期刊
ACS APPLIED MATERIALS & INTERFACES
卷 9, 期 37, 页码 31853-31860出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.7b08691
关键词
solid-state synthesis; Au-Ni bimetallic nanoparticle; activation of oxygen; gas-phase selective oxidation of alcohol; bimetallic nanophase diagram
资金
- Shell Global Solutions International B.V. [PT71423]
- National Natural Science Foundation of China [21271153, 21373181, 21222307, U1402233]
- Major Research Plan Of National Natural Science Foundation of China [91545113]
- Fok Ying Tung Education Foundation [131015]
- Fundamental Research Funds for the Central Universities [2014XZZX003-02, 2017FZA3007]
A facile confined solid-state seed-mediated alloying strategy is applied for the rational synthesis of supported Au-Ni bimetallic nanoparticles (BMNPs). The method sequentially deposits nickel salts and AuNP seeds into the ordered array of extra-large mesopores (EP-FDU-12 support) followed by a high-temperature annealing process. The size, structure, and composition of the AuNi BMNPs can be well tuned by varying the AuNP seeds, annealing temperature, and feeding ratio of metal precursors. Kinetic studies and DFT calculations suggest that the introduction of the Ni component can significantly prompt the 02 activation on AuNPs, which is critical for the selective alcohol oxidation using molecular 02 as the oxidant. The optimal Au-Ni BMNP catalyst showed the highest turnover frequency (TOE) (59 000 h(-1), 240 degrees C) and highest space-time yield (STY) of benzyl aldehyde (BAD) productivity (9.23 kg.g(Au)(-1).h(-1)) in the gas-phase oxidation of benzyl alcohol (BA), which is at least about 5-fold higher than that of other supported Au catalysts.
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