A Nanoscale Ternary Amide‐rGO Composite with Boosted Kinetics for Reversible H2 Storage

Abstract Metal amides are attractive candidates for hydrogen storage due to their high volumetric and gravimetric hydrogen densities. However, the sluggish kinetics and competing side reactions during hydrogen uptake and release limit their practical use. Here, a novel nanoconfined Li2Mg(NH)2@reduce...

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Main Authors: Chaochao Dun, Sichi Li, Linfeng Chen, Robert D. Horton, Mark D. Allendorf, Brandon C. Wood, Vitalie Stavila, Jeffrey J. Urban
Format: Article
Language:English
Published: Wiley-VCH 2023-09-01
Series:Advanced Materials Interfaces
Subjects:
Online Access:https://doi.org/10.1002/admi.202300310
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author Chaochao Dun
Sichi Li
Linfeng Chen
Robert D. Horton
Mark D. Allendorf
Brandon C. Wood
Vitalie Stavila
Jeffrey J. Urban
author_facet Chaochao Dun
Sichi Li
Linfeng Chen
Robert D. Horton
Mark D. Allendorf
Brandon C. Wood
Vitalie Stavila
Jeffrey J. Urban
author_sort Chaochao Dun
collection DOAJ
description Abstract Metal amides are attractive candidates for hydrogen storage due to their high volumetric and gravimetric hydrogen densities. However, the sluggish kinetics and competing side reactions during hydrogen uptake and release limit their practical use. Here, a novel nanoconfined Li2Mg(NH)2@reduced graphene oxide (rGO) composite is presented, which is fabricated using a melt‐infiltration method with a minimum weight penalty of only 2 wt.%. The presence of rGO ensures close contact between the active phases, effectively preventing aggregation during cycling process. As a result, the reversible capacity of Li2Mg(NH)2@rGO reaches 4.42 wt.%, with no capacity degradation observed after multiple cycling. Theoretical calculations show that rGO catalyzes the hydrogen bond cleavage at the Mg‐amide/Li hydride interface, leading to local dehydrogenation hotspots and significantly improves kinetics of dehydrogenation compared to the bulk counterpart. This study provides a promising strategy for designing metal imide‐based composites to overcome the kinetic limitations and improve their reversible hydrogen storage performance.
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spelling doaj.art-49a25fa8c56246988c9f4aa5be05f4e42023-09-23T07:05:54ZengWiley-VCHAdvanced Materials Interfaces2196-73502023-09-011027n/an/a10.1002/admi.202300310A Nanoscale Ternary Amide‐rGO Composite with Boosted Kinetics for Reversible H2 StorageChaochao Dun0Sichi Li1Linfeng Chen2Robert D. Horton3Mark D. Allendorf4Brandon C. Wood5Vitalie Stavila6Jeffrey J. Urban7The Molecular Foundry Lawrence Berkeley National Laboratory Berkeley CA 94720 USALawrence Livermore National Laboratory 7000 East Avenue Livermore CA 94550 USAThe Molecular Foundry Lawrence Berkeley National Laboratory Berkeley CA 94720 USASandia National Laboratories Livermore CA 94550 USASandia National Laboratories Livermore CA 94550 USALawrence Livermore National Laboratory 7000 East Avenue Livermore CA 94550 USASandia National Laboratories Livermore CA 94550 USAThe Molecular Foundry Lawrence Berkeley National Laboratory Berkeley CA 94720 USAAbstract Metal amides are attractive candidates for hydrogen storage due to their high volumetric and gravimetric hydrogen densities. However, the sluggish kinetics and competing side reactions during hydrogen uptake and release limit their practical use. Here, a novel nanoconfined Li2Mg(NH)2@reduced graphene oxide (rGO) composite is presented, which is fabricated using a melt‐infiltration method with a minimum weight penalty of only 2 wt.%. The presence of rGO ensures close contact between the active phases, effectively preventing aggregation during cycling process. As a result, the reversible capacity of Li2Mg(NH)2@rGO reaches 4.42 wt.%, with no capacity degradation observed after multiple cycling. Theoretical calculations show that rGO catalyzes the hydrogen bond cleavage at the Mg‐amide/Li hydride interface, leading to local dehydrogenation hotspots and significantly improves kinetics of dehydrogenation compared to the bulk counterpart. This study provides a promising strategy for designing metal imide‐based composites to overcome the kinetic limitations and improve their reversible hydrogen storage performance.https://doi.org/10.1002/admi.202300310hydrogen storagekinetics of dehydrogenationsmelt infiltrationsnanoconfinementreduced graphene oxides
spellingShingle Chaochao Dun
Sichi Li
Linfeng Chen
Robert D. Horton
Mark D. Allendorf
Brandon C. Wood
Vitalie Stavila
Jeffrey J. Urban
A Nanoscale Ternary Amide‐rGO Composite with Boosted Kinetics for Reversible H2 Storage
Advanced Materials Interfaces
hydrogen storage
kinetics of dehydrogenations
melt infiltrations
nanoconfinement
reduced graphene oxides
title A Nanoscale Ternary Amide‐rGO Composite with Boosted Kinetics for Reversible H2 Storage
title_full A Nanoscale Ternary Amide‐rGO Composite with Boosted Kinetics for Reversible H2 Storage
title_fullStr A Nanoscale Ternary Amide‐rGO Composite with Boosted Kinetics for Reversible H2 Storage
title_full_unstemmed A Nanoscale Ternary Amide‐rGO Composite with Boosted Kinetics for Reversible H2 Storage
title_short A Nanoscale Ternary Amide‐rGO Composite with Boosted Kinetics for Reversible H2 Storage
title_sort nanoscale ternary amide rgo composite with boosted kinetics for reversible h2 storage
topic hydrogen storage
kinetics of dehydrogenations
melt infiltrations
nanoconfinement
reduced graphene oxides
url https://doi.org/10.1002/admi.202300310
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