期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 3, 期 45, 页码 22807-22815出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c5ta05487g
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资金
- Program for New Century Excellent Talents in University of the Ministry of Education of China [NCET-13-0846]
- National Natural Science Foundation of China [21101089]
- Inner Mongolia Natural Science Foundation [2011JQ01]
- Program for Young Talents of Science and Technology in Universities of Inner Mongolia Autonomous Region [NJYT-13-A01]
- Program for the Development of Innovative Teams in Universities of Inner Mongolia [NMGIRT1105]
- Program for Science and technology leading talent and innovation team of Inner Mongolia [209182]
Two N-doped carbon materials, N-doped Vulcan XC-72 carbon labelled as NXC and graphite carbon nitride labelled as C3N4, were selected as supports to prepare a series of bimetallic AuM (M = Co, Ni) nanoparticles (NPs) using three different reduction ways towards mixed metal ions AuCl4- and M2+, and then the as-synthesized supported bimetallic AuM NPs were used as catalysts for hydrolytic dehydrogenation of ammonia borane (NH3BH3). All the catalysts exhibited high dispersion and small size of bimetallic NPs; however, they exhibited remarkably different catalytic activities featuring total turnover frequency (TOF) values from 6.4 to 42.1 mol(H2) mol(cat)(-1) min(-1). Among all the catalysts, the NXC-immobilized AuCo NPs through in situ synthesis using NaBH4 and NH3BH3 as reductants exhibited the highest activity with a total TOF value of 42.1 mol(H2) mol(cat)(-1) min(-1), which was among the highest values for Co-based catalysts ever reported for hydrolytic dehydrogenation of NH3BH3. This remarkably enhanced activity may be attributed to the synergistic effect of the N-doped NXC support and AuCo NPs and the resulting highly efficient activation of N-B bond in NH3BH3. In addition, the AuCo catalysts showed good recyclability, demonstrating that they had high stability/durability.
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