Selective synthesis of butane from carbon monoxide using cascade electrolysis and thermocatalysis at ambient conditions

Mi Gyoung Lee; Xiao Yan Li; Adnan Ozden; Joshua Wicks; Pengfei Ou; Yuhang Li; Roham Dorakhan; Jaekyoung Lee; Hoon Kee Park; Jin Wook Yang; Bin Chen; Jehad Abed; Roberto Moreno Souza dos Reis; Geonhui Lee; Jianan Erick Huang; Tao Peng; Ya Huei (Cathy) Chin; David Sinton; Edward H. Sargent

doi:10.1038/s41929-023-00937-0

Selective synthesis of butane from carbon monoxide using cascade electrolysis and thermocatalysis at ambient conditions

Mi Gyoung Lee, Xiao Yan Li, Adnan Ozden, Joshua Wicks, Pengfei Ou, Yuhang Li, Roham Dorakhan, Jaekyoung Lee, Hoon Kee Park, Jin Wook Yang, Bin Chen, Jehad Abed, Roberto Moreno Souza dos Reis, Geonhui Lee, Jianan Erick Huang, Tao Peng, Ya Huei (Cathy) Chin, David Sinton, Edward H. Sargent^*

^*Corresponding author for this work

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

47 Scopus citations

Abstract

It is of interest to extend the reach of CO₂ and CO electrochemistry to the synthesis of products with molecular weights higher than the C₁ and C₂ seen in most prior reports carried out near ambient conditions. Here we present a cascade C₁–C₂–C₄ system that combines electrochemical and thermochemical reactors to produce C₄H₁₀ selectively at ambient conditions. In a C₂H₄ dimerization reactor, we directly upgrade the gas outlet stream of the CO₂ or CO electrolyser without purification. We find that CO, which is present alongside C₂H₄, enhances C₂H₄ dimerization selectivity to give C₄H₁₀ to 95%, a much higher performance than when a CO₂ electrolyser is used instead. We achieve an overall two-stage CO-to-C₄H₁₀ cascade selectivity of 43%. Mechanistic investigations, complemented by density functional theory calculations reveal that increased CO coverage favours C₂H₄ dimerization and hydrogenation of *C_xH_y adsorbates, as well as destabilizes the *C₄H₉ intermediate, and so promotes the selective production of the target alkane. [Figure not available: see fulltext.]

Original language	English (US)
Pages (from-to)	310-318
Number of pages	9
Journal	Nature Catalysis
Volume	6
Issue number	4
DOIs	https://doi.org/10.1038/s41929-023-00937-0
State	Published - Apr 2023

Funding

All DFT calculations were performed on the Niagara supercomputer of the SciNet HPC Consortium. SciNet is funded by the Canada Foundation for Innovation, the Government of Ontario, Ontario Research Fund Research Excellence Program and the University of Toronto. M.G.L. acknowledges the Basic Science Research Program through the NRF funded by the Ministry of Education (2021R1A6A3A03039988). J.W.Y. acknowledges the Basic Science Research Program through the NRF funded by the Ministry of Education (2021R1A6A3A13046700). All DFT calculations were performed on the Niagara supercomputer of the SciNet HPC Consortium. SciNet is funded by the Canada Foundation for Innovation, the Government of Ontario, Ontario Research Fund Research Excellence Program and the University of Toronto. M.G.L. acknowledges the Basic Science Research Program through the NRF funded by the Ministry of Education (2021R1A6A3A03039988). J.W.Y. acknowledges the Basic Science Research Program through the NRF funded by the Ministry of Education (2021R1A6A3A13046700).

ASJC Scopus subject areas

Catalysis
Bioengineering
Biochemistry
Process Chemistry and Technology

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Lee, M. G., Li, X. Y., Ozden, A., Wicks, J., Ou, P., Li, Y., Dorakhan, R., Lee, J., Park, H. K., Yang, J. W., Chen, B., Abed, J., Souza dos Reis, R. M., Lee, G., Huang, J. E., Peng, T., Chin, Y. H., Sinton, D., & Sargent, E. H. (2023). Selective synthesis of butane from carbon monoxide using cascade electrolysis and thermocatalysis at ambient conditions. Nature Catalysis, 6(4), 310-318. https://doi.org/10.1038/s41929-023-00937-0

