Platinum and Other Transition Metal Nanoclusters (Pd, Rh) Stabilized by PAMAM Dendrimer as Excellent Heterogeneous Catalysts: Application to the Methylcyclopentane (MCP) Hydrogenative Isomerization

被引:60
作者
Deraedt, Christophe [1 ,2 ]
Melaet, Gerome [1 ,2 ]
Ralston, Walter T. [1 ,2 ]
Ye, Rong [1 ,2 ]
Somorjai, Gabor A. [1 ,2 ]
机构
[1] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA
[2] Univ Calif Berkeley, Chem Sci Div, Berkeley, CA 94720 USA
基金
美国能源部;
关键词
Nanoparticle; dendrimer; heterogeneous catalysis; MCP; C-C breaking; PALLADIUM NANOPARTICLES; MESOPOROUS ZEOLITES; CLICK DENDRIMERS; ENCAPSULATED PD; CONVERSION; NANOCOMPOSITES; SELECTIVITY; EFFICIENT; SUPPORT; SILICA;
D O I
10.1021/acs.nanolett.6b05156
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Pt, Rh, and Pd nanoclusters stabilized by PAMAM dendrimer are used for the first time in a gas flow reactor at high temperature (150-250 degrees C). Pt nanoclusters show a very high activity for the hydrogenation of the methylcyclopentane (MCP) at 200-225 degrees C with turnover freqency (TOF) up to 334 h(-1) and selectivity up to 99.6% for the ring opening isomerization at very high conversion (94%). Rh nanoclusters show different selectivity for the reaction, that is, ring opening isomerization at 175 degrees C and cracking at higher temperature whereas Pd nanoclusters perform ring enlargement plus dehydrogenation, while maintaining a high activity. The difference in these results as compared to unsupported/uncapped nanoparticles, demonstrates the crucial role of dendrimer. The tenability of the selectivity of the reaction as well as the very high activity of the metal nanoclusters stabilized by dendrimer under heterogeneous conditions open a new application for dendrimer catalysts.
引用
收藏
页码:1853 / 1862
页数:10
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