A cocoon silk chemistry strategy to ultrathin N-doped carbon nanosheet with metal single-site catalysts

Youqi Zhu, Wenming Sun, Jun Luo, Wenxing Chen, Tai Cao, Lirong Zheng, Juncai Dong, Jian Zhang, Maolin Zhang, Yunhu Han, Chen Chen, Qing Peng, Dingsheng Wang*, Yadong Li

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

227 Citations (Scopus)

Abstract

Development of single-site catalysts supported by ultrathin two-dimensional (2D) porous matrix with ultrahigh surface area is highly desired but also challenging. Here we report a cocoon silk chemistry strategy to synthesize isolated metal single-site catalysts embedded in ultrathin 2D porous N-doped carbon nanosheets (M-ISA/CNS, M = Fe, Co, Ni). X-ray absorption fine structure analysis and spherical aberration correction electron microscopy demonstrate an atomic dispersion of metal atoms on N-doped carbon matrix. In particular, the Co-ISA/CNS exhibit ultrahigh specific surface area (2105 m2 g−1) and high activity for C–H bond activation in the direct catalytic oxidation of benzene to phenol with hydrogen peroxide at room temperature, while the Co species in the form of phthalocyanine and metal nanoparticle show a negligible activity. Density functional theory calculations discover that the generated O = Co = O center intermediates on the single Co sites are responsible for the high activity of benzene oxidation to phenol.

Original languageEnglish
Article number3861
JournalNature Communications
Volume9
Issue number1
DOIs
Publication statusPublished - 1 Dec 2018
Externally publishedYes

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