期刊
ADVANCED MATERIALS
卷 31, 期 18, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201900509
关键词
freeze drying; nitrogen-doped graphene; Pd single-atom catalysts; photothermal catalysis; selective hydrogenation of acetylene
类别
资金
- National Key Projects for Fundamental Research and Development of China [2017YFA0206904, 2017YFA0206900, 2016YFB0600901, 2018YFB1502002]
- National Natural Science Foundation of China [51825205, U1662118, 51772305, 51572270, 21871279, 21802154]
- Beijing Natural Science Foundation [2191002, 2194089, 2182078]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB17000000]
- Beijing Municipal Science and Technology Project [Z181100005118007]
- K. C. Wong Education Foundation
- Youth Innovation Promotion Association of the CAS
- University of Auckland Faculty Research Development Fund
- Energy Education Trust of New Zealand
- MacDiarmid Institute for Advanced Materials and Nanotechnology
- Royal SocietyNewton Advanced Fellowship [NA170422]
- International Partnership Program of Chinese Academy of Sciences [GJHZ1819]
The selective hydrogenation of acetylene to ethylene in an ethylene-rich gas stream is an important process in the chemical industry. Pd-based catalysts are widely used in this reaction due to their excellent hydrogenation activity, though their selectivity for acetylene hydrogenation and durability need improvement. Herein, the successful synthesis of atomically dispersed Pd single-atom catalysts on nitrogen-doped graphene (Pd-1/N-graphene) by a freeze-drying-assisted method is reported. The Pd-1/N-graphene catalyst exhibits outstanding activity and selectivity for the hydrogenation of C2H2 with H-2 in the presence of excess C2H4 under photothermal heating (UV and visible-light irradiation from a Xe lamp), achieving 99% conversion of acetylene and 93.5% selectivity to ethylene at 125 degrees C. This remarkable catalytic performance is attributed to the high concentration of Pd active sites on the catalyst surface and the weak adsorption energy of ethylene on isolated Pd atoms, which prevents C2H4 hydrogenation. Importantly, the Pd-1/N-graphene catalyst exhibits excellent durability at the optimal reaction temperature of 125 degrees C, which is explained by the strong local coordination of Pd atoms by nitrogen atoms, which suppresses the Pd aggregation. The results presented here encourage the wider pursuit of solar-driven photothermal catalyst systems based on single-atom active sites for selective hydrogenation reactions.
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