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author:

Bao, T. (Bao, T..) [1] | Wu, Y. (Wu, Y..) [2] | Tang, C. (Tang, C..) [3] | Xi, Y. (Xi, Y..) [4] | Zou, Y. (Zou, Y..) [5] | Shan, P. (Shan, P..) [6] | Zhang, C. (Zhang, C..) [7] | Drożd, W. (Drożd, W..) [8] | Stefankiewicz, A.R. (Stefankiewicz, A.R..) [9] | Yuan, P. (Yuan, P..) [10] | Yu, C. (Yu, C..) [11] | Liu, C. (Liu, C..) [12]

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Abstract:

The design of bifunctional and high-performance electrocatalysts that can be used as both cathodes and anodes for the two-electron oxygen reduction reaction (2e− ORR) and biomass valorization is attracting increasing attention. Herein, a conserved ligand replacement strategy is developed for the synthesis of highly ordered conductive metal-organic frameworks (Ni-HITP, HITP = 2, 3, 6, 7, 10, 11-hexaiminotriphenylene) with chemically confined phosphotungstic acid (PW12) nanoclusters in the nanopores. The newly formed Ni−O−W bonds in the resultant Ni-HITP/PW12 electrocatalysts modulate the electronic structures of both Ni and W sites, which are favorable for cathodic 2e− ORR to H2O2 production and anodic 5-hydroxymethylfurfural oxidation reaction (HMFOR) to 2, 5-furandicarboxylic acid (FDCA), respectively. In combination with the deliberately retained conductive frameworks and ordered pores, the dual-functional Ni-HITP/PW12 composites enable a H2O2 production rate of 9.51 mol gcat−1 h−1 and an FDCA yield of 96.8% at a current density of 100 mA cm−2/cell voltage of 1.38 V in an integrated 2e− ORR/HMFOR system, significantly improved than the traditional 2e− ORR/oxygen evolution reaction system. This work has provided new insights into the rational design of advanced electrocatalysts and electrocatalytic systems for the green synthesis of valuable chemicals. © 2025 Wiley-VCH GmbH.

Keyword:

biomass valorization conductive metal-organic frameworks electrocatalysis polyoxometalates two-electron reduction reaction

Community:

  • [ 1 ] [Bao T.]School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200241, China
  • [ 2 ] [Wu Y.]School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200241, China
  • [ 3 ] [Tang C.]School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200241, China
  • [ 4 ] [Xi Y.]School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200241, China
  • [ 5 ] [Zou Y.]School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200241, China
  • [ 6 ] [Shan P.]Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, School of Energy and Environment, Southeast University, Nanjing, 210096, China
  • [ 7 ] [Zhang C.]School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200241, China
  • [ 8 ] [Drożd W.]Center for Advanced Technologies, Adam Mickiewicz University, Uniwersytetu Poznańskiego 10, Poznań, 61-614, Poland
  • [ 9 ] [Drożd W.]Faculty of Chemistry, Adam Mickiewicz University, Uniwersytetu Poznańskiego 8, Poznań, 61-614, Poland
  • [ 10 ] [Stefankiewicz A.R.]Center for Advanced Technologies, Adam Mickiewicz University, Uniwersytetu Poznańskiego 10, Poznań, 61-614, Poland
  • [ 11 ] [Stefankiewicz A.R.]Faculty of Chemistry, Adam Mickiewicz University, Uniwersytetu Poznańskiego 8, Poznań, 61-614, Poland
  • [ 12 ] [Yuan P.]College of Chemical Engineering, National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, 350002, China
  • [ 13 ] [Yu C.]School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200241, China
  • [ 14 ] [Yu C.]State Key Laboratory of Petroleum Molecular and Process Engineering, SKLPMPE, East China Normal University, Shanghai, 200062, China
  • [ 15 ] [Yu C.]Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, 4072, QLD, Australia
  • [ 16 ] [Liu C.]School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200241, China
  • [ 17 ] [Liu C.]State Key Laboratory of Petroleum Molecular and Process Engineering, SKLPMPE, East China Normal University, Shanghai, 200062, China

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Source :

Advanced Materials

ISSN: 0935-9648

Year: 2025

2 7 . 4 0 0

JCR@2023

CAS Journal Grade:1

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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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