Citation: Tingting Gong, Zhen Liu, Wen Jin, Jiamei Li, Min Wang, Luhua Jiang. Anions-mediated interfacial-water regulation boosts C2+ selectivity for CO2 electroreduction over Cu-based catalysts[J]. Chinese Journal of Structural Chemistry, ;2026, 45(9): 100967. doi: 10.1016/j.cjsc.2026.100967 shu

Anions-mediated interfacial-water regulation boosts C2+ selectivity for CO2 electroreduction over Cu-based catalysts

The electrochemical CO2 reduction reaction (CO2RR) offers a promising strategy to produce high-value-added C2+ products. Cu-based catalysts enable C-C coupling but suffer from low C2+ selectivity. Although electronic/structural engineering and cation effects have been widely studied, the role of anions in tuning interfacial water structure and CO2RR pathways remains insufficiently understood. Herein, a series of low-concentration anions were introduced into 1 M KOH to regulate the interfacial water environment over reconstructed CuO. By combining in-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) and electrochemical impedance spectroscopy, it is revealed that low-concentration anions in 1 M KOH increase the proportion of strong interfacial-water structure in the order of F- > Cl- > Br- > NO3-. Moreover, the moderate strong interfacial-water structure can accelerate *H transfer and promote *CO hydrogenation to *COH, thus favoring asymmetric C-C coupling to produce C2+ products. However, excessively stable interfacial water structure in F--containing electrolyte induces enhanced *H coverage and dominant H2 evolution. A volcano-type relationship is thus observed between C2+ selectivity and the proportion of strongly hydrogen-bonded water. This work emphasizes anion-mediated interfacial water regulation as an effective strategy to enhance C2+ selectivity for CO2RR.
- CO2 electrochemical reduction,
- Cu-based catalysts,
- Interfacial water,
- Anions,
- In-situ ATR-SEIRAS
1. [1]
  Lewa Zhang , Quan Zhou , Chenyuan Zhu , Yizhao Li , Shihan Zhang , Fan Dong . Rational Cu-based catalyst and electrolyte design for electrochemical nitrate reduction towards ammonia. Chinese Chemical Letters, 2026, 37(8): 112325-. doi: 10.1016/j.cclet.2025.112325
2. [2]
  Yixin Zhang , Ting Wang , Jixiang Zhang , Pengyu Lu , Neng Shi , Liqiang Zhang , Weiran Zhu , Nongyue He . Formation mechanism for stable system of nanoparticle/protein corona and phospholipid membrane. Chinese Chemical Letters, 2024, 35(4): 108619-. doi: 10.1016/j.cclet.2023.108619
3. [3]
  Yufei Jia , Fei Li , Ke Fan . Surface reconstruction of Cu-based bimetallic catalysts for electrochemical CO2 reduction. Chinese Journal of Structural Chemistry, 2024, 43(3): 100255-100255. doi: 10.1016/j.cjsc.2024.100255
4. [4]
  Muhammad Humayun , Mohamed Bououdina , Abbas Khan , Sajjad Ali , Chundong Wang . Designing single atom catalysts for exceptional electrochemical CO2 reduction. Chinese Journal of Structural Chemistry, 2024, 43(1): 100193-100193. doi: 10.1016/j.cjsc.2023.100193
5. [5]
  Xueyang Zhao , Bangwei Deng , Hongtao Xie , Yizhao Li , Qingqing Ye , Fan Dong . Recent process in developing advanced heterogeneous diatomic-site metal catalysts for electrochemical CO₂ reduction. Chinese Chemical Letters, 2024, 35(7): 109139-. doi: 10.1016/j.cclet.2023.109139
6. [6]
  Tinghui Yang , Min Kuang , Jianping Yang . Mesoporous CuCe dual-metal catalysts for efficient electrochemical reduction of CO2 to methane. Chinese Journal of Structural Chemistry, 2024, 43(8): 100350-100350. doi: 10.1016/j.cjsc.2024.100350
7. [7]
  Zekun Zhang , Shiji Li , Qian Zhang , Shanshan Li , Liu Yang , Wei Yan , Hao Xu . Further study of CO₂ electrochemical reduction to gas products on Cu: Influence of the electrolyte. Chinese Chemical Letters, 2025, 36(9): 110742-. doi: 10.1016/j.cclet.2024.110742
8. [8]
