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学者姓名:谢在来
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Glycosyl aryl sulfones exhibit diverse biological activities. Herein, we developed a copper-promoted coupling strategy using glycosyl sodium sulfinates and aryl iodides or bromides, enabling efficient synthesis of carbohydrate-based sulfone with broad functional group compatibility. This method offers a versatile approach for the late-stage modification of bioactive molecules.
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GB/T 7714 | Wang, Linyitian , Guo, Huize , Luo, Jiaxin et al. Copper-promoted late-stage glycosylsulfonylation of aryl iodide and bromide to access glycosyl aryl sulfones [J]. | ORGANIC & BIOMOLECULAR CHEMISTRY , 2025 . |
MLA | Wang, Linyitian et al. "Copper-promoted late-stage glycosylsulfonylation of aryl iodide and bromide to access glycosyl aryl sulfones" . | ORGANIC & BIOMOLECULAR CHEMISTRY (2025) . |
APA | Wang, Linyitian , Guo, Huize , Luo, Jiaxin , Zhen, Wenxu , Wang, Shiping , Xie, Zailai et al. Copper-promoted late-stage glycosylsulfonylation of aryl iodide and bromide to access glycosyl aryl sulfones . | ORGANIC & BIOMOLECULAR CHEMISTRY , 2025 . |
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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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An Fe3C-based catalyst was fabricated via a facile template-free route. Owing to surface structure modulation, optimal FeNC800 presented well-dispersed Fe3C on N-doped carbon, the highest surface area, a mesoporous structure, most defects and maximum surface content of Fe. As a result, FeNC800 exhibited distinguished catalytic performance for transfer hydrogenation of nitroarenes with hydrazine hydrate at near room temperature.
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GB/T 7714 | Wu, Dan , Wu, Shuchang , Liu, Jinliang et al. Tuning the surface structure of an Fe-based catalyst for transfer hydrogenation of nitroarenes at near room temperature [J]. | CHEMICAL COMMUNICATIONS , 2025 , 61 (29) : 5455-5458 . |
MLA | Wu, Dan et al. "Tuning the surface structure of an Fe-based catalyst for transfer hydrogenation of nitroarenes at near room temperature" . | CHEMICAL COMMUNICATIONS 61 . 29 (2025) : 5455-5458 . |
APA | Wu, Dan , Wu, Shuchang , Liu, Jinliang , Zhang, Xiaomin , Fang, Xiaomin , Li, Shuchun et al. Tuning the surface structure of an Fe-based catalyst for transfer hydrogenation of nitroarenes at near room temperature . | CHEMICAL COMMUNICATIONS , 2025 , 61 (29) , 5455-5458 . |
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The oxidative dehydrogenation of propane (ODHP) represents a highly promising route for the industrial-scale production of propene. Non-metallic boron nitride (BN)-based materials, known for their high propene selectivity, have emerged as next-generation ODH catalysts. However, the real active sites on surfaces remain unclear due to the absence of visual experimental evidence. In this work, we introduce a chemical titration approach to clarify the active centers of NaOH modified BN (BN-NaOH) catalysts for ODHP. The BN-NaOH catalyst demonstrates outstanding performance, achieving over 90 % olefin selectivity and a stable propane conversion of 23.2 %. Notably, the turnover frequency (TOF) for B-OH sites reaching 1.2 h- 1, which significantly surpassed that of unmodified BN catalysts (0.6 h- 1). In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) analysis revealed that the formation of OH-nests on the BN-NaOH surface was primarily accountable for the enhanced reactivity. Moreover, the crucial role of these OH-nests during ODHP was further validated through selective chemical titration of B-OH groups using benzoic anhydride.
