Che Huinan, Che Guangbo, Zhou Pengjie, Song Ning, Li Chunxue, Li Chunmei, Liu Chunbo, Liu Xiaoteng, Dong Hongjun
School of the Environment and Safety Engineering, Jiangsu University, China; Institute of Green Chemistry and Chemical Technology, School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, China.
Key Laboratory of Preparation and Applications of Environmental Friendly Materials, Jilin Normal University, Ministry of Education, Changchun 130103, China.
J Colloid Interface Sci. 2019 Jul 1;547:224-233. doi: 10.1016/j.jcis.2019.03.106. Epub 2019 Apr 1.
Precursor-reforming strategy induced graphitic carbon nitride (g-CN) with different morphologies for enhanced photocatalytic hydrogen (H) evolution activity is highly desirable. Herein, g-CN microtubes (mg-CN) with adjustable closure degree of microtube orifice and spatial anisotropic charge separation are established by conquering hydrogen bond during thermally exfoliate precursor. Compared to the bulk g-CN (bg-CN) and ultrathin g-CN (ug-CN), the tubular structure endows mg-CN with spatial anisotropic charge separation that accelerates transfer of charge carriers. As expected, the photocatalytic H evolution (PHE) activity of mg-CN has been obviously enhanced. Particularly, the mg-CN-24 shows the best PHE activity (957.9 μmol h g), which is over 18.72 and 3.77 times higher than the bg-CN and ug-CN, respectively. In addition, selective photo-deposition experiment results reveal a charge carriers migration behavior that photoproduction electrons migrate to the outer shell and holes prefer to move onto the inner shell of mg-CN, thus achieving efficient spatial anisotropic charge separation. We firmly believe that the work presents significant advancement for the design of other materials by precursor-reforming strategy.
前驱体重整策略诱导具有不同形貌的石墨相氮化碳(g-CN)以增强光催化析氢(H)活性是非常可取的。在此,通过在热剥离前驱体过程中克服氢键,建立了具有可调节微管孔封闭度和空间各向异性电荷分离的g-CN微管(mg-CN)。与块状g-CN(bg-CN)和超薄g-CN(ug-CN)相比,管状结构赋予mg-CN空间各向异性电荷分离,加速了电荷载流子的转移。正如预期的那样,mg-CN的光催化析氢(PHE)活性得到了明显增强。特别是,mg-CN-24表现出最佳的PHE活性(957.9 μmol h g),分别比bg-CN和ug-CN高18.72倍和3.77倍以上。此外,选择性光沉积实验结果揭示了一种电荷载流子迁移行为,即光生电子迁移到mg-CN的外壳,而空穴则倾向于迁移到内壳,从而实现了有效的空间各向异性电荷分离。我们坚信这项工作为通过前驱体重整策略设计其他材料带来了重大进展。