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 () and Yadong Li ()
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Youqi Zhu: Tsinghua University
Wenming Sun: China Building Materials Academy
Jun Luo: Tianjin University of Technology
Wenxing Chen: Tsinghua University
Tai Cao: Tsinghua University
Lirong Zheng: Chinese Academy of Sciences
Juncai Dong: Chinese Academy of Sciences
Jian Zhang: Tsinghua University
Maolin Zhang: Tsinghua University
Yunhu Han: Tsinghua University
Chen Chen: Tsinghua University
Qing Peng: Tsinghua University
Dingsheng Wang: Tsinghua University
Yadong Li: Tsinghua University

Nature Communications, 2018, vol. 9, issue 1, 1-9

Abstract: 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.

Date: 2018
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DOI: 10.1038/s41467-018-06296-w

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