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

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.

SUBMITTER: Zhu Y 

PROVIDER: S-EPMC6155020 | biostudies-literature | 2018 Sep

REPOSITORIES: biostudies-literature