Issue 18, 2020

Defect enriched N-doped carbon nanoflakes as robust carbocatalysts for H2S selective oxidation

Abstract

Nanocarbons have emerged as low-cost, efficient and durable nonmetallic catalysts for H2S selective oxidation. However, the most efficient active sites for H2S activation remain elusive, which restricts further development of high-performance catalysts for industrial application. Herein, we report on the synthesis of N-doped carbon nanoflakes with tunable nitrogen dopants and abundant structural defects for H2S selective oxidation. These defect enriched N-doped carbon nanoflakes exhibited significantly enhanced catalytic performance (>740 gsulfur kgcat.−1 h−1), stability (>110 h) and decent tolerance to impurity gas (CO2) and steam toward continuous H2S selective oxidation. Combined advanced characterization, control experiments and theoretical simulation showed that the N species along with defects on N-doped carbon nanoflakes could enhance significantly the catalytic activity, and further confirmed that the pyridinic N was the most active species and the C atoms adjacent to N atoms exhibit strong interaction with HS. Our study provides predictive guidelines for the rational design of highly efficient and durable carbocatalysts for continuous catalytic oxidative desulfurization.

Graphical abstract: Defect enriched N-doped carbon nanoflakes as robust carbocatalysts for H2S selective oxidation

Supplementary files

Article information

Article type
Paper
Submitted
06 Jan 2020
Accepted
01 Mar 2020
First published
02 Mar 2020

J. Mater. Chem. A, 2020,8, 8892-8902

Defect enriched N-doped carbon nanoflakes as robust carbocatalysts for H2S selective oxidation

S. Li, Q. Gu, N. Cao, Q. Jiang, C. Xu, C. Jiang, C. Chen, C. Pham-Huu and Y. Liu, J. Mater. Chem. A, 2020, 8, 8892 DOI: 10.1039/D0TA00212G

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