Journal
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
Volume 8, Issue 19, Pages 7513-7522Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.0c02496
Keywords
nanoparticles; B-2(OH)(4); H-2 evolution; kinetic isotopic effect; graphene quantum dots; D-2
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Funding
- National Natural Science Foundation of China [21805166]
- 111 Project [D20015]
- Engineering Research Center of Eco-environment in Three Gorges Reservoir Region, Ministry of Education, China Three Gorges University [KF2019-05]
- Universite de Bordeaux
- CNRS
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The search of new H-2 evolution systems avoiding fossil sources and their mechanisms is a priority in the 21st century society. Hydrolysis of tetrahydroxydiboron (TDB), a current borylation source in the literature, is used here for H-2 evolution for the first time. It is catalyzed by graphene quantum dot-stabilized nanoparticles (NPs). With RhNP- or PtNP-catalyzed reactions, D-2 formation from D2O confirms that water is the only hydrogen source. Kinetic isotopic effects yield k(H)/k(D) = 5.91 and 4.18, strongly suggesting double water O-H bond cleavage on the NP surface in the rate-limiting step. The most efficient catalysts are the RhNP and PtNP (total turnover frequencies: 3658 and 4603 mol(H2).mol(cat)(-1).min(-1), respectively). The order of catalytic activity is as follows: PtNP > RhNP > AuNP > PdNP > IrNP > RuNP, and a catalytic mechanism of TDB hydrolysis is proposed.
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