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Controlling selectivities in CO2 reduction through mechanistic understanding

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  • Xiang Wang

    (Pacific Northwest National Laboratory)

  • Hui Shi

    (Pacific Northwest National Laboratory)

  • János Szanyi

    (Pacific Northwest National Laboratory)

Abstract

Catalytic CO2 conversion to energy carriers and intermediates is of utmost importance to energy and environmental goals. However, the lack of fundamental understanding of the reaction mechanism renders designing a selective catalyst inefficient. Here we show the correlation between the kinetics of product formation and those of surface species conversion during CO2 reduction over Pd/Al2O3 catalysts. The operando transmission FTIR/SSITKA (Fourier transform infrared spectroscopy/steady-state isotopic transient kinetic analysis) experiments demonstrates that the rate-determining step for CO formation is the conversion of adsorbed formate, whereas that for CH4 formation is the hydrogenation of adsorbed carbonyl. The balance of the hydrogenation kinetics between adsorbed formates and carbonyls governs the selectivities to CH4 and CO. We apply this knowledge to the catalyst design and achieve high selectivities to desired products.

Suggested Citation

  • Xiang Wang & Hui Shi & János Szanyi, 2017. "Controlling selectivities in CO2 reduction through mechanistic understanding," Nature Communications, Nature, vol. 8(1), pages 1-6, December.
    • Handle: RePEc:nat:natcom:v:8:y:2017:i:1:d:10.1038_s41467-017-00558-9
    DOI: 10.1038/s41467-017-00558-9
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    Cited by:

    1. Vijay K. Velisoju & Jose L. Cerrillo & Rafia Ahmad & Hend Omar Mohamed & Yerrayya Attada & Qingpeng Cheng & Xueli Yao & Lirong Zheng & Osama Shekhah & Selvedin Telalovic & Javier Narciso & Luigi Caval, 2024. "Copper nanoparticles encapsulated in zeolitic imidazolate framework-8 as a stable and selective CO2 hydrogenation catalyst," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    2. Wang, Honglin & Liu, Yanrong & Laaksonen, Aatto & Krook-Riekkola, Anna & Yang, Zhuhong & Lu, Xiaohua & Ji, Xiaoyan, 2020. "Carbon recycling – An immense resource and key to a smart climate engineering: A survey of technologies, cost and impurity impact," Renewable and Sustainable Energy Reviews, Elsevier, vol. 131(C).
    3. Yang Liu & Jianhui Sun & Houhou Huang & Linlu Bai & Xiaomeng Zhao & Binhong Qu & Lunqiao Xiong & Fuquan Bai & Junwang Tang & Liqiang Jing, 2023. "Improving CO2 photoconversion with ionic liquid and Co single atoms," Nature Communications, Nature, vol. 14(1), pages 1-11, December.

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