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学者姓名：陈嘉彬
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Abstract ：
Single-atom catalysts (SACs) enable atomic-level control over active sites, but orbital-level manipulation to steer catalytic behavior remains challenging. Here, we address this issue through d-orbital engineering of Cu SACs, achieving simultaneous control over coordination geometry (Cu-N3) and high metal loading (33.2 wt%) for direct benzene-to-phenol oxidation with H2O2. The tri-coordinated Cu SAC (Cu-N3-33.2) exhibits the highest performance with 85.8% benzene conversion and a turnover frequency of 680.3 h-1 at 60 oC, ranking it among the best metal-based catalysts. In-situ ATR-IR spectroscopy and DFT calculations reveal that dynamically formed Cu-O intermediates, driven by p-d orbital hybridization between Cu (d orbitals) and O (p orbitals), lower the H2O2 activation barrier by 0.98 eV compared to Cu-N4 sites. High-density atomic Cu sites prevent over-oxidation by consuming singlet oxygen (1O2). This work establishes a dual-parameter optimization paradigm, including orbital configuration and site density, redefining design principles for selective oxidation SACs.
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| GB/T 7714 | Li, Shuchun , Cao, Changsheng , Chen, Jiabin et al. Manipulating d-orbital of Cu single atom site by coordination engineering for selective oxidation of benzene [J]. | NATURE COMMUNICATIONS , 2025 , 16 (1) . |
| MLA | Li, Shuchun et al. "Manipulating d-orbital of Cu single atom site by coordination engineering for selective oxidation of benzene" . | NATURE COMMUNICATIONS 16 . 1 (2025) . |
| APA | Li, Shuchun , Cao, Changsheng , Chen, Jiabin , Wen, Wen , Zhang, Xuefei , Cui, Longji et al. Manipulating d-orbital of Cu single atom site by coordination engineering for selective oxidation of benzene . | NATURE COMMUNICATIONS , 2025 , 16 (1) . |
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Abstract ：
Transition metal-based electrocatalysts are a promising alternative to noble metal catalysts for electrochemical upgrading of biomass-derived 5-hydroxymethylfurfural (HMF) into high-value 2,5furandicarboxylic acid (FDCA). However, the rational design of efficient electrocatalysts with precisely tailored structure-activity correlations remains a critical challenge. Herein, we report a hierarchically structured self-supporting electrode (Vo-NiCo(OH)2-NF) synthesized through in situ electrochemical reconstruction of NiCo-Prussian blue analogue (NiCo-PBA) precursor, in which oxygen vacancy (Vo)rich Co-doped Ni(OH)2 nanosheet arrays are vertically aligned on nickel foam (NF), creating an interconnected conductive network. When evaluated for the HMF oxidation reaction (HMFOR), Vo-NiCo(OH)2-NF exhibits exceptional electrochemical performance, achieving near-complete HMF conversion (99%), ultrahigh FDCA Faradaic efficiency (97.5%), and remarkable product yield (96.2%) at 1.45 V, outperforming conventional Co-doped Ni(OH)2 (NiCo(OH)2-NF) and pristine Ni(OH)2 (Ni(OH)2-NF) electrodes. By combining in situ spectroscopic characterization and theoretical calculations, we elucidate that the synergistic effects of Co-doping and oxygen vacancy engineering effectively modulate the electronic structure of Ni active centers, favor the formation of high-valent Ni3+ species, and optimize HMF adsorption, thereby improving the HMFOR performance. This work provides valuable mechanistic insights for catalyst design and may inspire the development of advanced transition metal-based electrodes for efficient biomass conversion systems. (c) 2025 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
Keyword ：
Biomass upgrading Biomass upgrading Electrolysis Electrolysis Hierarchical structure Hierarchical structure Oxygen vacancy Oxygen vacancy Transition metal-based electrodes Transition metal-based electrodes
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| GB/T 7714 | Xie, Diexin , Chen, Jiabin , Hou, Jingxin et al. Rational design of oxygen vacancy-rich self-supporting NiCo(OH)2 electrode for efficient biomass upgrading [J]. | JOURNAL OF ENERGY CHEMISTRY , 2025 , 108 : 558-566 . |
| MLA | Xie, Diexin et al. "Rational design of oxygen vacancy-rich self-supporting NiCo(OH)2 electrode for efficient biomass upgrading" . | JOURNAL OF ENERGY CHEMISTRY 108 (2025) : 558-566 . |
| APA | Xie, Diexin , Chen, Jiabin , Hou, Jingxin , Yang, Fangfang , Feng, Runping , Cao, Changsheng et al. Rational design of oxygen vacancy-rich self-supporting NiCo(OH)2 electrode for efficient biomass upgrading . | JOURNAL OF ENERGY CHEMISTRY , 2025 , 108 , 558-566 . |
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Abstract ：
Transition metal-based electrocatalysts are a promising alternative to noble metal catalysts for electrochemical upgrading of biomass-derived 5-hydroxymethylfurfural (HMF) into high-value 2,5-furandicarboxylic acid (FDCA). However, the rational design of efficient electrocatalysts with precisely tailored structure–activity correlations remains a critical challenge. Herein, we report a hierarchically structured self-supporting electrode (Vo-NiCo(OH)2-NF) synthesized through in situ electrochemical reconstruction of NiCo-Prussian blue analogue (NiCo-PBA) precursor, in which oxygen vacancy (Vo)-rich Co-doped Ni(OH)2 nanosheet arrays are vertically aligned on nickel foam (NF), creating an interconnected conductive network. When evaluated for the HMF oxidation reaction (HMFOR), Vo-NiCo(OH)2-NF exhibits exceptional electrochemical performance, achieving near-complete HMF conversion (99%), ultrahigh FDCA Faradaic efficiency (97.5%), and remarkable product yield (96.2%) at 1.45 V, outperforming conventional Co-doped Ni(OH)2 (NiCo(OH)2-NF) and pristine Ni(OH)2 (Ni(OH)2-NF) electrodes. By combining in situ spectroscopic characterization and theoretical calculations, we elucidate that the synergistic effects of Co-doping and oxygen vacancy engineering effectively modulate the electronic structure of Ni active centers, favor the formation of high-valent Ni3+ species, and optimize HMF adsorption, thereby improving the HMFOR performance. This work provides valuable mechanistic insights for catalyst design and may inspire the development of advanced transition metal-based electrodes for efficient biomass conversion systems. © 2025 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences.
Keyword ：
Coated wire electrodes Coated wire electrodes Electrolytic reduction Electrolytic reduction Nanosheets Nanosheets Reconstruction (structural) Reconstruction (structural) Structural analysis Structural analysis Structural dynamics Structural dynamics
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| GB/T 7714 | Xie, Diexin , Chen, Jiabin , Hou, Jingxin et al. Rational design of oxygen vacancy-rich self-supporting NiCo(OH)2 electrode for efficient biomass upgrading [J]. | Journal of Energy Chemistry , 2025 , 108 : 558-566 . |
| MLA | Xie, Diexin et al. "Rational design of oxygen vacancy-rich self-supporting NiCo(OH)2 electrode for efficient biomass upgrading" . | Journal of Energy Chemistry 108 (2025) : 558-566 . |
| APA | Xie, Diexin , Chen, Jiabin , Hou, Jingxin , Yang, Fangfang , Feng, Runping , Cao, Changsheng et al. Rational design of oxygen vacancy-rich self-supporting NiCo(OH)2 electrode for efficient biomass upgrading . | Journal of Energy Chemistry , 2025 , 108 , 558-566 . |
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