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[期刊论文]

Synergistic Ru Species on Poly(heptazine imide) Enabling Efficient Photocatalytic CO2 Reduction with H2O beyond 800 nm

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author:

Su, Bo (Su, Bo.) [1] | Wang, Sibo (Wang, Sibo.) [2] (Scholars:汪思波) | Xing, Wandong (Xing, Wandong.) [3] | Unfold

Indexed by:

Scopus SCIE

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 Ru-NPs/Ru-PHI catalyst assembled by anchoring Ru single atoms (SAs) and nanoparticles (NPs) onto poly(heptazine imide) (PHI) via the in-plane Ru-N-4 coordination and interfacial Ru-N bonds, respectively. This catalyst shows an unsurpassed CO production (32.8 mu mol 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.

Keyword:

Carbon nitrides CO2 reduction Photocatalysis Poly (heptazine imide)

Community:

  • [ 1 ] [Su, Bo]Fuzhou Univ, Coll Chem, State Key Lab Chem NBC Hazards Protect, Fuzhou 350116, Peoples R China
  • [ 2 ] [Wang, Sibo]Fuzhou Univ, Coll Chem, State Key Lab Chem NBC Hazards Protect, Fuzhou 350116, Peoples R China
  • [ 3 ] [Xing, Wandong]Fuzhou Univ, Coll Chem, State Key Lab Chem NBC Hazards Protect, Fuzhou 350116, Peoples R China
  • [ 4 ] [Liu, Kunlong]Fuzhou Univ, Coll Chem, State Key Lab Chem NBC Hazards Protect, Fuzhou 350116, Peoples R China
  • [ 5 ] [Chen, Xiong]Fuzhou Univ, Coll Chem, State Key Lab Chem NBC Hazards Protect, Fuzhou 350116, Peoples R China
  • [ 6 ] [Fang, Yuanxing]Fuzhou Univ, Coll Chem, State Key Lab Chem NBC Hazards Protect, Fuzhou 350116, Peoples R China
  • [ 7 ] [Zhang, Guigang]Fuzhou Univ, Coll Chem, State Key Lab Chem NBC Hazards Protect, Fuzhou 350116, Peoples R China
  • [ 8 ] [Wang, Xinchen]Fuzhou Univ, Coll Chem, State Key Lab Chem NBC Hazards Protect, Fuzhou 350116, Peoples R China
  • [ 9 ] [Su, Bo]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China
  • [ 10 ] [Wang, Sibo]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China
  • [ 11 ] [Xing, Wandong]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China
  • [ 12 ] [Liu, Kunlong]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China
  • [ 13 ] [Chen, Xiong]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China
  • [ 14 ] [Fang, Yuanxing]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China
  • [ 15 ] [Zhang, Guigang]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China
  • [ 16 ] [Wang, Xinchen]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China
  • [ 17 ] [Hung, Sung-Fu]Natl Yang Ming Chiao Tung Univ, Dept Appl Chem, Hsinchu 300, Taiwan
  • [ 18 ] [Hung, Sung-Fu]Natl Yang Ming Chiao Tung Univ, Ctr Emergent Funct Matter Sci, Hsinchu 300, Taiwan
  • [ 19 ] [Zhang, Huabin]King Abdullah Univ Sci & Technol, KAUST Catalysis Ctr, Phys Sci & Engn Div, Thuwal 23955, Saudi Arabia

Reprint 's Address:

  • 汪思波

    [Wang, Sibo]Fuzhou Univ, Coll Chem, State Key Lab Chem NBC Hazards Protect, Fuzhou 350116, Peoples R China;;[Wang, Xinchen]Fuzhou Univ, Coll Chem, State Key Lab Chem NBC Hazards Protect, Fuzhou 350116, Peoples R China;;[Wang, Sibo]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China;;[Wang, Xinchen]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China

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Source :

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

Year: 2025

1 6 . 1 0 0

JCR@2023

CAS Journal Grade:1

Cited Count:

WoS CC Cited Count:

30 Days PV: 1

操作日志

管理员  2025-06-25 20:29:33  追加

管理员  2025-05-27 15:57:25  创建

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