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In situ embedded bismuth nanoparticles among highly porous carbon fibers for efficient carbon dioxide reduction

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Abstract

Electrocatalysis provides an optimal approach for the conversion of carbon dioxide (CO2) into high-value chemicals, thereby presenting a promising avenue toward achieve carbon neutrality. However, addressing the selectivity and stability challenges of metal catalysts in electrolytic reduction remains a daunting task. In this study, the electrospinning method is employed to fabricate porous carbon nanofibers loaded with bismuth nanoparticles with the help of in situ pyrolysis. The porous carbon nanofibers as conductive support would facilitate the dispersion of bismuth active sites while inhibiting their aggregation and promoting the mass transfer, thus enhancing their electrocatalytic activity and stability. Additionally, nitrogen doping induces electron delocalization in bismuth atoms through metal-support interactions, thus enabling efficient adsorption of intermediates for improving selectivity based on the theoretical calculation. Consequently, Bi@PCNF-500 exhibits the exceptional selectivity and stability across a wide range of potential windows. Notably, its faradaic efficiency (FE) of formate reaches 92.7% in H-cell and 94.9% in flow cell, respectively, with good electrocatalytic stability. The in situ characterization and theoretical calculations elucidate the plausible reaction mechanism to obtain basic rules for designing efficient electrocatalyst.

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摘要

电催化还原是将二氧化碳转化为高价值化学品的理想途径之一，为实现碳中和提供了富有前景的方式。然而，金属催化剂的选择性低和稳定性差是限制电催化转化性能的瓶颈。本研究采用静电纺丝方法与原位热解协同策略制备了负载铋（Bi）纳米颗粒的多孔碳纳米纤维。其中，多孔碳纳米纤维作为导电载体，可有效抑制铋纳米颗粒的聚集，促进活性位点的分散和传质过程，从而实现电催化活性和稳定性的增强。结合理论计算表明，氮掺杂碳载体-金属相互作用可诱导铋原子中的电子离域，从而增强中间体的高效吸附，提高电催化选择性。因此，该Bi@PCNF-500电催剂在宽电位窗口范围内表现出了优异的选择性和稳定性。在H池和流动池中，生成甲酸的法拉第效率可达到92.7和94.9%，且具有良好的电催化稳定性。结合原位表征和理论计算阐明的电催化机理为设计高效电催化剂提供了理论支撑。

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 22175108 and 22379086), the Natural Science Foundation of Shandong Province (Nos.ZR2020JQ09 and ZR2022ZD27) and Taishan Scholars Program of Shandong Province (tstp20221105). The authors also acknowledge the assistance of the Analytical Center for Structural Constituent and Physical Property of Core Facilities Sharing Platform, Shandong University.

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  1. Key Laboratory for Colloid and Interface Chemistry (Ministry of Education), School of Chemistry and Chemical Engineering, Shandong University, Jinan, 250100, China

    Wei-Jian Guo, Ao Zhou, Wen-Wen Cai & Jin-Tao Zhang

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Guo, WJ., Zhou, A., Cai, WW. et al. In situ embedded bismuth nanoparticles among highly porous carbon fibers for efficient carbon dioxide reduction. Rare Met. (2024). https://doi.org/10.1007/s12598-024-02803-9

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