Adaptive Pore Opening to Form Tailored Adsorption Sites in a Cooperatively Flexible Framework Enables Record Inverse Propane/Propylene Separation

Klein, Ryan A.; Bingel, Lukas W.; Halder, Arijit; Carter, Marcus; Trump, Benjamin A.; Bloch, Eric D.; Zhou, Wei; Walton, Krista S.; Brown, Craig M.; McGuirk, C. Michael

doi:10.1021/jacs.3c06754

Adaptive Pore Opening to Form Tailored Adsorption Sites in a Cooperatively Flexible Framework Enables Record Inverse Propane/Propylene Separation

Journal Article · Fri Sep 29 00:00:00 EDT 2023 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.3c06754· OSTI ID:2203517

Klein, Ryan A. ^[1]; Bingel, Lukas W. ^[2]; ^[3]; Carter, Marcus ^[4]; Trump, Benjamin A. ^[4]; ^[5]; ^[4]; Walton, Krista S. ^[2]; ^[6]; ^[3]

National Renewable Energy Laboratory (NREL), Golden, CO (United States); National Institute of Standards and Technology (NIST), Gaithersburg, MD (United States)
Georgia Institute of Technology, Atlanta, GA (United States)
Colorado School of Mines, Golden, CO (United States)
National Institute of Standards and Technology (NIST), Gaithersburg, MD (United States)
University of Delaware, Newark, DE (United States)
National Institute of Standards and Technology (NIST), Gaithersburg, MD (United States); University of Delaware, Newark, DE (United States)

A proposed low-energy alternative to the separation of alkanes from alkenes by energy-intensive cryogenic distillation is separation by porous adsorbents. Unfortunately, most adsorbents preferentially take up the desired, high-value major component alkene, requiring frequent regeneration. Adsorbents with inverse selectivity for the minor component alkane would enable the direct production of purified, reagent-grade alkene, greatly reducing global energy consumption. However, such materials are exceedingly rare, especially for propane/propylene separation. Here, we report that through adaptive and spontaneous pore size and shape adaptation to optimize an ensemble of weak noncovalent interactions, the structurally responsive metal-organic framework CdIF-13 (sod-Cd(benzimidazolate)₂) exhibits inverse selectivity for propane over propylene with record-setting separation performance under industrially relevant temperature, pressure, and mixture conditions. Powder synchrotron X-ray diffraction measurements combined with first-principles calculations yield atomic-scale insight and reveal the induced fit mechanism of adsorbate-specific pore adaptation and ensemble interactions between ligands and adsorbates. Dynamic column breakthrough measurements confirm that CdIF-13 displays selectivity under mixed-component conditions of varying ratios, with a record measured selectivity factor of α ≈ 3 at 95:5 propylene:propane at 298 K and 1 bar. When sequenced with a low-cost rigid adsorbent, we demonstrated the direct purification of propylene under ambient conditions. In conclusion, this combined atomic-level structural characterization and performance testing firmly establishes how cooperatively flexible materials can be capable of unprecedented separation factors.

View Accepted Manuscript (DOE)

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Hydrogen Fuel Cell Technologies Office (HFTO); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; AC36-08GO28308; EE0008823

OSTI ID:: 2203517

Report Number(s):: NREL/JA--5900-85399; MainId:86172; UUID:30baaddd-2074-4a21-af59-80123d387cd4; MainAdminID:70779

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 40 Vol. 145; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Adaptive Pore Opening to Form Tailored Adsorption Sites in a Cooperatively Flexible Framework Enables Record Inverse Propane/Propylene Separation

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