  Lihui Ou , Zhancheng Liu , Dai-Huo Liu , Zhi Zhang . Cl-adsorbed Cu(111)/H₂O interface selectively realizes electrochemical CO₂ reduction towards C₂H₄ product: Mechanistic understanding. Chinese Chemical Letters, 2026, 37(2): 111920-. doi: 10.1016/j.cclet.2025.111920
9. [9]
  Ping Wang , Tianbao Zhang , Zhenxing Li . Reconstruction mechanism of Cu surface in CO2 reduction process. Chinese Journal of Structural Chemistry, 2024, 43(8): 100328-100328. doi: 10.1016/j.cjsc.2024.100328
10. [10]
  Yinglian LI , Chengcheng ZHANG , Xinyu ZHANG , Xinyi WANG . Spin crossover in [Co(pytpy)₂]²⁺ complexes modified by organosulfonate anions. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1162-1172. doi: 10.11862/CJIC.20240087
11. [11]
  Hong-Rui Li , Xia Kang , Rui Gao , Miao-Miao Shi , Bo Bi , Ze-Yu Chen , Jun-Min Yan . Interfacial interactions of Cu/MnOOH enhance ammonia synthesis from electrochemical nitrate reduction. Chinese Chemical Letters, 2025, 36(2): 109958-. doi: 10.1016/j.cclet.2024.109958
12. [12]
  Yuxiang Zhang , Jia Zhao , Sen Lin . Nitrogen doping retrofits the coordination environment of copper single-atom catalysts for deep CO2 reduction. Chinese Journal of Structural Chemistry, 2024, 43(11): 100415-100415. doi: 10.1016/j.cjsc.2024.100415
13. [13]
  Xiangyu Chen , Aihao Xu , Dong Wei , Fang Huang , Junjie Ma , Huibing He , Jing Xu . Atomic cerium-doped CuO_x catalysts for efficient electrocatalytic CO₂ reduction to CH₄. Chinese Chemical Letters, 2025, 36(1): 110175-. doi: 10.1016/j.cclet.2024.110175
14. [14]
  Weibin Shen , Jie Liu , Gongyu Wen , Shuai Li , Binhui Yu , Shuangyu Song , Bojie Gong , Rongyang Zhang , Shibao Liu , Hongpeng Wang , Yao Wang , Yujing Liu , Huadong Yuan , Jianming Luo , Shihui Zou , Xinyong Tao , Jianwei Nai . Formation of FeNi-based nanowire-assembled superstructures with tunable anions for electrocatalytic oxygen evolution reaction. Chinese Chemical Letters, 2025, 36(7): 110184-. doi: 10.1016/j.cclet.2024.110184
15. [15]
  Jiawei Hu , Qiao-Yan Qi , Qingxuan Tang , Wen-Zhuang Wang , Zhan-Ting Li , Jia Tian . Water-dispersible cyclen-based porous organic polymers for CO₂ direct air capture and photoreduction. Chinese Chemical Letters, 2026, 37(9): 112222-. doi: 10.1016/j.cclet.2025.112222
16. [16]
  Yan Zhao , Zhenming Tian , Qisen Jia , Ting Yao , Jiashu Li , Yanan Wang , Xuejing Cui , Jing Liu , Xin Chen , Luhua Jiang . Crystal orientation dependent charge transfer dynamics and interfacial water configuration boosting photoelectrocatalytic water oxidation to H2O2. Chinese Journal of Structural Chemistry, 2025, 44(7): 100619-100619. doi: 10.1016/j.cjsc.2025.100619
17. [17]
  Qin Cheng , Ming Huang , Qingqing Ye , Bangwei Deng , Fan Dong . Indium-based electrocatalysts for CO₂ reduction to C1 products. Chinese Chemical Letters, 2024, 35(6): 109112-. doi: 10.1016/j.cclet.2023.109112
18. [18]
  Di Wang , Qing-Song Chen , Yi-Ran Lin , Yun-Xin Hou , Wei Han , Juan Yang , Xin Li , Zhen-Hai Wen . Tuning strategies and electrolyzer design for Bi-based nanomaterials towards efficient CO2 reduction to formic acid. Chinese Journal of Structural Chemistry, 2024, 43(8): 100346-100346. doi: 10.1016/j.cjsc.2024.100346
19. [19]
  Xiuzheng Deng , Yi Ke , Jiawen Ding , Yingtang Zhou , Hui Huang , Qian Liang , Zhenhui Kang . Construction of ZnO@CDs@Co₃O₄ sandwich heterostructure with multi-interfacial electron-transfer toward enhanced photocatalytic CO₂ reduction. Chinese Chemical Letters, 2024, 35(4): 109064-. doi: 10.1016/j.cclet.2023.109064
20. [20]
  Juan Zhu , Jingxiang Xia , Wei Luo . Oxophilic support mediated interfacial water reconstruction on RuO2 for high-efficiency proton exchange membrane electrolysis. Chinese Journal of Structural Chemistry, 2026, 45(4): 100857-100857. doi: 10.1016/j.cjsc.2025.100857

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