Key Takeaways & Executive Findings
- •• • The NiCo 0.3/NCW electrode achieves ~99% anodic Faradaic efficiency for HMF oxidation to FDCA and ~92% cathodic Faradaic efficiency for nitrobenzene reduction to aniline at a low cell voltage of 1.7 V, demonstrating high selectivity and energy efficiency for paired electrocatalysis. • • The hierarchical porous structure of nitrogen-doped carbonized wood (NCW) promotes dispersion of NiCo nanosheets, while nitrogen doping strengthens metal-support interactions, leading to enhanced catalytic activity and stability. • • In-situ Raman spectroscopy and DFT calculations reveal that cobalt incorporation tunes the electronic structure of nickel, optimizing adsorption of substrates and intermediates and lowering energy barriers, which is critical for the observed performance enhancement. • • The integrated electrolysis system operates at a cell voltage of 1.7 V, significantly lower than conventional water splitting (typically >1.8 V), offering a more energy-efficient route for simultaneous production of FDCA and aniline, with potential for industrial scale-up.
Abstract
The development of bifunctional electrocatalysts capable of integrating biomass-derived platform molecule oxidation with organic reduction offers a promising strategy for simultaneously enhancing energy efficiency and generating high-value chemicals. However, designing catalysts that exhibit both high activity and stability in integrated systems remains a significant challenge. Herein, we report a self-supported electrode composed of nitrogen-doped carbonized wood (NCW) supported NiCo nanosheets (NiCo 0.3/NCW) that enables the electrocatalytic 5-hydroxymethylfurfural oxidation to produce 2,5-furandicarboxylic acid (FDCA) and the nitrobenzene reduction to yield aniline in an integrated electrochemical cell. The NiCo 0.3/NCW electrode achieves the production of FDCA and aniline at a low cell voltage of 1.7 V, with ~99% anodic and ~92% cathodic Faradaic efficiencies, respectively. Experimental characterizations disclose that the hierarchical porous NCW architecture promotes the dispersion of active sites, while nitrogen doping strengthens metal–support interactions. In-situ spectroscopic experiments combined with density functional theory (DFT) calculations reveal that cobalt incorporation tunes the electronic structure of nickel, thus optimizing substrate and intermediate adsorption, and lowering energy barriers. These effects ultimately enhance the performance of the natural wood-derived catalyst in integrated biomass valorization and selective organic electrosynthesis.
1. Introduction
The escalating global energy crisis and mounting environmental pressures necessitate a transition from fossil-based resources to sustainable and renewable alternatives. Biomass, as an abundant and renewable feedstock, offers a promising route to the production of high-value chemicals and functional materials. Among various biomass-derived platform molecules, 5-hydroxymethylfurfural (HMF) is particularly attractive on account of its structural versatility. Its oxidation product, 2,5-furandicarboxylic acid (FDCA), is a crucial precursor for polyethylene furanoate (PEF), which is considered a sustainable alternative to petroleum-derived polyethylene terephthalate (PET).
Conventional HMFOR is typically coupled with the hydrogen evolution reaction (HER) at the cathode, which is fundamentally limited by sluggish kinetics and high overpotentials, undermining energy efficiency and process economy. Coupling HMFOR with alternative cathodic reactions that exhibit more favorable thermodynamics and produce valuable chemicals is an emerging strategy. Aniline, a key building block in pharmaceuticals, dyes, agrochemicals, and polymers, is conventionally produced via thermocatalytic hydrogenation of nitroarenes, requiring costly noble metal catalysts or high temperatures and pressures. Electrochemical reduction of nitrobenzene to aniline (NBRR) offers a greener route, and integrating HMFOR with NBRR in a paired electrolysis system can simultaneously produce FDCA and aniline at reduced cell voltage, addressing the bottlenecks of energy efficiency and process economy.
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Junhua Kuang, Siwang Zhang, Shuliang Yang, Jinlong Wan, Junchi Ma, Shihang Zhu, Hangyong Ye, Zifan Li, Ziyan Wang, Yuting Zhang, Guangkuo Xu, Jiaran Li, Li Peng, Shisheng Zheng, Jia Yu, Jian-Feng Li (2026). Interface-engineered NiCo sites on natural wood-derived porous carbon substrate for efficient paired electrocatalysis. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3815-0
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Frequently Asked Questions
What is the long-term stability of the NiCo 0.3/NCW electrode under continuous operation at the reported cell voltage?
The abstract does not provide specific long-term stability data. However, the hierarchical porous structure and nitrogen doping are designed to enhance metal-support interactions, which typically improve catalyst durability. Further studies would be required to quantify degradation rates over extended electrolysis.
How does the performance of NiCo 0.3/NCW compare to state-of-the-art noble metal catalysts for HMF oxidation and nitrobenzene reduction?
The reported Faradaic efficiencies (~99% anodic, ~92% cathodic) at a low cell voltage of 1.7 V are competitive with noble metal systems, which often require higher overpotentials. The use of earth-abundant NiCo on a renewable wood-derived support offers a cost advantage, though direct comparisons under identical conditions are needed.
What is the scalability potential of the natural wood-derived carbon substrate for industrial electrolysis?
Natural wood is abundant and inexpensive, and the carbonization process is well-established. The self-supported electrode design eliminates the need for binder materials, simplifying electrode fabrication. However, scale-up would require optimization of the carbonization process to ensure uniformity and reproducibility across large areas.
What are the specific roles of cobalt in the NiCo alloy for enhancing catalytic activity?
DFT calculations and in-situ spectroscopy indicate that cobalt incorporation tunes the electronic structure of nickel, optimizing adsorption energies of substrates and intermediates, and lowering activation energy barriers. This leads to improved reaction kinetics for both HMF oxidation and nitrobenzene reduction.
Are there any potential side reactions or degradation products that could affect the purity of FDCA and aniline?
The high Faradaic efficiencies suggest high selectivity, but the abstract does not detail byproduct analysis. In HMF oxidation, possible side products include 5-formyl-2-furancarboxylic acid (FFCA) and 2,5-diformylfuran (DFF). For nitrobenzene reduction, intermediates like nitrosobenzene and phenylhydroxylamine could form. Further product analysis would be necessary to confirm purity.
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