5 years ago

Metal (Hydr)oxides@Polymer Core–Shell Strategy to Metal Single-Atom Materials

Metal (Hydr)oxides@Polymer Core–Shell Strategy to Metal Single-Atom Materials
Wenxing Chen, Shubo Tian, Jun Luo, Lirong Zheng, Dingsheng Wang, Yang-Gang Wang, Maolin Zhang, Weng-Chon Cheong, Jiawei Wan, Yadong Li, Juncai Dong
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.

Publisher URL: http://dx.doi.org/10.1021/jacs.7b05372

DOI: 10.1021/jacs.7b05372

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