Journal
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
Volume 9, Issue 3, Pages 1333-1340Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.0c07930
Keywords
nitrogen self-doped; photocatalytic CO2 conversion; covalent triazine-based framework; selectivity
Categories
Funding
- National Natural Science Foundation of China [51672047, 21707173, 51672048]
- National Natural Science Foundation of Fujian Province [2019 J01648, 2019 J01226]
- Youth Talent Support Program of Fujian Province [00387077]
- Independent Research Project of State Key Laboratory of Photocatalysis on Energy and Environment [2014C03]
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A novel nitrogen self-doped covalent triazine-based framework (NCTF-1) was prepared for photocatalytic CO2 reduction to CH4 under visible light, exhibiting a high CH4 evolution rate and selectivity for CO2 conversion.
Photocatalytic reduction of carbon dioxide to hydrocarbon fuel provides a sustainable strategy for addressing the increasing energy crisis as well as alleviating the greenhouse effect. Yet, seeking effective, affordable, and metal-free photo-catalysts is still a challenging issue. Herein, a novel nitrogen self-doped covalent triazine-based framework (NCTF-1) was prepared via a simple hydrothermal process for photocatalytic CO2 reduction to CH4 using visible light. NCTF-1 exhibited a CH4 evolution rate of 11.48 pmol h(-1), corresponding to ninefold enhancement, compared with bare covalent triazine-based frameworks (CTF-1). The photocatalytic enhancement mechanism was probed by a variety of instrumental measurements. Results showed that the modification of nitrogen atoms in NCTF-1 could extend the responsive range of the visible-light spectrum, promote CO2 capture, and thus greatly elevate the photocatalytic CO2 reduction activity. Notably, NCTF-1 displayed a satisfactory selectivity for CO2 conversion with CH4 accounting for over 85% of the reduction products. This study offers a promising avenue for achieving robust CO2-to-CH4 conversion and provides insight into the impact of nitrogen self-doping on covalent triazine-based frameworks.
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