Enhancing Selective Hydrofluorocarbon Greenhouse Gas Capture via Halogenation of Metal–Organic Frameworks

Jerozal, Ronald T.; Kim, Jaehwan; Ma, Carolyn; Pitt, Tristan A.; Lee, Jung-Hoon; Milner, Phillip J.

doi:10.1021/jacs.5c00393

Enhancing Selective Hydrofluorocarbon Greenhouse Gas Capture via Halogenation of Metal–Organic Frameworks

Journal Article · Sun Feb 16 00:00:00 EST 2025 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.5c00393· OSTI ID:3010121

Jerozal, Ronald T. ^[1]; ^[1]; Ma, Carolyn ^[1]; Pitt, Tristan A. ^[1]; ^[2]; ^[1]

Cornell Univ., Ithaca, NY (United States)
Korea Institute of Science and Technology (KIST), Seoul (Korea, Republic of); Korea Univ., Seoul, (Korea, Republic of)

Hydrofluorocarbons (HFCs) are anthropogenically produced greenhouse gases with longer atmospheric lifetimes and higher global warming potentials than those of carbon dioxide. General strategies to abate their emissions from industrial point sources, such as via adsorptive capture, remain scarce. Herein, we uncover the key structure–property relationships that lead to strong binding of HFCs such as fluoroform (CHF₃) and difluoromethane (CH₂F₂) in metal–organic frameworks (MOFs) under the low pressures relevant to flue gas scrubbing. Extensive gas sorption and computational studies support that the Zr-based microporous framework MOF-801-Br or HHU-2-Br (HHU = Heinrich-Heine-University Düsseldorf) strongly binds HFCs due to its synergistic combination of Zr-OH sites on the nodes and bromine sites on the linkers. As such, MOF-801-Br demonstrates a record-setting performance for separating CHF₃ from N₂ under dilute conditions. Our work highlights that the combination of multiple hydrogen-bonding sites in microporous MOFs represents a generalizable strategy for HFC capture, enabling their selective removal from industrial waste streams.

View Accepted Manuscript (DOE)

Research Organization:: Cornell Univ., Ithaca, NY (United States)

Sponsoring Organization:: Camille and Henry Dreyfus Foundation; Korea Institute of Science and Technology; National Research Foundation of Korea; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0021000

OSTI ID:: 3010121

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 8 Vol. 147; ISSN 0002-7863; ISSN 1520-5126

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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