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Acidic electroreduction CO2 to formic acid via interfacial modification of Bi nanoparticles at industrial-level current

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Abstract

Electrocatalytic CO2 reduction reaction (CO2RR) in acidic media is a promising approach to overcome the unavoidable formation of carbonates in alkaline or neutral electrolytes. However, the proton-rich environment near the catalyst surface favors hydrogen evolution reactions (HER), leading to lower energy efficiency of the desired products, especially in industrial-level current densities. Here, quaternary ammonium cationic surfactant (cetyltrimethylammonium bromide (CTAB)) was introduced into acidic electrolyte to modulate the interfacial microenvironment, which greatly enhanced CO2 electroreduction to formic acid (HCOOH) at the Bi/C nanoparticles electrode. Using a Bi/C nanoparticles electrode with CTAB added, constant production of formic acid was enabled with a cathodic energy efficiency of > 40% and maximum FEHCOOH (FE = Faradaic efficiency) of 86.2% at −400 mA·cm−2 over 24 h. Combined with in-situ attenuated total reflection Fourier transform infrared spectroscopy, the concentration of *OCHO intermediates significantly increased after CTAB modification, confirming that the hydrophobic interface microenvironment formed by dynamic adsorption of positively charged long alkyl chains on Bi/C nanoparticle electrodes inhibited HER and improved the selectivity of CO2RR to HCOOH.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 52072197, 22302108, 21971132, and 52272222), Youth Innovation and Technology Foundation of Shandong Higher Education Institutions, China (No. 2023KJ313), Outstanding Youth Foundation of Shandong Province, China (No. ZR2019JQ14), Major Scientific and Technological Innovation Project (No. 2019JZZY020405), Major Basic Research Program of Natural Science Foundation of Shandong Province (No. ZR2020ZD09), Natural Science Foundation of Qingdao (No. 23-2-1-12-zyyd-jch), and Qingdao Postdoctoral Researcher Applied Research Project (No. QDBSH20220202043).

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Authors and Affiliations

  1. Key Laboratory of Eco-Chemical Engineering, International Science and Technology Cooperation Base of Eco-Chemical Engineering and Green Manufacturing, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao, 266042, China

    Tian Dong, Hongdong Li, Zhenhui Wang, Yanling Geng, Rui Chang, Xiaofeng Tian, Jianping Lai, Shouhua Feng & Lei Wang

  2. Shandong Engineering Research Center for Marine Environment Corrosion and Safety Protection, College of Environment and Safety Engineering, Qingdao University of Science and Technology, Qingdao, 266042, China

    Lei Wang

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  1. Tian Dong
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  2. Hongdong Li
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  9. Lei Wang
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Correspondence to Hongdong Li or Lei Wang.

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Dong, T., Li, H., Wang, Z. et al. Acidic electroreduction CO2 to formic acid via interfacial modification of Bi nanoparticles at industrial-level current. Nano Res. (2024). https://doi.org/10.1007/s12274-024-6536-2

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