TY - JOUR
T1 - Conductive Boron-Doped Graphene as an Ideal Material for Electrocatalytically Switchable and High-Capacity Hydrogen Storage
AU - Tan, Xin
AU - Tahini, Hassan A.
AU - Smith, Sean C.
N1 - Publisher Copyright:
© 2016 American Chemical Society.
PY - 2016/12/7
Y1 - 2016/12/7
N2 - Electrocatalytic, switchable hydrogen storage promises both tunable kinetics and facile reversibility without the need for specific catalysts. The feasibility of this approach relies on having materials that are easy to synthesize, possessing good electrical conductivities. Graphitic carbon nitride (g-C4N3) has been predicted to display charge-responsive binding with molecular hydrogen - the only such conductive sorbent material that has been discovered to date. As yet, however, this conductive variant of graphitic carbon nitride is not readily synthesized by scalable methods. Here, we examine the possibility of conductive and easily synthesized boron-doped graphene nanosheets (B-doped graphene) as sorbent materials for practical applications of electrocatalytically switchable hydrogen storage. Using first-principle calculations, we find that the adsorption energy of H2 molecules on B-doped graphene can be dramatically enhanced by removing electrons from and thereby positively charging the adsorbent. Thus, by controlling charge injected or depleted from the adsorbent, one can effectively tune the storage/release processes which occur spontaneously without any energy barriers. At full hydrogen coverage, the positively charged BC5 achieves high storage capacities up to 5.3 wt %. Importantly, B-doped graphene, such as BC49, BC7, and BC5, have good electrical conductivity and can be easily synthesized by scalable methods, which positions this class of material as a very good candidate for charge injection/release. These predictions pave the route for practical implementation of electrocatalytic systems with switchable storage/release capacities that offer high capacity for hydrogen storage.
AB - Electrocatalytic, switchable hydrogen storage promises both tunable kinetics and facile reversibility without the need for specific catalysts. The feasibility of this approach relies on having materials that are easy to synthesize, possessing good electrical conductivities. Graphitic carbon nitride (g-C4N3) has been predicted to display charge-responsive binding with molecular hydrogen - the only such conductive sorbent material that has been discovered to date. As yet, however, this conductive variant of graphitic carbon nitride is not readily synthesized by scalable methods. Here, we examine the possibility of conductive and easily synthesized boron-doped graphene nanosheets (B-doped graphene) as sorbent materials for practical applications of electrocatalytically switchable hydrogen storage. Using first-principle calculations, we find that the adsorption energy of H2 molecules on B-doped graphene can be dramatically enhanced by removing electrons from and thereby positively charging the adsorbent. Thus, by controlling charge injected or depleted from the adsorbent, one can effectively tune the storage/release processes which occur spontaneously without any energy barriers. At full hydrogen coverage, the positively charged BC5 achieves high storage capacities up to 5.3 wt %. Importantly, B-doped graphene, such as BC49, BC7, and BC5, have good electrical conductivity and can be easily synthesized by scalable methods, which positions this class of material as a very good candidate for charge injection/release. These predictions pave the route for practical implementation of electrocatalytic systems with switchable storage/release capacities that offer high capacity for hydrogen storage.
KW - boron-doped graphene
KW - charge-controlled switchable
KW - density functional theory
KW - high capacity
KW - hydrogen storage
UR - http://www.scopus.com/inward/record.url?scp=85002950284&partnerID=8YFLogxK
U2 - 10.1021/acsami.6b10814
DO - 10.1021/acsami.6b10814
M3 - Article
SN - 1944-8244
VL - 8
SP - 32815
EP - 32822
JO - ACS applied materials & interfaces
JF - ACS applied materials & interfaces
IS - 48
ER -