Single-Atom Pd1/Graphene Catalyst Achieved by Atomic Layer Deposition: Remarkable Performance in Selective Hydrogenation of 1,3-Butadiene
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- 作者：Huan Yan ; Hao Cheng ; Hong Yi ; Yue Lin ; Tao Yao ; Chunlei Wang ; Junjie Li ; Shiqiang Wei ; Junling Lu
- 刊名：Journal of the American Chemical Society
- 出版年：2015
- 出版时间：August 26, 2015
- 年：2015
- 卷：137
- 期：33
- 页码：10484-10487
- 全文大小：362K
- ISSN：1520-5126
文摘
We reported that atomically dispersed Pd on graphene can be fabricated using the atomic layer deposition technique. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure spectroscopy both confirmed that isolated Pd single atoms dominantly existed on the graphene support. In selective hydrogenation of 1,3-butadiene, the single-atom Pd1/graphene catalyst showed about 100% butenes selectivity at 95% conversion at a mild reaction condition of about 50 掳C, which is likely due to the changes of 1,3-butadiene adsorption mode and enhanced steric effect on the isolated Pd atoms. More importantly, excellent durability against deactivation via either aggregation of metal atoms or carbonaceous deposits during a total 100 h of reaction time on stream was achieved. Therefore, the single-atom catalysts may open up more opportunities to optimize the activity, selectivity, and durability in selective hydrogenation reactions.