Highly Ordered Conductive Metal-Organic Frameworks with Chemically Confined Polyoxometalate Clusters: A Dual-Functional Electrocatalyst for Efficient H2O2 Synthesis and Biomass Valorization - Details

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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：

Anodic oxidation Bioremediation Biosynthesis Doping (additives) Electrocatalysts Electrolysis Electrolytic reduction Green Synthesis Metal-Organic Frameworks Nanopores Nickel Oxygen reduction reaction

Community：

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

Reprint 's Address：

[yu, chengzhong]australian institute for bioengineering and nanotechnology, the university of queensland, brisbane; qld; 4072, australia;;[yu, chengzhong]state key laboratory of petroleum molecular and process engineering, sklpmpe, east china normal university, shanghai; 200062, china;;[yu, chengzhong]school of chemistry and molecular engineering, east china normal university, shanghai; 200241, china

Email：

czyu@chem.ecnu.edu.cncliu@chem.ecnu.edu.cn

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Source ：

Advanced Materials

ISSN： 0935-9648

Year： 2025

Issue： 17

Volume： 37

2 7 . 4 0 0

JCR@2023

CAS Journal Grade：1

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SCOPUS Cited Count：

ESI Highly Cited Papers on the List： 0 Unfold All

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30 Days PV： 0

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