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author:

Su, Bo (Su, Bo.) [1] | Wang, Sibo (Wang, Sibo.) [2] | Xing, Wandong (Xing, Wandong.) [3] | Liu, Kunlong (Liu, Kunlong.) [4] | Hung, Sung-Fu (Hung, Sung-Fu.) [5] | Chen, Xiong (Chen, Xiong.) [6] | Fang, Yuanxing (Fang, Yuanxing.) [7] | Zhang, Guigang (Zhang, Guigang.) [8] | Zhang, Huabin (Zhang, Huabin.) [9] | Wang, Xinchen (Wang, Xinchen.) [10]

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EI

Abstract:

Photocatalytic CO2 conversion with H2O to carbonaceous fuels is a desirable strategy for CO2 management and solar utilization, yet its efficiency remains suboptimal. Herein, efficient and durable CO2 photoreduction is realized over a RuNPs/Ru-PHI catalyst assembled by anchoring Ru single atoms (SAs) and nanoparticles (NPs) onto poly(heptazine imide) (PHI) via the in-plane Ru-N4 coordination and interfacial Ru-N bonds, respectively. This catalyst shows an unsurpassed CO production (32.8 µmol h−1), a record-high apparent quantum efficiency (0.26%) beyond 800 nm, and the formation of the valuable H2O2. Ru SAs tune PHI's electronic structure to promote in-plane charge transfer to Ru NPs, forming a built-in electron field at the interface, which directs electron-hole separation and rushes excited electron movement from Ru-PHI to Ru NPs. Simultaneously, Ru SAs introduce an impurity level in PHI to endow long-wavelength photoabsorption, while Ru NPs strengthen CO2 adsorption/activation and expedite CO desorption. These effects of Ru species together effectively ensure CO2-to-CO conversion. The CO2 reduction on the catalyst is revealed to follow the pathway CO2→ *CO2→ *COOH→ *CO→ CO, based on the intermediates identified by in situ diffuse reflectance infrared Fourier transform spectroscopy and further supported by density functional theory calculations. © 2025 Wiley-VCH GmbH.

Keyword:

Fourier transform infrared spectroscopy Nitrides Photocatalysis

Community:

  • [ 1 ] [Su, Bo]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
  • [ 2 ] [Su, Bo]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
  • [ 3 ] [Wang, Sibo]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
  • [ 4 ] [Wang, Sibo]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
  • [ 5 ] [Xing, Wandong]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
  • [ 6 ] [Xing, Wandong]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
  • [ 7 ] [Liu, Kunlong]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
  • [ 8 ] [Liu, Kunlong]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
  • [ 9 ] [Hung, Sung-Fu]Department of Applied Chemistry and Center for Emergent Functional Matter Science, National Yang Ming Chiao Tung University, Hsinchu; 300, Taiwan
  • [ 10 ] [Chen, Xiong]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
  • [ 11 ] [Chen, Xiong]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
  • [ 12 ] [Fang, Yuanxing]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
  • [ 13 ] [Fang, Yuanxing]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
  • [ 14 ] [Zhang, Guigang]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
  • [ 15 ] [Zhang, Guigang]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
  • [ 16 ] [Zhang, Huabin]KAUST Catalysis Center, Physical Sciences and Engineering Division, King Abdullah University of Science and Technology, Thuwal; 23955, Saudi Arabia
  • [ 17 ] [Wang, Xinchen]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
  • [ 18 ] [Wang, Xinchen]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350116, China

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Source :

Angewandte Chemie - International Edition

ISSN: 1433-7851

Year: 2025

Issue: 27

Volume: 64

1 6 . 1 0 0

JCR@2023

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ESI Highly Cited Papers on the List: 0 Unfold All

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Chinese Cited Count:

30 Days PV: 0

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