Keyword :
Active sites Active sites Boron hydroxyl group Boron hydroxyl group In situ DRIFTS In situ DRIFTS Oxidative dehydrogenation of propane Oxidative dehydrogenation of propane
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GB/T 7714 | Duan, Qiwei , Hu, Zhengli , Hu, Aoxue et al. Identification of active sites in boron nitride for propane oxidative dehydrogenation catalysis [J]. | CHEMICAL ENGINEERING SCIENCE , 2025 , 306 . |
MLA | Duan, Qiwei et al. "Identification of active sites in boron nitride for propane oxidative dehydrogenation catalysis" . | CHEMICAL ENGINEERING SCIENCE 306 (2025) . |
APA | Duan, Qiwei , Hu, Zhengli , Hu, Aoxue , Huang, Shuping , Chen, Ziyi , Yu, Kaihua et al. Identification of active sites in boron nitride for propane oxidative dehydrogenation catalysis . | CHEMICAL ENGINEERING SCIENCE , 2025 , 306 . |
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NiFe-based (oxy)hydroxides are widely recognized as highly promising electrocatalysts for the alkaline oxygen evolution reaction (OER). Despite their potential, their low conductivity and sluggish charge transfer kinetics pose significant challenges to further enhancing their catalytic activity. Herein, a novel catalyst featuring Ru single-atoms (SAs) coordinately dispersed on nickel-iron vanadium layered triple hydroxides (Ru SAs@NiFeV-LTHs) to improve alkaline OER performance is reported. With a Ru loading of 0.33 wt.%, this catalyst demonstrates outstanding performance, with a low Tafel slope of 27.15 mV dec(-1) and minimal overpotentials of 221 and 269 mV to achieve current densities of 10 and 100 mA cm(-2), respectively, outperforming unmodified NiFeV-LTHs and most other layered hydroxides reported in the literature. Furthermore, the catalyst exhibits exceptional durability, maintaining stable overpotentials for 200 hours at current densities of 10 mA cm(-2), 100 mA cm(-2), and 500 mA cm(-2). Density functional theory (DFT) calculations, coupled with experimental observations, identify the presence of Ru SAs as the key factor, which not only serve as superior active sites but also as modifiers of the electronic properties of the support material, thereby improving the overall conductivity and enhancing the intrinsic activity of metal sites in the catalyst's support.
Keyword :
electronic interactions electronic interactions layered triple hydroxides layered triple hydroxides oxygen evolution reaction oxygen evolution reaction Ru single-atoms Ru single-atoms
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GB/T 7714 | Shi, Ningning , Xue, Weichao , Liu, Panpan et al. Atomically Dispersed Ru on NiFeV Layered Triple Hydroxides for Enhanced Water Oxidation [J]. | ADVANCED FUNCTIONAL MATERIALS , 2025 , 35 (24) . |
MLA | Shi, Ningning et al. "Atomically Dispersed Ru on NiFeV Layered Triple Hydroxides for Enhanced Water Oxidation" . | ADVANCED FUNCTIONAL MATERIALS 35 . 24 (2025) . |
APA | Shi, Ningning , Xue, Weichao , Liu, Panpan , Zeng, Chaobin , Yue, Shengnan , Xie, Wangjing et al. Atomically Dispersed Ru on NiFeV Layered Triple Hydroxides for Enhanced Water Oxidation . | ADVANCED FUNCTIONAL MATERIALS , 2025 , 35 (24) . |
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The electrochemical CO2 reduction reaction (CO2RR) provides a promising approach to mitigate the global greenhouse effect by converting CO2 into high-value chemicals or fuels. Noble metal-based nanomaterials are widely regarded as efficient catalysts for CO2RR due to their high catalytic activity and excellent stability. However, these catalysts typically favor the formation of C1 products, which have relatively low economic value. Moreover, the high cost and limited availability of noble materials necessitate strategies to reduce their usage, often by dispersing them on suitable support materials to enhance catalytic performance. In this study, a novel metal-based support, zirconium phosphate Zr-3(PO4)(4), was used to anchor ultrasmall palladium nanoparticles (pre-ZrP-Pd). Compared to the reversible hydrogen electrode, the pre-ZrP-Pd achieved a maximum Faradaic efficiency (FE) of 92.1% for ethanol at -0.8 V versus RHE, along with a peak ethanol current density of 0.82 mA/cm(2). Density functional theory (DFT) calculations revealed that the strong metal-support interactions between the ZrP support and Pd nanoparticles lead to an upward shift of the Pd d-band center, enhancing the adsorption of CO* and promoting the coupling of CO and CO to produce ethanol.
