吸电子配体修饰促进低浓度CO2电解

doi:10.1016/S1872-2067(26)65151-0

催化学报 ›› 2026, Vol. 90: 210-219.DOI: 10.1016/S1872-2067(26)65151-0

吸电子配体修饰促进低浓度CO₂电解

温晓娟^a^,^b, 魏鹏飞^a, 姜一元^a, 宋延鹏^a, 王含羽^a^,^b, 薛靖^a^,^b, 刘天夫^a^,^b^,^*(), 高敦峰^a^,^b^,^*(), 汪国雄^a^,^c, 包信和^a^,^b^,^c

^a 中国科学院大连化学物理研究所, 能源催化转化全国重点实验室, 辽宁大连 116023
^b 中国科学院大学, 北京 100049
^c 复旦大学化学系, 未来能源高等研究院, 上海市资源电热转化与循环重点实验室, 能源材料化学协同创新中心, 多孔材料与分离转化全国重点实验室, 上海 200438

收稿日期:2026-01-20 接受日期:2026-02-25 出版日期:2026-11-18 发布日期:2026-09-09
通讯作者: *电子信箱: ltianfu@dicp.ac.cn (刘天夫),
dfgao@dicp.ac.cn (高敦峰).
基金资助:
国家重点研发计划(2022YFA1504600);国家自然科学基金(22372171);国家自然科学基金(22472176);国家自然科学基金(22494711);国家自然科学基金(22002155);国家自然科学基金(22125205);国家自然科学基金(22321002);中国科学院战略性先导科技专项(XDB0600200);中央高校基本科研业务费专项资金(20720220008);中国科学院洁净能源创新研究院-榆林学院联合基金(YLU-DNL fund2025012);辽宁滨海实验室(LBLD-2024-02);辽宁省兴辽英才计划(XLYC2203178);大连市杰出青年科技人才计划(2024RJ003);大连化学物理研究所自主部署项目(DICP I202504);面向二氧化碳的光子科学建制化研究平台(JZHKYPT-2021-07)

Promoting dilute CO₂ electrolysis with electron-withdrawing ligand modification

Xiaojuan Wen^a^,^b, Pengfei Wei^a, Yiyuan Jiang^a, Yanpeng Song^a, Hanyu Wang^a^,^b, Jing Xue^a^,^b, Tianfu Liu^a^,^b^,^*(), Dunfeng Gao^a^,^b^,^*(), Guoxiong Wang^a^,^c, Xinhe Bao^a^,^b^,^c

^a State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China
^b University of Chinese Academy of Sciences, Beijing 100049, China
^c Department of Chemistry, Advanced Institute of Future Energy, Shanghai Key Laboratory of Electrochemical and Thermochemical Conversion for Resources Recycling, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), State Key Laboratory of Porous Materials for Separation and Conversion, Fudan University, Shanghai 200438, China

Received:2026-01-20 Accepted:2026-02-25 Online:2026-11-18 Published:2026-09-09
Contact: *E-mail:ltianfu@dicp.ac.cn(T. Liu),dfgao@dicp.ac.cn(D. Gao).
Supported by:
National Key R&D Program of China(2022YFA1504600);National Natural Science Foundation of China(22372171);National Natural Science Foundation of China(22472176);National Natural Science Foundation of China(22494711);National Natural Science Foundation of China(22002155);National Natural Science Foundation of China(22125205);National Natural Science Foundation of China(22321002);Strategic Priority Research Program of the Chinese Academy of Sciences(XDB0600200);Fundamental Research Funds for the Central Universities(20720220008);Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(YLU-DNL fund2025012);Liaoning Binhai Laboratory(LBLD-2024-02);Liaoning Revitalization Talents Program(XLYC2203178);Dalian Outstanding Young Scientist Foundation(2024RJ003);Dalian Institute of Chemical Physics(DICP I202504);Photon Science Center for Carbon Neutrality(JZHKYPT-2021-07)

