Defect enriched N-doped carbon nanoflakes as robust carbocatalysts for H2S selective oxidation
| Autor: | Chi Xu, Yuefeng Liu, Cuong Pham-Huu, Congmei Chen, Qian Jiang, Ning Cao, Qingqing Gu, Shiyan Li, Chengfa Jiang |
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| Rok vydání: | 2020 |
| Předmět: |
Dopant
Renewable Energy Sustainability and the Environment Doped carbon Rational design chemistry.chemical_element 02 engineering and technology General Chemistry 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences Nitrogen 0104 chemical sciences Catalysis Flue-gas desulfurization chemistry Chemical engineering Impurity General Materials Science 0210 nano-technology Carbon |
| Zdroj: | Journal of Materials Chemistry A. 8:8892-8902 |
| ISSN: | 2050-7496 2050-7488 |
| DOI: | 10.1039/d0ta00212g |
| Popis: | 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. |
| Databáze: | OpenAIRE |
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