Theoretical chemistry (DLPNO-CCSD(T)/def2-TZVP//M06-2x/aug-cc-pVDZ) was used to design a system based on ammonia boranes catalyzed by pyrazoles with the aim of producing dihydrogen, nowadays of high interest as clean fuel. The reactivity of ammonia borane and cyclotriborazane were investigated, including catalytic activation through 1H-pyrazole, 4-methoxy-1H-pyrazole, and 4-nitro-1H-pyrazole. The results point toward a catalytic cycle by which, at the same time, ammonia borane can initially store and then, through catalysis, produce dihydrogen and amino borane. Subsequently, amino borane can trimerize to form cyclotriborazane that, in presence of the same catalyst, can also produce dihydrogen. This study proposes therefore a consistent progress in using environmentally sustainable (metal free) catalysts to efficiently extract dihydrogen from small B-N bonded molecules.
Keywords: ammonia borane; cyclotriborazane; hydrogen storage; organic catalyst; pyrazole.
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