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Vol. 16 (2024)

Enhancing the Electrocatalytic Oxidation of 5-Hydroxymethylfurfural Through Cascade Structure Tuning for Highly Stable Biomass Upgrading

https://doi.org/10.1007/s40820-024-01493-3
Xiaoli Jiang
School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, People’s Republic of China
Xianhui Ma
Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, People’s Republic of China
Yuanteng Yang
School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, People’s Republic of China
Yang Liu
School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, People’s Republic of China
Yanxia Liu
School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, People’s Republic of China
Lin Zhao
School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, People’s Republic of China
Penglei Wang
School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, People’s Republic of China
Yagang Zhang
School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, People’s Republic of China
Yue Lin
Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, People’s Republic of China
Yen Wei
The Key Laboratory of Bioorganic Phosphorus Chemistry and Chemical Biology (Ministry of Education), Department of Chemistry, Tsinghua University, Beijing 100084, People’s Republic of China

Corresponding Author: Yen Wei

weiyen@tsinghua.edu.cn

Nano-Micro Letters, Vol. 16 (2024), Article Number: 275

Abstract

Electrocatalytic 5-hydroxymethylfurfural oxidation reaction (HMFOR) provides a promising strategy to convert biomass derivative to high-value-added chemicals. Herein, a cascade strategy is proposed to construct Pd–NiCo2O4 electrocatalyst by Pd loading on Ni-doped Co3O4 and for highly active and stable synergistic HMF oxidation. An elevated current density of 800 mA cm–2 can be achieved at 1.5 V, and both Faradaic efficiency and yield of 2,5-furandicarboxylic acid remained close to 100% over 10 consecutive electrolysis. Experimental and theoretical results unveil that the introduction of Pd atoms can modulate the local electronic structure of Ni/Co, which not only balances the competitive adsorption of HMF and OH– species, but also promote the active Ni3+ species formation, inducing high indirect oxidation activity. We have also discovered that Ni incorporation facilitates the Co2+ pre-oxidation and electrophilic OH* generation to contribute direct oxidation process. This work provides a new approach to design advanced electrocatalyst for biomass upgrading.


Highlights:
1 A novel cascade strategy is proposed to construct Pd-NiCo2O4 electrocatalyst.
2 First time discovery that Ni incorporation together with Pd loading is able to balance the competitive adsorption of OH– and 5-hydroxymethylfurfural.
3 Pd–NiCo2O4 promotes both the indirect and direct synergistic oxidation process.
4 Pd–NiCo2O4 catalyst exhibits extraordinary current density and excellent Faradaic Efficiency at a low potential.

Keywords

5-Hydroxymethylfurfural oxidation reaction Competitive adsorption Cascade strategy Elevated current density
Jiang, Xiaoli, Xianhui Ma, Yuanteng Yang, Yang Liu, Yanxia Liu, Lin Zhao, Penglei Wang, Yagang Zhang, Yue Lin, and Yen Wei. 2024. “Enhancing the Electrocatalytic Oxidation of 5-Hydroxymethylfurfural Through Cascade Structure Tuning for Highly Stable Biomass Upgrading”. Nano-Micro Letters 16 (August):275. https://doi.org/10.1007/s40820-024-01493-3.
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