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Boosting the direct conversion of NH4HCO3 electrolyte to syngas on Ag/Zn zeolitic imidazolate framework derived nitrogen-carbon skeleton

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Abstract

The electrochemical reduction of NH4HCO3 to syngas can bypass the high energy consumption of high-purity CO2 release and compression after the ammonia-based CO2 capture process. This technology has broad prospects in industrial applications and carbon neutrality. A zeolitic imidazolate framework-8 precursor was introduced with different Ag contents via colloid chemical synthesis. This material was carbonized at 1000 °C to obtain AgZn zeolitic imidazolate framework derived nitrogen carbon catalysts, which were used for the first time for boosting the direct conversion of NH4HCO3 electrolyte to syngas. The AgZn zeolitic imidazolate framework derived nitrogen carbon catalyst with a Ag/Zn ratio of 0.5:1 achieved the highest CO Faradaic efficiency of 52.0% with a current density of 1.15 mA·cm−2 at −0.5 V, a H2/CO ratio of 1–2 (−0.5 to −0.7 V), and a stable catalytic activity of more than 6 h. Its activity is comparable to that of the CO2-saturated NH4HCO3 electrolyte. The highly discrete Ag-Nx and Zn-Nx nodes may have combined catalytic effects in the catalysts synthesized by appropriate Ag doping and sufficient carbonization. These nodes could increase active sites of catalysts, which is conducive to the transport and adsorption of reactant CO2 and the stability of *COOH intermediate, thus can improve the selectivity and catalytic activity of CO.

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Acknowledgements

This work was supported by the 2022 Heilongjiang Province’s “Emission and carbon neutrality” the open competition mechanism to select the best candidate project (Adsorption-type compression of carbon dioxide energy storage key technology research and demonstration: Grant No. 2022ZXJ09C01).

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Authors and Affiliations

  1. Institute of Combustion Engineering, School of Energy Science and Engineering, Harbin Institute of Technology, Harbin, 150001, China

    Huiyi Li, Jianmin Gao, Qian Du & Yu Zhang

  2. MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001, China

    Jingjing Shan & Zhijiang Wang

  3. Harbin Bolier Co., Ltd., Harbin, 150040, China

    Xin Guo

  4. Department of Environmental Engineering, Shanxi University, Taiyuan, 030006, China

    Shaohua Wu

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  1. Huiyi Li
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  5. Yu Zhang
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Correspondence to Jianmin Gao.

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Li, H., Gao, J., Shan, J. et al. Boosting the direct conversion of NH4HCO3 electrolyte to syngas on Ag/Zn zeolitic imidazolate framework derived nitrogen-carbon skeleton. Front. Chem. Sci. Eng. 17, 1196–1207 (2023). https://doi.org/10.1007/s11705-022-2289-1

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