将CO₂还原成基础化学品为CO₂资源化利用提供了一种绿色可行的策略。铜是唯一能够高效地将CO₂还原成C₂₊产物的金属催化剂，然而其催化产物多达16种，产物的多样性严重增加了后期产物分离的成本并大幅降低了整个电催化二氧化碳还原(eCO₂RR)系统的能量转换效率，是eCO₂RR走向工业化生产的一个重要瓶颈，因此对铜基催化剂进行合理的调控，以提高其对单一产物的选择性一直是研究的热点问题。经过30余年的发展，铜基催化剂的研究已经取得了巨大的进展，回溯近期铜基催化剂电催化CO₂还原领域的研究历程，本文综述了电催化二氧化碳还原的反应原理、反应路径和针对不同产物的调控策略，着重总结了提高铜基催化剂对单一产物选择性的设计策略和设计方法，最后展望了铜基催化剂面临的挑战和未来的发展方向。

关键词: 电化学, 二氧化碳, 还原, 铜基催化剂, 产物选择性

Abstract:

Directly converting CO₂ into valuable chemicals in aqueous electrolytes using renewable electric energy provides a sustainable strategy for the CO₂ utilization. Copper is the only metal catalyst that can efficiently produce C₂₊ products at appreciable rates. However, the diverse distribution of products (more than 16 types) in the electrocatalytic CO₂ reduction reaction (eCO₂RR) significantly increases the cost of product separation and weakens the energy conversion efficiency of the system, thus hindering the industrialization of eCO₂RR. Therefore, it is of great importance to rationally design copper-based catalysts that exhibit high selectivity toward a specific product. During more than 30 years of development, the research on copper-based catalysts has made great progress. This review provided an overview of the reaction mechanisms, reaction paths and regulation strategies of eCO₂RR using copper-based catalysts based on recent studies. The regulation strategies for achieving various products were comprehensively summarized. Finally, challenges and future directions for copper-based catalysts were discussed.

Key words: electrochemistry, carbon dioxide, reduction, copper-based catalysts, product selectivity

中图分类号:

O646.5

王耀刚, 韩子姗, 高嘉辰, 王新宇, 李思琪, 杨全红, 翁哲. 铜基催化剂电还原二氧化碳选择性的调控策略[J]. 化工进展, 2023, 42(8): 4043-4057.

WANG Yaogang, HAN Zishan, GAO Jiachen, WANG Xinyu, LI Siqi, YANG Quanhong, WENG Zhe. Strategies for regulating product selectivity of copper-based catalysts in electrochemical CO₂ reduction[J]. Chemical Industry and Engineering Progress, 2023, 42(8): 4043-4057.

图/表 12

图1 铜基催化剂发展历程[14-21]

图2 H-cell示意图[33]

图3 eCO2RR不同产物路径[23]

图4 卟啉铜反应机理示意图(a)[44]；金属铜催化剂表面在有/无EDTMPA吸附时的产物选择性(b)；金属铜催化剂在EDTMPA作用下的稳定性测试(c)[46]

图5 不同*CO覆盖度下两个相互竞争的反应（*CO质子化到*CHO，以及C—C偶联）的反应能垒(a)；电还原N2和CO2混合气体的反应示意图(b)[40]；Cu/PTFE在不同电位下的产物选择性(c)；CuAu催化剂在不同金含量下电流密度与产物选择性的关系(d)[48]

图6 存在eCO2RR或HER中间体的铜簇的伍尔夫结构(a)；富(100)晶面铜基催化剂在不同电位下的产物选择性(b)[43]；OH-吸附实验表征晶面占比(c)；在不同(100)晶面占比下产物的选择性(d)[49-50]

图7 聚合物分子在气体扩散电极中的作用示意图(a)[51]；Cu在不同电位下的产物选择性(b)；Cu-PANI在不同电位下的产物选择性(c)[52]

图8 OD-Cu催化剂在eCO2RR条件下的XANES谱图(a)；制备得到的催化剂与参考样品的EXAFS光谱比较(b)；原位条件下催化剂的EXAFS谱图(c)[48]；多孔球在eCO2RR条件下的原位拉曼光谱图(d)；实心球在eCO2RR条件下的原位拉曼光谱图(e)[49]

图9 Cu(a)、Cu4Zn(b)在不同电位下的产物选择性[56]；OD-Cu NW(c)、Cu(Ag-20)20(d)在不同电位下的产物选择性[39]；Ag/Cu上*HCCOH、*CCH（乙烯路径）和*HCCHOH（乙醇路径）的形成能(e) 在Cu和Ag/Cu催化剂上乙烯和乙醇路径的反应能垒计算(f)[57]

图10 Cu/Cu-MnO2/Cu-CeO2表面的水解离能和氢吸附能(a)；Ce(OH) x /Cu/PTFE在不同电位下的原位XAS谱图(b)；Ce(OH) x /Cu/PTFE和Cu在-0.7V(vs. RHE)下的产物分布(c)；不同掺杂剂下HOCCH*自由能与H吸附自由能之间的关系图(d)[58]；不同Pd掺杂构型下HOCCH*的氢化反应自由能，1[Pd]、2[Pd]、3[Pd]、4[Pd]是指表面Pd含量分别为1/16、1/8、3/16、1/4(e)；不同电位下醇类产物的偏电流密度(f)[59]

图11 双硫空位的CuS x 将CO2转化为正丙醇的反应能垒计算(a)；CuS x 在不同电位下的产物选择性(b)[60]；Ag-Ru-Cu催化剂在不同电流密度下的产物选择性(c)[61]

图12 限域效应示意图(a)；实心球/空心球Ⅰ/空心球Ⅱ/碎片在-0.56 V vs. RHE电位下的产物分布(b)[40]；电沉积、热处理、CO2RR反应后三个阶段的材料对应的SEM和TEM图像(c)[62]

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铜基催化剂电还原二氧化碳选择性的调控策略

Strategies for regulating product selectivity of copper-based catalysts in electrochemical CO₂ reduction

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铜基催化剂电还原二氧化碳选择性的调控策略

Strategies for regulating product selectivity of copper-based catalysts in electrochemical CO2 reduction

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Strategies for regulating product selectivity of copper-based catalysts in electrochemical CO₂ reduction