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title = "Selective synthesis of butane from carbon monoxide using cascade electrolysis and thermocatalysis at ambient conditions",

abstract = "It is of interest to extend the reach of CO2 and CO electrochemistry to the synthesis of products with molecular weights higher than the C1 and C2 seen in most prior reports carried out near ambient conditions. Here we present a cascade C1–C2–C4 system that combines electrochemical and thermochemical reactors to produce C4H10 selectively at ambient conditions. In a C2H4 dimerization reactor, we directly upgrade the gas outlet stream of the CO2 or CO electrolyser without purification. We find that CO, which is present alongside C2H4, enhances C2H4 dimerization selectivity to give C4H10 to 95%, a much higher performance than when a CO2 electrolyser is used instead. We achieve an overall two-stage CO-to-C4H10 cascade selectivity of 43%. Mechanistic investigations, complemented by density functional theory calculations reveal that increased CO coverage favours C2H4 dimerization and hydrogenation of *CxHy adsorbates, as well as destabilizes the *C4H9 intermediate, and so promotes the selective production of the target alkane. [Figure not available: see fulltext.]",

author = "Lee, {Mi Gyoung} and Li, {Xiao Yan} and Adnan Ozden and Joshua Wicks and Pengfei Ou and Yuhang Li and Roham Dorakhan and Jaekyoung Lee and Park, {Hoon Kee} and Yang, {Jin Wook} and Bin Chen and Jehad Abed and {Souza dos Reis}, {Roberto Moreno} and Geonhui Lee and Huang, {Jianan Erick} and Tao Peng and Chin, {Ya Huei (Cathy)} and David Sinton and Sargent, {Edward H.}",

note = "Publisher Copyright: {\textcopyright} 2023, The Author(s), under exclusive licence to Springer Nature Limited.",

year = "2023",

month = apr,

doi = "10.1038/s41929-023-00937-0",

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Lee, MG, Li, XY, Ozden, A, Wicks, J, Ou, P, Li, Y, Dorakhan, R, Lee, J, Park, HK, Yang, JW, Chen, B, Abed, J, Souza dos Reis, RM, Lee, G, Huang, JE, Peng, T, Chin, YH, Sinton, D & Sargent, EH 2023, 'Selective synthesis of butane from carbon monoxide using cascade electrolysis and thermocatalysis at ambient conditions', Nature Catalysis, vol. 6, no. 4, pp. 310-318. https://doi.org/10.1038/s41929-023-00937-0

TY - JOUR

T1 - Selective synthesis of butane from carbon monoxide using cascade electrolysis and thermocatalysis at ambient conditions

AU - Lee, Mi Gyoung

AU - Li, Xiao Yan

AU - Ozden, Adnan

AU - Wicks, Joshua

AU - Ou, Pengfei

AU - Li, Yuhang

AU - Dorakhan, Roham

AU - Lee, Jaekyoung

AU - Park, Hoon Kee

AU - Yang, Jin Wook

AU - Chen, Bin

AU - Abed, Jehad

AU - Souza dos Reis, Roberto Moreno

AU - Lee, Geonhui

AU - Huang, Jianan Erick

AU - Peng, Tao

AU - Chin, Ya Huei (Cathy)

AU - Sinton, David

AU - Sargent, Edward H.

PY - 2023/4

Y1 - 2023/4

N2 - It is of interest to extend the reach of CO2 and CO electrochemistry to the synthesis of products with molecular weights higher than the C1 and C2 seen in most prior reports carried out near ambient conditions. Here we present a cascade C1–C2–C4 system that combines electrochemical and thermochemical reactors to produce C4H10 selectively at ambient conditions. In a C2H4 dimerization reactor, we directly upgrade the gas outlet stream of the CO2 or CO electrolyser without purification. We find that CO, which is present alongside C2H4, enhances C2H4 dimerization selectivity to give C4H10 to 95%, a much higher performance than when a CO2 electrolyser is used instead. We achieve an overall two-stage CO-to-C4H10 cascade selectivity of 43%. Mechanistic investigations, complemented by density functional theory calculations reveal that increased CO coverage favours C2H4 dimerization and hydrogenation of *CxHy adsorbates, as well as destabilizes the *C4H9 intermediate, and so promotes the selective production of the target alkane. [Figure not available: see fulltext.]

AB - It is of interest to extend the reach of CO2 and CO electrochemistry to the synthesis of products with molecular weights higher than the C1 and C2 seen in most prior reports carried out near ambient conditions. Here we present a cascade C1–C2–C4 system that combines electrochemical and thermochemical reactors to produce C4H10 selectively at ambient conditions. In a C2H4 dimerization reactor, we directly upgrade the gas outlet stream of the CO2 or CO electrolyser without purification. We find that CO, which is present alongside C2H4, enhances C2H4 dimerization selectivity to give C4H10 to 95%, a much higher performance than when a CO2 electrolyser is used instead. We achieve an overall two-stage CO-to-C4H10 cascade selectivity of 43%. Mechanistic investigations, complemented by density functional theory calculations reveal that increased CO coverage favours C2H4 dimerization and hydrogenation of *CxHy adsorbates, as well as destabilizes the *C4H9 intermediate, and so promotes the selective production of the target alkane. [Figure not available: see fulltext.]

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Selective synthesis of butane from carbon monoxide using cascade electrolysis and thermocatalysis at ambient conditions

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