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author:

Zhang, P. (Zhang, P..) [1] | Tong, Y. (Tong, Y..) [2] | Liu, Y. (Liu, Y..) [3] | Vequizo, J.J.M. (Vequizo, J.J.M..) [4] | Sun, H. (Sun, H..) [5] | Yang, C. (Yang, C..) [6] | Yamakata, A. (Yamakata, A..) [7] | Fan, F. (Fan, F..) [8] | Lin, W. (Lin, W..) [9] | Wang, X. (Wang, X..) [10] | Choi, W. (Choi, W..) [11]

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Scopus

Abstract:

Polymeric carbon nitride modified with selected heteroatom dopants was prepared and used as a model photocatalyst to identify and understand the key mechanisms required for efficient photoproduction of H2O2 via selective oxygen reduction reaction (ORR). The photochemical production of H2O2 was achieved at a millimolar level per hour under visible-light irradiation along with 100 % apparent quantum yield (in 360–450 nm region) and 96 % selectivity in an electrochemical system (0.1 V vs. RHE). Spectroscopic analysis in spatiotemporal resolution and theoretical calculations revealed that the synergistic association of alkali and sulfur dopants in the polymeric matrix promoted the interlayer charge separation and polarization of trapped electrons for preferable oxygen capture and reduction in ORR kinetics. This work highlights the key features that are responsible for controlling the photocatalytic activity and selectivity toward the two-electron ORR, which should be the basis of further development of solar H2O2 production. © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

Keyword:

doping; H2O2 production; oxygen reduction reaction; photocatalysts; solar fuel

Community:

  • [ 1 ] [Zhang, P.]Division of Environmental Science and Engineering, Pohang University of Science and Technology (POSTECH), Pohang, 37673, South Korea
  • [ 2 ] [Tong, Y.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350002, China
  • [ 3 ] [Liu, Y.]State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian National Laboratory for Clean Energy, Dalian, 116023, China
  • [ 4 ] [Vequizo, J.J.M.]Graduate School of Engineering, Toyota Technological Institute, 2-12-1 Hisakata, Tempaku, Nagoya, 468-8511, Japan
  • [ 5 ] [Sun, H.]Division of Environmental Science and Engineering, Pohang University of Science and Technology (POSTECH), Pohang, 37673, South Korea
  • [ 6 ] [Yang, C.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350002, China
  • [ 7 ] [Yamakata, A.]Graduate School of Engineering, Toyota Technological Institute, 2-12-1 Hisakata, Tempaku, Nagoya, 468-8511, Japan
  • [ 8 ] [Fan, F.]State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian National Laboratory for Clean Energy, Dalian, 116023, China
  • [ 9 ] [Lin, W.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350002, China
  • [ 10 ] [Wang, X.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350002, China
  • [ 11 ] [Choi, W.]Division of Environmental Science and Engineering, Pohang University of Science and Technology (POSTECH), Pohang, 37673, South Korea

Reprint 's Address:

  • [Choi, W.]Division of Environmental Science and Engineering, Pohang University of Science and Technology (POSTECH)South Korea

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Source :

Angewandte Chemie - International Edition

ISSN: 1433-7851

Year: 2020

Issue: 37

Volume: 59

Page: 16209-16217

1 5 . 3 3 6

JCR@2020

1 6 . 1 0 0

JCR@2023

ESI HC Threshold:160

JCR Journal Grade:1

CAS Journal Grade:2

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count: 362

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 1

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