• 文献标题:   Catalyzed Hydrolysis of Tetrahydroxydiboron by Graphene Quantum Dot-Stabilized Transition-Metal Nanoparticles for Hydrogen Evolution
  • 文献类型:   Article
  • 作  者:   CHEN WF, SHEN AL, HUANG YP, LIU X, ASTRUC D
  • 作者关键词:   nanoparticle, b2 oh 4, h2 evolution, kinetic isotopic effect, graphene quantum dot, d2
  • 出版物名称:   ACS SUSTAINABLE CHEMISTRY ENGINEERING
  • ISSN:   2168-0485
  • 通讯作者地址:   China Three Gorges Univ
  • 被引频次:   2
  • DOI:   10.1021/acssuschemeng.0c02496
  • 出版年:   2020

▎ 摘  要

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.