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author:

Xiao, Z. (Xiao, Z..) [1] | Shen, J. (Shen, J..) [2] | Jiang, J. (Jiang, J..) [3] | Zhang, J. (Zhang, J..) [4] | Liang, S. (Liang, S..) [5] | Han, S. (Han, S..) [6] | Long, J. (Long, J..) [7] | Dai, W. (Dai, W..) [8] | Li, Y. (Li, Y..) [9] | Wang, X. (Wang, X..) [10] | Xi, H. (Xi, H..) [11] | Fu, X. (Fu, X..) [12] | Zhang, Z. (Zhang, Z..) [13]

Indexed by:

Scopus

Abstract:

CH3OH is the most desired product of photocatalytic CH4 conversion. The prominent metal-decorated photocatalyst is challenging in both high yield and selectivity for CH3OH products due to over-oxidation by •OH mechanism. Here, interstitial Zn is fabricated into ZniO to induce the formation of Zn atom island for rapid single electron reduction of O2 into •OOH instead of •OH for the selective combination with methyl into CH3OOH. AuPd alloy is simultaneously decorated on ZniO surface for tuning CH3OOH adsorption and reduction into CH3OH. The synergy of Zn atom island and AuPd alloy achieve a tandem reaction pathway (CH4→CH3OOH→CH3OH) for an unprecedented CH3OH yield of 2444 mmol gAuPd−1 h−1 (or 8800 µmol gcat−1 h−1) with 98.3% selectivity, which bypasses the •OH mechanism for tuning the high selectivity of CH3OH. An apparent quantum efficiency of 18.53% at 370 nm for CH4 conversion are super to the reported photocatalytic systems. Thus, this work provides the new strategy of the synergetic atom island and metal alloy photocatalysts through a tandem reaction pathway to mediate the photocatalytic selective oxidation of CH4 into the desired CH3OH. © 2025 Wiley-VCH GmbH.

Keyword:

atom island AuPd alloy methanol selectivity photocatalysis tandem reaction

Community:

  • [ 1 ] [Xiao Z.]State Key Lab of Photocatalysis on Energy and Environment College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 2 ] [Xiao Z.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 3 ] [Shen J.]State Key Lab of Photocatalysis on Energy and Environment College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 4 ] [Shen J.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 5 ] [Jiang J.]State Key Lab of Photocatalysis on Energy and Environment College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 6 ] [Jiang J.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 7 ] [Zhang J.]State Key Lab of Photocatalysis on Energy and Environment College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 8 ] [Zhang J.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 9 ] [Liang S.]State Key Lab of Photocatalysis on Energy and Environment College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 10 ] [Liang S.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 11 ] [Han S.]State Key Laboratory of NBC Protection for Civilian, Beijing, 102205, China
  • [ 12 ] [Long J.]State Key Lab of Photocatalysis on Energy and Environment College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 13 ] [Long J.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 14 ] [Dai W.]State Key Lab of Photocatalysis on Energy and Environment College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 15 ] [Dai W.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 16 ] [Li Y.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 17 ] [Wang X.]State Key Lab of Photocatalysis on Energy and Environment College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 18 ] [Wang X.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 19 ] [Xi H.]State Key Laboratory of NBC Protection for Civilian, Beijing, 102205, China
  • [ 20 ] [Fu X.]State Key Lab of Photocatalysis on Energy and Environment College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 21 ] [Fu X.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 22 ] [Zhang Z.]State Key Lab of Photocatalysis on Energy and Environment College of Chemistry, Fuzhou University, Fuzhou, 350116, China
  • [ 23 ] [Zhang Z.]College of Chemistry, Fuzhou University, Fuzhou, 350116, China

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Source :

Advanced Functional Materials

ISSN: 1616-301X

Year: 2025

1 8 . 5 0 0

JCR@2023

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ESI Highly Cited Papers on the List: 0 Unfold All

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30 Days PV: 0

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