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 journalArticlepeer-review

16 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 *CxHy adsorbates, as well as destabilizes the *C4H9 intermediate, and so promotes the selective production of the target alkane. [Figure not available: see fulltext.]

Original languageEnglish (US)
Pages (from-to)310-318
Number of pages9
JournalNature Catalysis
Volume6
Issue number4
DOIs
StatePublished - Apr 2023

ASJC Scopus subject areas

  • Catalysis
  • Bioengineering
  • Biochemistry
  • Process Chemistry and Technology

Fingerprint

Dive into the research topics of 'Selective synthesis of butane from carbon monoxide using cascade electrolysis and thermocatalysis at ambient conditions'. Together they form a unique fingerprint.

Cite this