Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO                         2                          by Supporting Palladium on Metal Carbides

Jiajun Wang; Shyam Kattel; Christopher J. Hawxhurst; Ji Hoon Lee; Brian M. Tackett; Kuan Chang; Ning Rui; Chang Jun Liu; Jingguang G. Chen

doi:10.1002/anie.201900781

Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO ₂ by Supporting Palladium on Metal Carbides

Jiajun Wang, Shyam Kattel, Christopher J. Hawxhurst, Ji Hoon Lee, Brian M. Tackett, Kuan Chang, Ning Rui, Chang Jun Liu, Jingguang G. Chen

Research output: Contribution to journal › Article › peer-review

137 Scopus citations

Abstract

Electrochemical CO ₂ reduction reaction (CO ₂ RR) with renewable electricity is a potentially sustainable method to reduce CO ₂ emissions. Palladium supported on cost-effective transition-metal carbides (TMCs) are studied to reduce the Pd usage and tune the activity and selectivity of the CO ₂ RR to produce synthesis gas, using a combined approach of studying thin films and practical powder catalysts, in situ characterization, and density functional theory (DFT) calculations. Notably, Pd/TaC exhibits higher CO ₂ RR activity, stability and CO Faradaic efficiency than those of commercial Pd/C while significantly reducing the Pd loading. In situ measurements confirm the transformation of Pd into hydride (PdH) under the CO ₂ RR environment. DFT calculations reveal that the TMC substrates modify the binding energies of key intermediates on supported PdH. This work suggests the prospect of using TMCs as low-cost and stable substrates to support and modify Pd for enhanced CO ₂ RR activity.

Original language	English
Pages (from-to)	6271-6275
Number of pages	5
Journal	Angewandte Chemie - International Edition
Volume	58
Issue number	19
DOIs	https://doi.org/10.1002/anie.201900781
State	Published - 6 May 2019

Keywords

CO electroreduction
carbides
computational chemistry
in situ X-ray spectroscopy
palladium hydride

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10.1002/anie.201900781

Cite this

Wang, J., Kattel, S., Hawxhurst, C. J., Lee, J. H., Tackett, B. M., Chang, K., Rui, N., Liu, C. J., & Chen, J. G. (2019). Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO ₂ by Supporting Palladium on Metal Carbides Angewandte Chemie - International Edition, 58(19), 6271-6275. https://doi.org/10.1002/anie.201900781

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title = " Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO 2 by Supporting Palladium on Metal Carbides ",

abstract = " Electrochemical CO 2 reduction reaction (CO 2 RR) with renewable electricity is a potentially sustainable method to reduce CO 2 emissions. Palladium supported on cost-effective transition-metal carbides (TMCs) are studied to reduce the Pd usage and tune the activity and selectivity of the CO 2 RR to produce synthesis gas, using a combined approach of studying thin films and practical powder catalysts, in situ characterization, and density functional theory (DFT) calculations. Notably, Pd/TaC exhibits higher CO 2 RR activity, stability and CO Faradaic efficiency than those of commercial Pd/C while significantly reducing the Pd loading. In situ measurements confirm the transformation of Pd into hydride (PdH) under the CO 2 RR environment. DFT calculations reveal that the TMC substrates modify the binding energies of key intermediates on supported PdH. This work suggests the prospect of using TMCs as low-cost and stable substrates to support and modify Pd for enhanced CO 2 RR activity.",

keywords = "CO electroreduction, carbides, computational chemistry, in situ X-ray spectroscopy, palladium hydride",

author = "Jiajun Wang and Shyam Kattel and Hawxhurst, {Christopher J.} and Lee, {Ji Hoon} and Tackett, {Brian M.} and Kuan Chang and Ning Rui and Liu, {Chang Jun} and Chen, {Jingguang G.}",

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Wang, J, Kattel, S, Hawxhurst, CJ, Lee, JH, Tackett, BM, Chang, K, Rui, N, Liu, CJ & Chen, JG 2019, ' Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO ₂ by Supporting Palladium on Metal Carbides ', Angewandte Chemie - International Edition, vol. 58, no. 19, pp. 6271-6275. https://doi.org/10.1002/anie.201900781

Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO ₂ by Supporting Palladium on Metal Carbides . / Wang, Jiajun; Kattel, Shyam; Hawxhurst, Christopher J. et al.
In: Angewandte Chemie - International Edition, Vol. 58, No. 19, 06.05.2019, p. 6271-6275.

Research output: Contribution to journal › Article › peer-review

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AU - Kattel, Shyam

AU - Hawxhurst, Christopher J.

AU - Lee, Ji Hoon

AU - Tackett, Brian M.

AU - Chang, Kuan

AU - Rui, Ning

AU - Liu, Chang Jun

AU - Chen, Jingguang G.

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AB - Electrochemical CO 2 reduction reaction (CO 2 RR) with renewable electricity is a potentially sustainable method to reduce CO 2 emissions. Palladium supported on cost-effective transition-metal carbides (TMCs) are studied to reduce the Pd usage and tune the activity and selectivity of the CO 2 RR to produce synthesis gas, using a combined approach of studying thin films and practical powder catalysts, in situ characterization, and density functional theory (DFT) calculations. Notably, Pd/TaC exhibits higher CO 2 RR activity, stability and CO Faradaic efficiency than those of commercial Pd/C while significantly reducing the Pd loading. In situ measurements confirm the transformation of Pd into hydride (PdH) under the CO 2 RR environment. DFT calculations reveal that the TMC substrates modify the binding energies of key intermediates on supported PdH. This work suggests the prospect of using TMCs as low-cost and stable substrates to support and modify Pd for enhanced CO 2 RR activity.

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Wang J, Kattel S, Hawxhurst CJ, Lee JH, Tackett BM, Chang K et al. Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO ₂ by Supporting Palladium on Metal Carbides Angewandte Chemie - International Edition. 2019 May 6;58(19):6271-6275. doi: 10.1002/anie.201900781