Pore Compartmentalization of CO 2 and H 2 O in a Redox‐Active Adsorbent

ABSTRACT Achieving sustainable carbon capture under realistic, humid conditions remains a central challenge for decarbonization technologies. Here we report an ultramicroporous oxofluorovanadate metal‐organic framework, Ni(pyrazine) 2 (VOF 4 ), that dynamically regulates competitive adsorption through reversible redox chemistry. Under humid dilute CO 2 streams (4 vol%), water chemisorbs at vanadium centers in the form of hydroxide ligands and induces a reversible V(+4)|V(+5) transformation to an isoreticular phase, Ni(pyrazine) 2 (VO(OH)F 4 ), while CO 2 is engaged in strong physisorption within pyrazine‐lined pore regions. This redox‐driven compartmentalization of H 2 O and CO 2 results in a dynamic breakthrough CO 2 capacity of 2.04 ± 0.07 mmol/g, sustained for up to 50 cycles and showing resilience under intense humidification or steam exposure. These findings establish redox‐adaptive adsorption in BVR‐X as a unique design paradigm, enabling scalable and durable carbon capture under realistic operating conditions.

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Publication Details

Journal
Angewandte Chemie International Edition
Published
2026-09-30
DOI
https://doi.org/10.1002/anie.9809119
Primary Topic
Metal-Organic Frameworks: Synthesis and Applications
Type
article
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article

Pore Compartmentalization of CO 2 and H 2 O in a Redox‐Active Adsorbent

Chun‐Wai Chang, Mourad Younes, Ah‐Young Song, Alireza Pourghaderi et al.
Angewandte Chemie International Edition
Metal-Organic Frameworks: Synthesis and Applications
article

Pore Compartmentalization of CO 2 and H 2 O in a Redox‐Active Adsorbent

Chun‐Wai Chang, Mourad Younes, Ah‐Young Song, Alireza Pourghaderi, Andrzej Gładysiak, Casey R. Simons, Jeffrey A. Reimer, Aqil Jamal, Zhenxing Feng, Kyriakos C. Stylianou, Emmanuel Nyela Musa, Ankit Kumar Yadav, Kai Shen Choong, Ammar Alahmed, Micah Lee Wilson
article en

Abstract

ABSTRACT Achieving sustainable carbon capture under realistic, humid conditions remains a central challenge for decarbonization technologies. Here we report an ultramicroporous oxofluorovanadate metal‐organic framework, Ni(pyrazine) 2 (VOF 4 ), that dynamically regulates competitive adsorption through reversible redox chemistry. Under humid dilute CO 2 streams (4 vol%), water chemisorbs at vanadium centers in the form of hydroxide ligands and induces a reversible V(+4)|V(+5) transformation to an isoreticular phase, Ni(pyrazine) 2 (VO(OH)F 4 ), while CO 2 is engaged in strong physisorption within pyrazine‐lined pore regions. This redox‐driven compartmentalization of H 2 O and CO 2 results in a dynamic breakthrough CO 2 capacity of 2.04 ± 0.07 mmol/g, sustained for up to 50 cycles and showing resilience under intense humidification or steam exposure. These findings establish redox‐adaptive adsorption in BVR‐X as a unique design paradigm, enabling scalable and durable carbon capture under realistic operating conditions.

Angewandte Chemie International Edition
Oregon State University (US), University of Oregon (US), Saudi Aramco (Saudi Arabia) (SA), Resonance Research (United States) (US), University of California, Berkeley (US)
Responsible consumption and production
Openalex Percentile: Top 27%
Metal-Organic Frameworks: Synthesis and Applications
DOISourceOpenAlex
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