摘要/Abstract

摘要：

利用可再生能源将二氧化碳(CO₂)电解转化为高值燃料和化学品是应对气候变化、缓解能源危机的重要途径. 然而, CO₂分子中C=O键解离能高、多电子还原过程动力学缓慢, 实现高活性、高选择性的CO₂电解仍面临巨大挑战. 此外, 工业烟道气中CO₂浓度低, 分离纯化成本高, 极大制约了该技术的实际应用. 与高纯CO₂电解相比, 低浓度CO₂电解的反应动力学更为迟缓. 尽管研究者已开发出多种可高效转化低浓度CO₂的催化剂, 并在一氧化碳(CO)、甲酸盐等C₁产物上实现了较高法拉第效率, 但低浓度CO₂电解高选择性制多碳(C₂₊)产物仍十分困难. 这是因为C₂₊产物的生成涉及C-C偶联步骤, 对中间体浓度与反应路径更为敏感. 因此, 在低浓度CO₂条件下有效富集*CO等关键C₁中间体、促进C-C偶联、提升反应动力学是实现高效C₂₊产物合成的关键.

本文选用对苯二甲酸(BDC)类配体, 其可通过苯环与CO₂之间形成π…C(CO₂)相互作用, 促进CO₂吸附, 对低浓度CO₂的高效电解转化尤为关键. 通过溶剂热法分别以BDC、氟取代BDC(BDC-F)及氨基取代BDC(BDC-NH₂)为配体, 合成了三种Cu-BDC-X金属有机框架(MOFs)材料前驱体. 扫描电镜、X射线衍射、高角环形暗场扫描透射电镜、X射线光电子能谱(XPS)及X-射线吸收谱(XAS)结果表明, Cu-BDC, Cu-BDC-F及Cu-BDC-NH₂均成功制备, 而Cu以Cu(II)形式存在并形成Cu-O配位结构. 在零间隙膜电极(MEA)电解器中系统评估了三种催化剂的CO₂电解性能. 在高纯CO₂条件下, Cu-BDC-F表现出更强的C-C偶联能力, C₂₊法拉第效率(C₂₊ FE)最高可达64.3%. 进一步在模拟工业烟气(15%低浓度CO₂)条件下测试, 通过加压可显著提升低浓度CO₂电解性能. 在0.4 MPa下, Cu-BDC-F在150 mA cm⁻²时C₂₊ FE达到67.9%, 最大C₂₊分电流密度为130 mA cm⁻², 优于相同压力下的Cu-BDC与Cu-BDC-NH₂, 且Cu-BDC-F表现出更低的电解电压. 反应后的催化剂结构表征表明, Cu-BDC-X MOFs在电解过程中发生显著的电化学重构, 由Cu-MOF转变为BDC-X配体修饰的Cu纳米颗粒. 准原位XPS及工况XAS结果共同表明, 在反应过程中Cu²⁺被还原为金属Cu. 膜电极工况拉曼测试和CO溶出伏安测试表明, 相比于Cu-BDC和Cu-BDC-NH₂, Cu-BDC-F对CO吸附更强. 这说明吸电子-F基团的修饰能够增强中间体*CO在Cu上的吸附. 密度泛函理论计算表明, Cu-BDC-F上*COCOH中间体形成能垒最低, 且后续加氢步骤热力学更有利. 晶体轨道哈密顿布居计算表明, BDC-F体系中Cu与*COCOH间Cu−C成键作用更强, 能有效稳定关键中间体、降低C-C偶联能垒.

综上, 本研究通过对BDC配体进行氟取代, 可精准调控Cu位点的电子结构与中间体吸附强度, 显著提升低浓度CO₂电解制C₂₊产物的活性与选择性, 为设计高效MOF衍生的低浓度CO₂电解催化剂提供了可行策略.

关键词: 低浓度CO₂电解, 吸电子, 配体修饰, 选择性, 多碳产物

Abstract:

The efficient production of valuable multicarbon (C₂₊) chemicals via direct electrolysis of dilute CO₂ derived from industrial flue gases is a promising route to close the carbon cycle, but is not yet practical owing to insufficient electrocatalytic performance limited by sluggish reaction kinetics at low CO₂ concentrations. Herein, we develop BDC-X (where BDC represents 1,4-benzenedicarboxylic acid and X represents H, F, and NH₂) ligand-modified Cu nanoparticle catalysts via in-situ electrochemical reconstruction of metal organic frameworks precursors, for dilute CO₂ electrolysis to C₂₊ products. The -X functional groups anchored on the BDC can be deemed as site-specific regulators for modulating the electronic structure of Cu nanoparticles. The BDC-F ligand with strong electron-withdrawing ability exhibits the most remarkable promoting effect, with an impressive C₂₊ Faradaic efficiency of 67.9% and a maximum C₂₊ partial current density of 130 mA cm⁻² under a 15% CO₂ feed at 0.4 MPa. Combined experimental and theoretical investigations indicate that the reduced electron density of Cu active sites induced by the electron-withdrawing -F group improves *CO adsorption and lowers energy barrier for C−C coupling, thus resulting in improved C₂₊ selectivity.

