Unveiling the role of Cu-amine complexes in optimizing interfacial charge transfer dynamics between MoO2/CdZnS photocatalyst and amine substrate - Details

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Abstract：

Engineering　interfacial　charge　transfer　between　the　excited　heterogeneous　photocatalysts　and　molecular　substrates　is　an　essential　step　in　photocatalytic　transformation　of　solar　energy　to　chemical　bonds.　However,　lack　of　accessing　channel　that　equates　bond　linkage　in　function　(at　the　molecular　level)　to　bridging　rigid　catalysts　and　soft　molecules　makes　the　charge　transfer　inefficient　at　the　border　crossing.　Herein,　by　merging　a　solid　catalyst　(MoO2/Cd0.9Zn0.1S)-initiated　photocatalytic　process　and　a　metal-complex-mediated　photoredox　process,　a　programming　charge　transfer　in　tandem　was　reached　with　distinct　kinetics,　and　thus　propelled　efficient　generation　of　long-lived　interfacial　electrons　in　photoredox　reactions.　In　principle,　the　introduced　Cu2+　metal　center　as　the　medium　enables　the　efficient　bridging　of　the　amine　substrate　and　oxidation　sites　and　reduction　sites　of　MoO2/Cd0.9Zn0.1S　(MS)　photocatalyst　via　in-situ　coordination　and　weak　interaction.　Such　formed　Cu-amine　complexes　serve　as　an　electron　shuttle　delivering　the　electron　from　amine　to　the　valence　band　of　Cd0.9Zn0.1S　(CZS)　via　LMCT　process,　thus　accelerating　the　oxidation　of　amine.　Moreover,　the　Mo–S　bond　at　the　interface　of　the　MS　Schottky　junction　significantly　enhances　electron　transfer　from　the　conduction　band　of　CZS　to　MoO2,　thereby　boosting　H2　generation.　As　a　result,　the　optimized　photocatalyst　afforded　high　H2　and　N-benzylideneaniline　production　in　photocatalytic　H2　generation　from　amine　and　synchronously　C–N　coupling,　which　is　significantly　higher　than　CZS　(78.6　and　18.0　times)　and　5　%　MS　(17.2　and　2.3　times)　respectively.　The　design　of　interfacial　electron　transfer　mode　will　deepen　our　understanding　of　surface　science　and　heterogeneous　photocatalysis　in　solar-driven　redox　reactions.　©　2025　Elsevier　Inc.

Keyword：

Bond strength (chemical) Charge transfer Complexation Copper compounds Design for testability Electron transitions Indium compounds Metal complexes Molecules Molybdenum oxide Photocatalysts Photocatalytic activity Reaction kinetics Redox reactions Substrates Sulfur compounds Surface reactions

Community：

[ 1 ] [Zhang, Shaohui]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
[ 2 ] [Zhang, Shaohui]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
[ 3 ] [Zhu, Yupei]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
[ 4 ] [Zhu, Yupei]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
[ 5 ] [Chen, Yibin]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
[ 6 ] [Chen, Yibin]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
[ 7 ] [Hu, Xiaoyi]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
[ 8 ] [Hu, Xiaoyi]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
[ 9 ] [Wang, Deshun]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
[ 10 ] [Wang, Deshun]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
[ 11 ] [Ma, Xiong-Feng]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
[ 12 ] [Ma, Xiong-Feng]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
[ 13 ] [Wang, Lele]School of Materials Science and Engineering, Jiangsu University, Jiangsu, Zhenjiang; 212013, China
[ 14 ] [Li, Jing]Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing; 100190, China
[ 15 ] [Lin, Huaxiang]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
[ 16 ] [Lin, Huaxiang]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
[ 17 ] [Long, Jinlin]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
[ 18 ] [Long, Jinlin]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
[ 19 ] [Li, Zhaohui]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
[ 20 ] [Li, Zhaohui]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
[ 21 ] [Yuan, Rusheng]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
[ 22 ] [Yuan, Rusheng]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350116, China

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