Parallel Interface Engineering of Single‐Atom Pt/g‐C <sub>3</sub> N <sub>4</sub> and Selenoviologen for Durable Photocatalysis via Efficient Directional Electron Flow
Abstract
ABSTRACT Photocatalysis offers a sustainable route for clean energy conversion, yet its efficiency is frequently constrained by uncontrolled charge‐carrier recombination and sluggish interfacial electron transfer. Here, we address this challenge by constructing a parallel photocatalytic interface through the dual covalent binding of selenoviologen electron mediators to defective g‐C 3 N 4 which is anchored with single‐atom Pt. This architecture forms a highly stable “electron overpass” that directs electron flow with exceptional efficiency. Ultrafast spectra and DFT calculations confirm that this overpass channels electrons from both photoexcited g‐C 3 N 4 and selenoviologen radical intermediates directly to the Pt catalytic sites. The system achieves a forward electron transfer rate of 0.043 L·g −1 ·s −1 , four times that of the single covalent binding control, and extends the charge carrier lifetime to 7998.8 ps. As a result, the photocatalyst delivers a remarkable hydrogen evolution rate of 3231.9 µmol·h −1 g −1 , while the concurrent anaerobic oxidation of benzylamine proceeds at 1390.6 µmol·h −1 g −1 . Crucially, the dual covalent binding affords outstanding durability, retaining 92% of the initial activity after six 24 h cycles, a nearly tenfold improvement over the conventional system. This work establishes parallel interface engineering as a general paradigm for directing electron flow, paving the way for advanced solar fuel production and artificial photosynthesis.
Article Details
Authors (10)
Zhaoguang Zhang
Xi’an Jiaotong University , , , ,
Chenjing Liu
Frontier Institute of Science and Technology, Interdisciplinary Research Center of Frontier Science and Technology, State Key Laboratory for Strength and Vibration of Mechanical Structures, Institute of New Concept Sensors and Molecular Materials, Shaanxi Key Laboratory of New Conceptual Sensors and Molecular Materials, Engineering Research Center of Key Materials for Efficient Utilization of Clean Energy of Shaanxi Province, Xi’an Key Laboratory of Electronic Devices and Material Chemistry
Jiayao Sha
School of Materials Science & Engineering Chang'an University Xi'an Shaanxi Province P. R. China
Yuxiang Zhang
Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543, Republic of Singapore
Yujing Gao
Frontier Institute of Science and Technology, Interdisciplinary Research Center of Frontier Science and Technology, State Key Laboratory for Strength and Vibration of Mechanical Structures, Institute of New Concept Sensors and Molecular Materials, Shaanxi Key Laboratory of New Conceptual Sensors and Molecular Materials, Engineering Research Center of Key Materials for Efficient Utilization of Clean Energy of Shaanxi Province, Xi’an Key Laboratory of Electronic Devices and Material Chemistry
Cui Yi
Frontier Institute of Science and Technology, Interdisciplinary Research Center of Frontier Science and Technology, State Key Laboratory for Strength and Vibration of Mechanical Structures, Institute of New Concept Sensors and Molecular Materials, Shaanxi Key Laboratory of New Conceptual Sensors and Molecular Materials, Engineering Research Center of Key Materials for Efficient Utilization of Clean Energy of Shaanxi Province, Xi’an Key Laboratory of Electronic Devices and Material Chemistry
Yawen Li
Ni Yan
Guoping Li
Frontier Institute of Science and Technology, Interdisciplinary Research Center of Frontier Science and Technology, State Key Laboratory for Strength and Vibration of Mechanical Structures, Institute of New Concept Sensors and Molecular Materials, Shaanxi Key Laboratory of New Conceptual Sensors and Molecular Materials, Engineering Research Center of Key Materials for Efficient Utilization of Clean Energy of Shaanxi Province, Xi’an Key Laboratory of Electronic Devices and Material Chemistry
Gang He