The mechanism of the chain-growth of ammoniaborane: A classic Lewis pairs catalysed by a Frustrated Lewis Pairs

The mechanism of the chain-growth of ammoniaborane: A classic Lewis pairs catalysed by a Frustrated Lewis Pairs
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氨硼烷的链增长机制:受阻路易斯对催化的经典路易斯对

DOI:
10.1016/j.ijhydene.2018.01.002
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发表时间:
2018-03
影响因子:
7.2
通讯作者:
Yu Xuebin
Yu Xuebin
中科院分区:
工程技术2区
文献类型:
--
作者:
Wang Kun;Cheng Longjiu;Zhang Jianguo;Yu Xuebin

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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 Bsingle bondN 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 Bsingle bondN chain (2) and an intermolecular dehydrogenation between terminal N-Hδ+andδ−Hsingle bondB (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.
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