期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 139, 期 32, 页码 10976-10979出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.7b05372
关键词
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资金
- China Ministry of Science and Technology [2016YFA (0202801)]
- National Natural Science Foundation of China [21521091, 21390393, U1463202, 21471089, 21671117]
Preparing metal single-atom materials is currently attracting tremendous attention and remains a significant challenge. Herein, we report a novel core-shell strategy to synthesize single-atom materials. In this strategy, metal hydroxides or oxides are coated with polymers, followed by high-temperature pyrolysis and acid leaching, metal single atoms are anchored on the inner wall of hollow nitrogen-doped carbon (CN) materials. By changing metal precursors or polymers, we demonstrate the successful synthesis of different metal single atoms dispersed on CN materials (SA-M/CN, M = Fe, Co, Ni, Mn, FeCo, FeNi, etc.). Interestingly, the obtained SA-Fe/CN exhibits much higher catalytic activity for hydroxylation of benzene to phenol than Fe nanoparticles/CN (45% vs 5% benzene conversion). First-principle calculations further reveal that the high reactivity originates from the easier formation of activated oxygen species at the single Fe site. Our methodology provides a convenient route to prepare a variety of metal single-atom materials representing a new class of catalysts.
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