Paradoxical roles of hydrogen in electrochemical performance of graphene: High rate capacity and atomistic origins

Ye, Jianchao C.; Ong, Mitchell T.; Heo, Tae Wook; Campbell, Patrick G.; Worsley, Marcus A.; Liu, Yuanyue Y.; Charnvanichborikarn, Supakit; Matthews, Manyalibo J.; Bagge-Hansen, Michael; Lee, Jonathan R. I.; Wood, Brandon C.; Wang, Y. Morris; Shin, Swanee J.

doi:10.1038/srep16190

Paradoxical roles of hydrogen in electrochemical performance of graphene: High rate capacity and atomistic origins

Journal Article · Thu Nov 05 00:00:00 EST 2015 · Scientific Reports

DOI:https://doi.org/10.1038/srep16190· OSTI ID:1251039

Ye, Jianchao C. ^[1]; Ong, Mitchell T. ^[1]; Heo, Tae Wook ^[1]; Campbell, Patrick G. ^[1]; Worsley, Marcus A. ^[1]; Liu, Yuanyue Y. ^[1]; Charnvanichborikarn, Supakit ^[1]; Matthews, Manyalibo J. ^[1]; Bagge-Hansen, Michael ^[1]; Lee, Jonathan R. I. ^[1]; Wood, Brandon C. ^[1]; Wang, Y. Morris ^[1]; Shin, Swanee J. ^[1]

Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Atomic hydrogen exists ubiquitously in graphene materials made by chemical methods. Yet determining the effect of hydrogen on the electrochemical performance of graphene remains a significant challenge. Here we report the experimental observations of high rate capacity in hydrogen-treated 3-dimensional (3D) graphene nanofoam electrodes for lithium ion batteries. Structural and electronic characterization suggests that defect sites and hydrogen play synergistic roles in disrupting sp² graphene to facilitate fast lithium transport and reversible surface binding, as evidenced by the fast charge-transfer kinetics and increased capacitive contribution in hydrogen-treated 3D graphene. In concert with experiments, multiscale calculations reveal that defect complexes in graphene are prerequisite for low-temperature hydrogenation, and that the hydrogenation of defective or functionalized sites at strained domain boundaries plays a beneficial role in improving rate capacity by opening gaps to facilitate easier Li penetration. Additional reversible capacity is provided by enhanced lithium binding near hydrogen-terminated edge sites. Furthermore, these findings provide qualitative insights in helping the design of graphene-based materials for high-power electrodes.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1251039

Report Number(s):: LLNL-JRNL--670804

Journal Information:: Scientific Reports, Journal Name: Scientific Reports Journal Issue: C Vol. 5; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Paradoxical roles of hydrogen in electrochemical performance of graphene: High rate capacity and atomistic origins

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