Key words: Dilute CO₂ electrolysis, Electron-withdrawing, Ligand modification, Selectivity, Multicarbon products

温晓娟, 魏鹏飞, 姜一元, 宋延鹏, 王含羽, 薛靖, 刘天夫, 高敦峰, 汪国雄, 包信和. 吸电子配体修饰促进低浓度CO₂电解[J]. 催化学报, 2026, 90: 210-219.

Xiaojuan Wen, Pengfei Wei, Yiyuan Jiang, Yanpeng Song, Hanyu Wang, Jing Xue, Tianfu Liu, Dunfeng Gao, Guoxiong Wang, Xinhe Bao. Promoting dilute CO₂ electrolysis with electron-withdrawing ligand modification[J]. Chinese Journal of Catalysis, 2026, 90: 210-219.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65151-0

https://www.cjcatal.com/CN/Y2026/V90/I11/210

图/表 4

Fig. 1. (a) Schematic illustration of the preparation of Cu-BDC-X MOFs. (b) SEM image of Cu-BDC. (c) FTIR spectra of Cu-BDC-X. C 1s (d) and Cu 2p (e) XPS spectra of Cu-BDC-X. Cu K-edge (f) XANES and (g) R-space EXAFS spectra for Cu-BDC-X, CuO, and Cu foil.

Fig. 2. FE and cell voltage as a function of applied current density over Cu-BDC (a), Cu-BDC-F (b), and Cu-BDC-NH2 (c) measured under high-purity CO2 feed. (d) Schematic of the production of chemicals and fuels via direct flue gas electrolysis. (e) C2+ FE on Cu-BDC-F at 150 mA cm-2 at different CO2 pressures. (f) FE and cell voltage as a function of applied current density over Cu-BDC-F measured under 0.4 MPa dilute CO2 (15%) feed. (g) C2+ FE as a function of applied current density over Cu-BDC, Cu-BDC-F, and Cu-BDC-NH2 measured under 0.4 MPa dilute CO2 (15%) feed. (h) Stability of Cu-BDC-F at 150 mA cm-2 under 0.4 MPa dilute CO2 (15%) feed.

Fig. 3. (a) FTIR spectra of Cu-BDC-X after CO2 electrolysis. (b) HRTEM image of the Cu-BDC-F electrode after CO2 electrolysis. (c) Quasi in-situ XPS spectra of Cu LMM of Cu-BDC-X after CO2 electrolysis at 250 mA cm-2. Operando Cu K-edge XANES (d) and EXAFS (e) spectra of Cu-BDC-F measured in a MEA cell. (f) Cu K-edge XANES spectra of Cu-BDC-X during CO2 electrolysis at 200 mA cm-2.

Fig. 4. Operando Raman spectra of Cu-BDC-F (a) and Cu-BDC (b) in a MEA cell at different applied current densities. (c) CO stripping experiments on Cu-BDC-X after CO2 electrolysis, with a scan rate of 50 mV s-1. (d) Gibbs free energy barriers for the formation of C2H4 on Cu-BDC-X during CO2 electrolysis, including the optimized structures of 2*CO, *COCOH, *COH-COH, *CCOH, *CHCOH, *CHCHOH, *CH2CHOH and *CH2CH on the Cu-BDC and Cu-BDC-F during CO2 electrolysis. Projected COHP (pCOHP) curves for the Cu-C1 (C1 originates from the carbon of the -CO fragment in *COCOH) and Cu-C2 (C2 originates from the carbon of the -COH fragment in *COCOH) interactions for the adsorbate carbon atoms in *COCOH and their coordinating Cu sites in Cu-BDC (e) and Cu-BDC-F (f).

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吸电子配体修饰促进低浓度CO₂电解

Promoting dilute CO₂ electrolysis with electron-withdrawing ligand modification

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