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author:

Xia, Yang (Xia, Yang.) [1] | Zhu, Bicheng (Zhu, Bicheng.) [2] | Li, Liuyi (Li, Liuyi.) [3] (Scholars:李留义) | Ho, Wingkei (Ho, Wingkei.) [4] | Wu, Jinsong (Wu, Jinsong.) [5] | Chen, Haoming (Chen, Haoming.) [6] | Yu, Jiaguo (Yu, Jiaguo.) [7]

Indexed by:

EI Scopus SCIE

Abstract:

In photocatalysis, reducing the exciton binding energy and boosting the conversion of excitons into free charge carriers are vital to enhance photocatalytic activity. This work presents a facile strategy of engineering Pt single atoms on a 2D hydrazone-based covalent organic framework (TCOF) to promote H-2 production coupled with selective oxidation of benzylamine. The optimised TCOF-Pt SA photocatalyst with 3 wt% Pt single atom exhibited superior performance to TCOF and TCOF-supported Pt nanoparticle catalysts. The production rates of H-2 and N-benzylidenebenzylamine over TCOF-Pt SA3 are 12.6 and 10.9 times higher than those over TCOF, respectively. Empirical characterisation and theoretical simulation showed that the atomically dispersed Pt is stabilised on the TCOF support through the coordinated N-1-Pt-C-2 sites, thereby induing the local polarization and improving the dielectric constant to reach the low exciton binding energy. These phenomena led to the promotion of exciton dissociation into electrons and holes and the acceleration of the separation and transport of photoexcited charge carriers from bulk to the surface. This work provides new insights into the regulation of exciton effect for the design of advanced polymer photocatalysts.

Keyword:

benzylamine oxidation covalent organic frameworks H-2 production photocatalysis single-atom engineering

Community:

  • [ 1 ] [Xia, Yang]Univ Hong Kong, Dept Sci & Environm Studies, Hong Kong 999077, Peoples R China
  • [ 2 ] [Ho, Wingkei]Univ Hong Kong, Dept Sci & Environm Studies, Hong Kong 999077, Peoples R China
  • [ 3 ] [Xia, Yang]Educ Univ Hong Kong, Ctr Environm & Sustainable Dev CESD, Hong Kong 999077, Peoples R China
  • [ 4 ] [Ho, Wingkei]Educ Univ Hong Kong, Ctr Environm & Sustainable Dev CESD, Hong Kong 999077, Peoples R China
  • [ 5 ] [Xia, Yang]Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China
  • [ 6 ] [Yu, Jiaguo]Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China
  • [ 7 ] [Zhu, Bicheng]China Univ Geosci, Fac Mat Sci & Chem, Lab Solar Fuel, 388 Lumo Rd, Wuhan 430074, Peoples R China
  • [ 8 ] [Yu, Jiaguo]China Univ Geosci, Fac Mat Sci & Chem, Lab Solar Fuel, 388 Lumo Rd, Wuhan 430074, Peoples R China
  • [ 9 ] [Li, Liuyi]Fuzhou Univ, Coll Mat Sci & Engn, Key Lab Ecomat Adv Technol, New Campus, Fujian 350108, Peoples R China
  • [ 10 ] [Ho, Wingkei]City Univ Hong Kong, State Key Lab Marine Pollut, Tat Chee Ave, Hong Kong 999077, Peoples R China
  • [ 11 ] [Chen, Haoming]Natl Taiwan Univ, Dept Chem, Taipei 10617, Taiwan

Reprint 's Address:

  • [Yu, Jiaguo]Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China;;[Yu, Jiaguo]China Univ Geosci, Fac Mat Sci & Chem, Lab Solar Fuel, 388 Lumo Rd, Wuhan 430074, Peoples R China;;[Ho, Wingkei]City Univ Hong Kong, State Key Lab Marine Pollut, Tat Chee Ave, Hong Kong 999077, Peoples R China;;[Chen, Haoming]Natl Taiwan Univ, Dept Chem, Taipei 10617, Taiwan

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Source :

SMALL

ISSN: 1613-6810

Year: 2023

Issue: 35

Volume: 19

1 3 . 0

JCR@2023

1 3 . 0 0 0

JCR@2023

ESI Discipline: MATERIALS SCIENCE;

ESI HC Threshold:49

JCR Journal Grade:1

CAS Journal Grade:1

Cited Count:

WoS CC Cited Count: 22

SCOPUS Cited Count: 28

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 1

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