期刊
NANO RESEARCH
卷 15, 期 3, 页码 1983-1992出版社
TSINGHUA UNIV PRESS
DOI: 10.1007/s12274-021-3849-2
关键词
mesoporous silica; metal-organic frameworks (MOF); semi-hydrogenation of phenylacetylene; synergistic effect; single site
类别
资金
- Beijing Natural Science Foundation [2182061]
- Science Foundation of China University of Petroleum, Beijing [2462019BJRC001]
A mesoporous silica stabilized Pd-Ru@ZIF-8 nanoreactor was designed and showed superior performance in selective semi-hydrogenation of phenylacetylene to styrene, with high conversion and selectivity. The synergistic effect of single-site Pd and Ru anchored into the ZIF-8 framework contributed to the enhanced catalytic activity.
Selective semi-hydrogenation of phenylacetylene to styrene is a crucial step in the polystyrene industry. Although Pd-based catalysts are widely used in this reaction due to their excellent hydrogenation activity, the selectivity for styrene remains a great challenge. Herein, we designed a mesoporous silica stabilized Pd-Ru@ZIF-8 (MS Pd-Ru@ZIF-8) nanoreactor with novel Pd and Ru single site synergistic catalytical system for semi-hydrogenation of phenylacetylene. The nanoreactor exhibited a superior performance, achieving 98% conversion of phenylacetylene and 96% selectivity to styrene. Turnover frequency (TOF) of nanoreactor was up to as high as 2,188 h(-1), which was 25 times and 5 times more than the single metal species catalysts, mesoporous silica stabilized Pd@ZIF-8 nanoreactor (MS Pd@ZIF-8), and mesoporous silica stabilized Ru@ZIF-8 nanoreactor (MS Ru@ZIF-8). This catalytic activity was attributed to the synergistic effect of Pd and Ru single site anchored strongly into the framework of ZIF-8, which reduced the desorption energy of styrene and increased the hydrogenation energy barrier of styrene. Importantly, since the ordered mesoporous silica was introduced into the nanoreactor shell to stabilize ZIF-8, MS Pd-Ru@ZIF-8 showed excellent reusability and stability. After the five cycles, the catalytical activity and selectivity still remained. This work provides insights for a synergistic catalytic system based on single-site active sites for selective hydrogenation reactions.
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