TY - JOUR
T1 - The mechanism of the chain-growth of ammoniaborane
T2 - A classic Lewis pairs catalysed by a Frustrated Lewis Pairs
AU - Wang, Kun
AU - Cheng, Long jiu
AU - Zhang, Jian guo
AU - Yu, Xue bin
N1 - Publisher Copyright:
© 2018 Hydrogen Energy Publications LLC
PY - 2018/3/1
Y1 - 2018/3/1
N2 - Ammonia borane (AB) is an outstanding hydrogen-storage material, which has been gained many attentions. It can be regenerated from polyborazylene based on the experimental study, but the uncontrollable B–N dehydro-coupling in the polymerization from AB to borazine is still a problem for the continuous application of AB. Frustrated Lewis Pairs (FLPs) is a landmark discovery to dissociate small molecules by activating strong nonpolar bonds reversibly, which is recently applied to directly polymerize three molecular AB to a cyclotriborazylene (CTB, B3N3H12, which transforms into borazine after releasing 3 equiv. H2). Here we analyse how a dimethylxanthene-derived FLPs catalyse AB to CTB. The cyclization experiences three steps by our calculation: the connection between FLPs and AB (1), the growth of B–N chain (2) and an intermolecular dehydrogenation between terminal N-Hδ+ and δ−H–B (3), which gives us a clue of a possible reversibility of the dehydrogenation of AB and broadens the applicability of this concept in the relevant catalyst design.
AB - Ammonia borane (AB) is an outstanding hydrogen-storage material, which has been gained many attentions. It can be regenerated from polyborazylene based on the experimental study, but the uncontrollable B–N dehydro-coupling in the polymerization from AB to borazine is still a problem for the continuous application of AB. Frustrated Lewis Pairs (FLPs) is a landmark discovery to dissociate small molecules by activating strong nonpolar bonds reversibly, which is recently applied to directly polymerize three molecular AB to a cyclotriborazylene (CTB, B3N3H12, which transforms into borazine after releasing 3 equiv. H2). Here we analyse how a dimethylxanthene-derived FLPs catalyse AB to CTB. The cyclization experiences three steps by our calculation: the connection between FLPs and AB (1), the growth of B–N chain (2) and an intermolecular dehydrogenation between terminal N-Hδ+ and δ−H–B (3), which gives us a clue of a possible reversibility of the dehydrogenation of AB and broadens the applicability of this concept in the relevant catalyst design.
KW - Density functional theory
KW - Frustrated Lewis Pairs (FLPs)
KW - Hydrogen-storage material
KW - Metal-free hydrogenation
KW - Reaction kinetic study
UR - http://www.scopus.com/inward/record.url?scp=85041588116&partnerID=8YFLogxK
U2 - 10.1016/j.ijhydene.2018.01.002
DO - 10.1016/j.ijhydene.2018.01.002
M3 - Article
AN - SCOPUS:85041588116
SN - 0360-3199
VL - 43
SP - 4177
EP - 4185
JO - International Journal of Hydrogen Energy
JF - International Journal of Hydrogen Energy
IS - 9
ER -
