期刊
JOURNAL OF COLLOID AND INTERFACE SCIENCE
卷 634, 期 -, 页码 1005-1013出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcis.2022.12.063
关键词
Carbon nitride; Bromine doping; Photocatalytic CO2 reduction; CH4; Charge separation
The direct conversion of CO2 into reusable CH4 fuel by solar energy can effectively solve the problems of energy crisis and carbon emissions. However, the challenge of photocatalytic CO2 reduction to produce CH4 is still low conversion efficiency and poor selectivity. This research demonstrates the fabrication of surface brominated carbon nitride (CNBr) as a stable and efficient photocatalyst for CO2 reduction to produce CH4, with a high rate (16.68 lmol h-1 g-1) and selectivity (70.27%). The incorporation of bromine atoms in CNBr enhances local charge separation, narrows the bandgap, and deepens the conduction band, enabling enriched CO2 adsorption and subsequent CH4 formation through hydrogenation.
The direct conversion of CO2 into reusable CH4 fuel by solar energy can effectively solve the problems of energy crisis and carbon emissions. However, the challenge of photocatalytic CO2 reduction to produce CH4 is still low conversion efficiency and poor selectivity. Here, surface brominated carbon nitride (named CNBr) is fabricated for stable and efficient photocatalytic CO2 reduction to produce CH4 with a rate of 16.68 lmol h-1 g-1 (70.27 % selectivity). Br atom in CNBr can substitute the N atom in the tris-triazine unites, which promotes local charge separation, narrows band gap and deepens the conduction band of CNBr. Benefiting from Br as active sites, CO2 can be enriched on the catalyst surface, and localized photogenerated electrons can activate the adsorbed CO2 to form CH4 through subsequent hydrogenation. Density functional theory results suggest that Br doping can effectively reduce the energy barrier of the rate-limiting step, accelerate the reaction, and induce the formation of *CHO, thereby improving the selectivity of CH4. This work reveals that surface modification can simultaneously increase the activation site of CO2 adsorption activation, enhance light absorption and accelerate charge, laying a solid foundation for the future design of carbon nitride based photocatalyst with high performance.(c) 2022 Elsevier Inc. All rights reserved.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据