Litcius/Paper detail

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

Mi Gyoung Lee‬, Sharath Kandambeth, Xiaoyan 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

2024Journal of the American Chemical Society22 citationsDOI

Abstract

Converting CO 2 to synthetic hydrocarbon fuels is of increasing interest. In light of progress in electrified CO 2 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 CO 2 to 1-C 4 H 8, wherein the outlet cathodic gas from a CO 2 -to-C 2 H 4 electrolyzer is fed directly (via a dehumidification stage) into the C 2 H 4 dimerizer, we study the highest-performing MOF found herein: M′ = Ru and M″ = Ni in the bimetallic two-dimensional M′ 2 (OAc) 4 M″(CN) 4 MOF. We report a 1-C 4 H 8 production rate of 1.3 mol g cat –1 h –1 and a C 2 H 4 conversion of 97%. From these experimental data, we project an estimated cradle-to-gate carbon intensity of −2.1 kg-CO 2 e/kg-1-C 4 H 8 when CO 2 is supplied from direct air capture and when the required energy is supplied by electricity having the carbon intensity of wind.

Topics & Concepts

ChemistryBimetallic stripMetal-organic frameworkEthyleneMetalOrganic chemistryCatalysisAdsorptionMetal-Organic Frameworks: Synthesis and ApplicationsCatalytic Processes in Materials ScienceCatalysis and Oxidation Reactions