title: Insights into enhanced visible-light photocatalytic activity of C60modified g-C3N4hybrids: the role of nitrogen.
abstract: Recent experiments have shown that the photocatalytic activity of g-C3N4can be greatly enhanced by C60modification, however, a fundamental understanding of its mechanistic operation is still lacking. Using first-principles calculations, the interfacial effects of C60/g-C3N4nanocomposites on the electronic properties, charge transfer and optical response have been explored in detail. For different stacking patterns, the two constituents are always linked by van der Waals (vdW) forces without any exception, and form type-II heterojunctions in most cases. The valence band maximum and conduction band minimum of these heterostructures are dominated by the unsaturated nitrogen (N2) atoms and C60molecule, respectively, which strongly interact with each other, resulting in strong charge transfer between the two involved constituents and an obvious bending of the g-C3N4sheets. The unsaturated N2atoms included in the interfaces have a significant influence on promoting the photocatalytic performance, while the existence of saturated nitrogen (N1and N3) atoms lying in the interfaces will weaken the interfacial interactions between C60molecules and the g-C3N4monolayers. Moreover, the sensitive optical response and satisfactory type-II band alignment clearly show that the C60/g-C3N4heterostructure is an outstanding photocatalyst for hydrogen production. We proposed a deep insight (the role of nitrogen) into understanding the improved photocatalytic ability of the C60/g-C3N4nanocomposites, which may contribute to the rational design of both C60/g-C3N4and g-C3N4-based nanocomposite photocatalysts.
authors.affiliation: School of Physics and Electronics, Hunan University, Changsha 410082, China. liangxu@hnu.edu.cn wqhuang@hnu.edu.cn.
authors.forename: Quan
authors.initials: Q
authors.lastname: Li
authors.affiliation: School of Physics and Electronics, Hunan University, Changsha 410082, China. liangxu@hnu.edu.cn wqhuang@hnu.edu.cn and College of Materials Science and Engineering, Hunan University, Changsha 410082, China.
authors.forename: Liang
authors.identifier: http://orcid.org/0000-0001-7473-6107
authors.initials: L
authors.lastname: Xu
authors.affiliation: Physical and Electronic Engineering Department, Tongren University, Tongren 554300, Guizhou, China.
authors.forename: Kai-Wu
authors.initials: KW
authors.lastname: Luo
authors.affiliation: School of Physics and Electronics, Hunan University, Changsha 410082, China. liangxu@hnu.edu.cn wqhuang@hnu.edu.cn.
authors.forename: Wei-Qing
authors.initials: WQ
authors.lastname: Huang
authors.affiliation: School of Physics and Electronics, Hunan University, Changsha 410082, China. liangxu@hnu.edu.cn wqhuang@hnu.edu.cn.
authors.forename: Ling-Ling
authors.initials: LL
authors.lastname: Wang
authors.affiliation: School of Optoelectronic Information, University of Electronic Science and Technology of China, Chengdu 610054, China.
authors.forename: Xiao-Fei
authors.initials: XF
authors.lastname: Li
authors.affiliation: School of Physics and Electronics, Hunan University, Changsha 410082, China. liangxu@hnu.edu.cn wqhuang@hnu.edu.cn.
authors.forename: Gui-Fang
authors.initials: GF
authors.lastname: Huang
authors.affiliation: School of Physics and Electronics, Hunan University, Changsha 410082, China. liangxu@hnu.edu.cn wqhuang@hnu.edu.cn.
authors.forename: Ya-Bin
authors.initials: YB
authors.lastname: Yu