Citation: Wei Hong, Xiaoqing Yan, Renhong Li, Jie Fan. Gold nanoparticle stabilization within tailored cubic mesoporous silica: Optimizing alcohol oxidation activity[J]. Chinese Journal of Catalysis, ;2017, 38(3): 545-553. doi: 10.1016/S1872-2067(17)62762-1 shu

Gold nanoparticle stabilization within tailored cubic mesoporous silica: Optimizing alcohol oxidation activity

Wei Hong ^a, ,
Xiaoqing Yan ^b ,
Renhong Li ^a,b ,
Jie Fan ^a

a Key Laboratory of Applied Chemistry of Zhejiang Province, Department of Chemistry, Zhejiang University, Hangzhou 310027, Zhejiang, China;
b Key Laboratory of Advanced Textile Materials and Manufacturing Technology, Ministry of Education of China, Zhejiang Sci-Tech University, Hangzhou 310018, Zhejiang, China

Received Date: 20 October 2016
Revised Date: 6 December 2016

Fund Project: This work was supported by the National Natural Science Foundation of China (21222307, 21373181, 21403197, 91545113, 21503189), the Fundamental Research Funds for the Central Universities (2014XZZX003-02), Zhejiang Provincial Natural Science Foundation (LY15B030009), and China Postdoctoral Science Foundation (2014M550333, 2015T80636).

Stabilizing gold nanoparticles (AuNPs) within a desired size range is critical to realize their promising catalytic performance in many important reactions. Herein, we investigate the anti-sintering properties of cubic mesoporous silica (FDU-12) as a function of pore entrance size. Simple adjustments to the type of organic template and reaction temperature enable the successful synthesis of FDU-12 with controllable entrance sizes (< 3, 3-5 and 7 nm). Excellent anti-sintering properties are observed for FDU-12 with a sub-5-nm entrance size (3-5 nm) over a wide loading concentration (1.0-8.3 wt%) and the AuNPs can be stabilized within a 4.5-5.0-nm range after calcination at 550℃ in air for 5 h. Smaller entrance size (< 3 nm) prevents ingress of 3-nm AuNPs to the mesopores and results in low loading capacity and sintering. Conversely, FDU-12 possessing a larger entrance size (7 nm) shows promising anti-sintering properties at high loading concentrations, although catalytic performance is significantly lost at lower concentrations (e.g. 2.1 wt%, 14.2 ± 5.5 nm). Different anti-sintering mechanisms are proposed for each of the different FDU-12 entrance sizes. Additionally, catalytic data indicates that the obtained 4.5-nm AuNPs supported on FDU-12 with a sub-5-nm entrance size exhibit excellent mass-specific activity (1544 mmol g_Au^-1 h^-1) and selectivity (> 99%) at 230℃ for the gas-phase selective oxidation of cyclohexanol.
- Gold nanoparticle,
- Cubic mesoporous silica,
- Entrance size,
- Anti-sintering property,
- Alcohol oxidation
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