title: Iron-Doped Carbon Nitride-Type Polymers as Homogeneous Organocatalysts for Visible Light-Driven Hydrogen Evolution.
abstract: Graphitic carbon nitrides have appeared as a new type of photocatalyst for water splitting, but their broader and more practical applications are oftentimes hindered by the insolubility or difficult dispersion of the material in solvents. We herein prepared novel two-dimensional (2D) carbon nitride-type polymers doped by iron under a mild one-pot method through preorganizing formamide and citric acid precursors into supramolecular structures, which eventually polycondensed into a homogeneous organocatalyst for highly efficient visible light-driven hydrogen evolution with a rate of ∼16.2 mmol g(-1) h(-1) and a quantum efficiency of 0.8%. Laser photolysis and electrochemical impedance spectroscopic measurements suggested that iron-doping enabled strong electron coupling between the metal and the carbon nitride and formed unique electronic structures favoring electron mobilization along the 2D nanomaterial plane, which might facilitate the electron transfer process in the photocatalytic system and lead to efficient H2 evolution. In combination with electrochemical measurements, the electron transfer dynamics during water reduction were depicted, and the earth-abundant Fe-based catalyst may open a sustainable strategy for conversion of sunlight into hydrogen energy and cope with current challenging energy issues worldwide.
authors.affiliation: State Key Laboratory of Applied Organic Chemistry (SKLAOC), Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, College of Chemistry and Chemical Engineering, Key Laboratory of Special Function Materials and Structure Design, Ministry of Education, Lanzhou University , Lanzhou, 730000, China.
authors.forename: Lin-Feng
authors.initials: LF
authors.lastname: Gao
authors.affiliation: State Key Laboratory of Applied Organic Chemistry (SKLAOC), Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, College of Chemistry and Chemical Engineering, Key Laboratory of Special Function Materials and Structure Design, Ministry of Education, Lanzhou University , Lanzhou, 730000, China.
authors.forename: Ting
authors.initials: T
authors.lastname: Wen
authors.affiliation: State Key Laboratory of Applied Organic Chemistry (SKLAOC), Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, College of Chemistry and Chemical Engineering, Key Laboratory of Special Function Materials and Structure Design, Ministry of Education, Lanzhou University , Lanzhou, 730000, China.
authors.forename: Jing-Yin
authors.initials: JY
authors.lastname: Xu
authors.affiliation: State Key Laboratory of Applied Organic Chemistry (SKLAOC), Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, College of Chemistry and Chemical Engineering, Key Laboratory of Special Function Materials and Structure Design, Ministry of Education, Lanzhou University , Lanzhou, 730000, China.
authors.forename: Xin-Ping
authors.initials: XP
authors.lastname: Zhai
authors.affiliation: State Key Laboratory of Applied Organic Chemistry (SKLAOC), Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, College of Chemistry and Chemical Engineering, Key Laboratory of Special Function Materials and Structure Design, Ministry of Education, Lanzhou University , Lanzhou, 730000, China.
authors.forename: Min
authors.initials: M
authors.lastname: Zhao
authors.affiliation: State Key Laboratory of Applied Organic Chemistry (SKLAOC), Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, College of Chemistry and Chemical Engineering, Key Laboratory of Special Function Materials and Structure Design, Ministry of Education, Lanzhou University , Lanzhou, 730000, China.
authors.forename: Guo-Wen
authors.initials: GW
authors.lastname: Hu
authors.affiliation: School of Pharmacy, Lanzhou University , Lanzhou, 730020, China.
authors.forename: Peng
authors.initials: P
authors.lastname: Chen
authors.affiliation: State Key Laboratory of Applied Organic Chemistry (SKLAOC), Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, College of Chemistry and Chemical Engineering, Key Laboratory of Special Function Materials and Structure Design, Ministry of Education, Lanzhou University , Lanzhou, 730000, China.
authors.forename: Qiang
authors.initials: Q
authors.lastname: Wang
authors.affiliation: State Key Laboratory of Applied Organic Chemistry (SKLAOC), Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, College of Chemistry and Chemical Engineering, Key Laboratory of Special Function Materials and Structure Design, Ministry of Education, Lanzhou University , Lanzhou, 730000, China.
authors.forename: Hao-Li
authors.initials: HL
authors.lastname: Zhang
keywords: carbon nitride; hydrogen evolution; laser photolysis; two-dimensional; visible light-driven photocatalysis