Universal roles of hydrogen in electrochemical performance of graphene: high rate capacity and atomistic origins.

Abstract:

: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 sp(2) 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. These findings provide qualitative insights in helping the design of graphene-based materials for high-power electrodes.

journal_name

Sci Rep

journal_title

Scientific reports

authors

Ye J,Ong MT,Heo TW,Campbell PG,Worsley MA,Liu Y,Shin SJ,Charnvanichborikarn S,Matthews MJ,Bagge-Hansen M,Lee JR,Wood BC,Wang YM

doi

10.1038/srep16190

subject

Has Abstract

pub_date

2015-11-05 00:00:00

pages

16190

issn

2045-2322

pii

srep16190

journal_volume

5

pub_type

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