期刊
JOURNAL OF PHYSICAL CHEMISTRY A
卷 120, 期 8, 页码 1135-1144出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpca.5b11156
关键词
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资金
- University of Michigan Energy Institute
- National Science Foundation [1256260]
- NSF CAREER award [1551994]
- Direct For Education and Human Resources [1256260] Funding Source: National Science Foundation
- Direct For Mathematical & Physical Scien [1551994] Funding Source: National Science Foundation
- Division Of Chemistry [1551994] Funding Source: National Science Foundation
- Division Of Graduate Education [1256260] Funding Source: National Science Foundation
This study employs computational reaction finding tools to probe the unique biphilic reactivity between ammonia-borane (AB) and CO2. The results show that sequential reactions involving multiple equivalents of AB and CO2 can lead to the formation of stable nonplanar B,C,N,O-heterocycles (Cy-BCN). Cy-BCN is shown to emerge through boron-oxygen bond formation, hydroboration, dative bond formation, and single- or double-hydrogen transfers. The most kinetically facile reactions (computed at the coupled cluster singles and doubles with perturbative triples (CCSD(T)) level of theory) result from polarized nitrogen-boron double bonds whereas thermodynamic stability results from formation of covalent boron-oxygen bonds. An important structure, HCOOBHNH2 (DHFAB), contains both of these features and is the key intermediate involved in generation of Cy-BCN. Crucially, it is shown that favorable boron-oxygen bond formation results in production of Cy-BCN species that are more stable than polyaminoboranes. These types of reaction intermediates could serve as building blocks in the formation of B,N-codoped graphene oxide (BCN).
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