Multigas adsorption with single-site cooperativity in a metal–organic framework

Cooperative gas adsorption in metal-organic frameworks (MOFs) is a rare phenomenon that generally involves long-range communication between multiple binding sites. We demonstrate a MOF containing cobalt(II)-methyl sites that selectively and reversibly capture two carbon monoxide (CO) molecules per site, leading to record-high adsorption capacities at ambient temperatures and pressures. Gas adsorption and structural, spectroscopic, and computational analyses support a mechanism in which binding of one CO molecule triggers a spin transition, followed by binding of a second CO molecule and migratory insertion of the first CO molecule into the cobalt-methyl bond to form an acetyl. The greater binding affinity associated with the second CO results in sigmoidal adsorption isotherms, a hallmark of cooperativity and phase-change materials, despite the absence of long-range interactions within the framework.

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Publication Details

Journal
Science
Published
2025-11-20
DOI
https://doi.org/10.1126/science.ady2607
Citations
3
Primary Topic
Metal-Organic Frameworks: Synthesis and Applications
Type
article
Field-Weighted Citation Impact
1.61
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article

Multigas adsorption with single-site cooperativity in a metal–organic framework

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3 citations
Science
Metal-Organic Frameworks: Synthesis and Applications
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article

Multigas adsorption with single-site cooperativity in a metal–organic framework

Hope A. Silva, Katie R. Meihaus, Nicholas P. Stadie, Yuto Yabuuchi, Andrew M. Minor, Kristin Aslaug Persson, Jeffrey R. Long, Kurtis M. Carsch, Ryan A. Murphy, Craig M. Brown, Ryan A. Klein, Zikri Hasanbasri, Henry Z. H. Jiang, Jordan W. Taylor, Jesse L. Peltier, Sarah L. Karstens, Hyunchul Kwon, Jonas Börgel, Matthew N. Dods, Andrew Rosen, R. David Britt, Karen C. Bustillo, Adrian J. Huang, Peyton S. Summerhill
article en
3 citations

Abstract

Cooperative gas adsorption in metal-organic frameworks (MOFs) is a rare phenomenon that generally involves long-range communication between multiple binding sites. We demonstrate a MOF containing cobalt(II)-methyl sites that selectively and reversibly capture two carbon monoxide (CO) molecules per site, leading to record-high adsorption capacities at ambient temperatures and pressures. Gas adsorption and structural, spectroscopic, and computational analyses support a mechanism in which binding of one CO molecule triggers a spin transition, followed by binding of a second CO molecule and migratory insertion of the first CO molecule into the cobalt-methyl bond to form an acetyl. The greater binding affinity associated with the second CO results in sigmoidal adsorption isotherms, a hallmark of cooperativity and phase-change materials, despite the absence of long-range interactions within the framework.

ScienceVol. 390(6775)
National Laboratory of the Rockies (US), National Institute of Standards and Technology (US), Lawrence Berkeley National Laboratory (US), Princeton University (US), Montana State University (US), Baker Hughes (United States) (US), Miller College (US), NIST Center for Neutron Research (US), University of California, Davis (US), University of Delaware (US), University of California, Berkeley (US)
Openalex Percentile: Top 15%
Metal-Organic Frameworks: Synthesis and Applications
1.61
DOISourceOpenAlex
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