Edge-activated graphene nanopores for thermally robust hydrogen membrane separations

Abstract Temperature-dependent, selective molecular diffusion through porous materials is crucial for membrane separations and is typically modeled as an Arrhenius-type activated process. Although this dependence can be described phenomenologically by an activation energy, tracing its molecular orig...

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Main Authors: Chi Cheng, Lohyun Kim, Aaron H. Persad, Chun Man Chow, Rohit Karnik
Format: Article
Language:English
Published: Nature Portfolio 2025-07-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-61110-8
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author Chi Cheng
Lohyun Kim
Aaron H. Persad
Chun Man Chow
Rohit Karnik
author_facet Chi Cheng
Lohyun Kim
Aaron H. Persad
Chun Man Chow
Rohit Karnik
author_sort Chi Cheng
collection DOAJ
description Abstract Temperature-dependent, selective molecular diffusion through porous materials is crucial for membrane separations and is typically modeled as an Arrhenius-type activated process. Although this dependence can be described phenomenologically by an activation energy, tracing its molecular origins is often difficult, hindering robust membrane design for practical applications. Here, we investigate gas transport across monolayer nanoporous graphene membranes and observe significant, reversible, temperature-robust, and gas species-selective activated transport, with increased selectivity at rising temperatures, unlike many conventional membranes. Combined experiment and modelling trace this behavior to graphene nanopore edge functional groups, whose thermal fluctuations modulate effective pore size. This activated transport remains stable with aging over 1 year and shows selectivity exceeding 70 for hydrogen/hydrocarbon mixture separation at 220 °C, representative of dehydrogenation reactor temperatures. Our results demonstrate the thermal and long-term robustness of nanoporous graphene membranes, suggesting potential for precise engineering of nanopore surface chemistries in membranes for challenging molecular separations.
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institution Kabale University
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spelling doaj-art-7f4e106fe9364b1c8308f1bca78f8af42025-08-20T04:01:36ZengNature PortfolioNature Communications2041-17232025-07-0116111410.1038/s41467-025-61110-8Edge-activated graphene nanopores for thermally robust hydrogen membrane separationsChi Cheng0Lohyun Kim1Aaron H. Persad2Chun Man Chow3Rohit Karnik4Department of Mechanical Engineering, Massachusetts Institute of TechnologyDepartment of Mechanical Engineering, Massachusetts Institute of TechnologyDepartment of Mechanical Engineering, Massachusetts Institute of TechnologyDepartment of Chemical Engineering, Massachusetts Institute of TechnologyDepartment of Mechanical Engineering, Massachusetts Institute of TechnologyAbstract Temperature-dependent, selective molecular diffusion through porous materials is crucial for membrane separations and is typically modeled as an Arrhenius-type activated process. Although this dependence can be described phenomenologically by an activation energy, tracing its molecular origins is often difficult, hindering robust membrane design for practical applications. Here, we investigate gas transport across monolayer nanoporous graphene membranes and observe significant, reversible, temperature-robust, and gas species-selective activated transport, with increased selectivity at rising temperatures, unlike many conventional membranes. Combined experiment and modelling trace this behavior to graphene nanopore edge functional groups, whose thermal fluctuations modulate effective pore size. This activated transport remains stable with aging over 1 year and shows selectivity exceeding 70 for hydrogen/hydrocarbon mixture separation at 220 °C, representative of dehydrogenation reactor temperatures. Our results demonstrate the thermal and long-term robustness of nanoporous graphene membranes, suggesting potential for precise engineering of nanopore surface chemistries in membranes for challenging molecular separations.https://doi.org/10.1038/s41467-025-61110-8
spellingShingle Chi Cheng
Lohyun Kim
Aaron H. Persad
Chun Man Chow
Rohit Karnik
Edge-activated graphene nanopores for thermally robust hydrogen membrane separations
Nature Communications
title Edge-activated graphene nanopores for thermally robust hydrogen membrane separations
title_full Edge-activated graphene nanopores for thermally robust hydrogen membrane separations
title_fullStr Edge-activated graphene nanopores for thermally robust hydrogen membrane separations
title_full_unstemmed Edge-activated graphene nanopores for thermally robust hydrogen membrane separations
title_short Edge-activated graphene nanopores for thermally robust hydrogen membrane separations
title_sort edge activated graphene nanopores for thermally robust hydrogen membrane separations
url https://doi.org/10.1038/s41467-025-61110-8
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AT aaronhpersad edgeactivatedgraphenenanoporesforthermallyrobusthydrogenmembraneseparations
AT chunmanchow edgeactivatedgraphenenanoporesforthermallyrobusthydrogenmembraneseparations
AT rohitkarnik edgeactivatedgraphenenanoporesforthermallyrobusthydrogenmembraneseparations