Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2019-07-18 , DOI: 10.1016/j.cej.2019.122282 Jiazhen Liao , Wen Cui , Jieyuan Li , Jianping Sheng , Hong Wang , Xing'an Dong , Peng Chen , Guangming Jiang , Zhiming Wang , Fan Dong
By heating g-C3N4 powder in the hydrogen atmosphere, nitrogen defects were introduced into the framework of g-C3N4 where the nitrogen atoms in g-C3N4 were reacted and partially removed with hydrogen. The effects of nitrogen defects on the electronic structure, optical properties, generation of reactive oxygen species and photocatalytic NO oxidation of g-C3N4 were investigated by combining experimental characterization and DFT theoretical calculations. The N defect is located at N2C sites and can be tuned by the H2 treating temperature. The obtained N defective g-C3N4 products possessed narrower bandgap adjusted by surface N defects and were able to promote the separation of photoexcited charge carries and produce reactive oxygen species more efficiently than pristine g-C3N4. The NO+ reaction intermediate was formed on the N defects sites and enabled an accelerated photocatalytic reaction that contributed to enhanced photocatalytic NO removal. The NO removal ratio on N defects g-C3N4 obtained at 600 °C (CH-H-600) was 2.6 times that of pristine g-C3N4 under visible light irradiation. The present work could provide new insights into the understanding of the role of N-defects in g-C3N4 and application of photocatalytic technology for efficient air purification.
中文翻译:
H 2处理的gC 3 N 4对氮缺陷结构和NO +中间体促进的光催化NO的去除
通过加热GC 3 Ñ 4中的氢气氛粉末,氮缺陷引入的GC的框架3 Ñ 4其中GC的氮原子3 Ñ 4进行反应,并用氢气部分地去除。结合实验表征和DFT理论计算,研究了氮缺陷对gC 3 N 4的电子结构,光学性质,活性氧的生成和光催化NO氧化的影响。N缺陷位于N 2C位置,可以通过H 2处理温度进行调整。得到的N缺陷gC 3N 4产物具有通过表面N缺陷调节的较窄的带隙,并且能够比原始gC 3 N 4促进光激发电荷载流子的分离并更有效地产生活性氧。NO +反应中间体在N个缺陷位点上形成,并能够促进光催化反应,从而促进了光催化NO的去除。在可见光照射下,在600°C(CH-H-600)下获得的N缺陷gC 3 N 4的NO去除率是原始gC 3 N 4的2.6倍。目前的工作可以为理解N缺陷在gC中的作用提供新的见解。3 N 4和光催化技术在高效空气净化中的应用。