Bimetallic Metal Sites in Metal-Organic Frameworks Facilitate the Production of 1-Butene from Electrosynthesized Ethylene

Mi Gyoung Lee, Sharath Kandambeth, Xiao Yan Li, Osama Shekhah, Adnan Ozden, Joshua Wicks, Pengfei Ou, Sasa Wang, Roham Dorakhan, Sungjin Park, Prashant M. Bhatt, Vinayak S. Kale, David Sinton, Mohamed Eddaoudi*, Edward H. Sargent*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

Converting CO2 to synthetic hydrocarbon fuels is of increasing interest. In light of progress in electrified CO2 to ethylene, we explored routes to dimerize to 1-butene, an olefin that can serve as a building block to ethylene longer-chain alkanes. With goal of selective and active dimerization, we investigate a series of metal-organic frameworks having bimetallic catalytic sites. We find that the tunable pore structure enables optimization of selectivity and that periodic pore channels enhance activity. In a tandem system for the conversion of CO2 to 1-C4H8, wherein the outlet cathodic gas from a CO2-to-C2H4 electrolyzer is fed directly (via a dehumidification stage) into the C2H4 dimerizer, we study the highest-performing MOF found herein: M′ = Ru and M″ = Ni in the bimetallic two-dimensional M′2(OAc)4M″(CN)4 MOF. We report a 1-C4H8 production rate of 1.3 mol gcat-1 h-1 and a C2H4 conversion of 97%. From these experimental data, we project an estimated cradle-to-gate carbon intensity of −2.1 kg-CO2e/kg-1-C4H8 when CO2 is supplied from direct air capture and when the required energy is supplied by electricity having the carbon intensity of wind.

Original languageEnglish (US)
Pages (from-to)14267-14277
Number of pages11
JournalJournal of the American Chemical Society
Volume146
Issue number20
DOIs
StatePublished - May 22 2024

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry
  • Biochemistry
  • Colloid and Surface Chemistry

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