Keyword :
density functional theory (DFT) calculations density functional theory (DFT) calculations electrochemical CO2 reduction reaction (CO2RR) electrochemical CO2 reduction reaction (CO2RR) ethanol selectivity ethanol selectivity noble metal-based nanocatalysts noble metal-based nanocatalysts zirconium phosphate (Zr-3(PO4)(4)) support zirconium phosphate (Zr-3(PO4)(4)) support
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GB/T 7714 | Zhong, Bowen , Hu, Chengwei , Sun, Kaian et al. Ultrasmall palladium nanoparticles supported on zirconium phosphate for electrochemical CO2 reduction to ethanol [J]. | FRONTIERS IN ENERGY , 2025 , 19 (4) : 545-551 . |
MLA | Zhong, Bowen et al. "Ultrasmall palladium nanoparticles supported on zirconium phosphate for electrochemical CO2 reduction to ethanol" . | FRONTIERS IN ENERGY 19 . 4 (2025) : 545-551 . |
APA | Zhong, Bowen , Hu, Chengwei , Sun, Kaian , Yan, Wei , Zhang, Jiujun , Xie, Zailai . Ultrasmall palladium nanoparticles supported on zirconium phosphate for electrochemical CO2 reduction to ethanol . | FRONTIERS IN ENERGY , 2025 , 19 (4) , 545-551 . |
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Harnessing supramolecular interactions to regulate the structure and performance of functional materials is a key challenge in materials chemistry. Herein, the study utilizes 18-crown-6 (18C6) ether-assisted alkali-metal (Na, K, Cs) copper(I) iodide supramolecular assemblies to precisely regulate the material structures. This approach facilitated the transition from 1D mono-royal crown coordination (18C6@KCuI2, CKCI) to 0D di-royal crown ((18C6)(2)@Na-2(H2O)(3)Cu4I6, CNCI) and tri-royal crown ((18C6)(3)@Cs2Cu2I4, CCCI) structures. Interestingly, the CCCI single-crystal exhibits outstanding scintillation properties, with a high relative light yield of 71 000 photons MeV-1 and an ultralow detection limit of 39.3 nGy s(-1), which can be attributed to the synergistic effects of 18C6 and copper-iodide clusters. It stabilizes the self-trapped exciton state, enhances exciton localization, and reduces non-radiative losses, thus resulting in a large Stokes shift of 193 nm and near-unity photoluminescence quantum yield of 99.4%. Additionally, 18C6 can promote crystal nucleation and growth, making it easy to prepare centimeter-scale transparent single crystals with >80% transmittance, such as CCCI single crystal can achieve an ultrahigh-resolution X-ray imaging of 26.3 lp mm(-1). It demonstrates that the structure and performance of halide scintillators can be regulated through supramolecular interactions, which provides a new approach for developing high-performance scintillator materials.
Keyword :
18-crown-6 18-crown-6 copper(I) iodide copper(I) iodide self-trapped exciton state self-trapped exciton state supramolecular scintillators supramolecular scintillators X-ray imaging X-ray imaging
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GB/T 7714 | Ye, Yuanji , Di, Yiming , Zhou, Jiahao et al. Crown Ether-Assisted Alkali-Metal Copper(I) Iodide Supramolecular Scintillators with Near-Unity Emission for Ultrahigh-Resolution X-Ray Imaging [J]. | ADVANCED FUNCTIONAL MATERIALS , 2025 , 35 (33) . |
MLA | Ye, Yuanji et al. "Crown Ether-Assisted Alkali-Metal Copper(I) Iodide Supramolecular Scintillators with Near-Unity Emission for Ultrahigh-Resolution X-Ray Imaging" . | ADVANCED FUNCTIONAL MATERIALS 35 . 33 (2025) . |
APA | Ye, Yuanji , Di, Yiming , Zhou, Jiahao , Qiu, Qiangwen , Chen, Yuhua , Zhong, Shanyuan et al. Crown Ether-Assisted Alkali-Metal Copper(I) Iodide Supramolecular Scintillators with Near-Unity Emission for Ultrahigh-Resolution X-Ray Imaging . | ADVANCED FUNCTIONAL MATERIALS , 2025 , 35 (33) . |
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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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Although the advanced oxidation processes (AOP) based on the activation of persulfate over carbon materials to degrade organic pollutants has attracted enormous attention, the surface engineering of carbon catalysts is still desired to boost their performance. Meanwhile, the synthesis of the nitrogen (N)-doped carbon commonly relies on an excessive external N source, which not only causes the waste of raw materials but also makes it difficult to realize the good distribution of N dopants. Herein, N-doped porous graphene-like carbon was synthesized using a nucleobase as endogenous N precursors, during which zinc nitrate was adopted to modulate the surface structures and the chemical state of each element. The optimal sample NG-5 was highly adsorptive and effective for the activation of peroxydisulfates (PDS) to degrade tetracycline (TC), which could also work in a relatively wide pH range and demonstrated high stability. The porous structure and high surface area facilitated the catalyst to expose more active sites. In-depth studies suggested that the activation of PDS followed mixed routes, where both radical and nonradical paths made notable contributions. Superoxide radicals and singlet oxygen were mainly responsible for TC degradation, while the contribution of hydroxyl and sulfate radicals could be ignored. © 2025 American Chemical Society
Keyword :
Catalyst activity Catalyst activity Chemical activation Chemical activation Degradation Degradation Doping (additives) Doping (additives) Nitrogen Nitrogen Organic carbon Organic carbon Porous carbon Porous carbon Sulfur compounds Sulfur compounds Zinc compounds Zinc compounds
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GB/T 7714 | Fang, Junjie , Wu, Shuchang , Li, Shuchun et al. Synergistic Radical and Nonradical Dual Pathways Enable High-Efficiency Tetracycline Degradation over Hierarchical Nitrogen-Doped Carbon [J]. | Industrial and Engineering Chemistry Research , 2025 , 64 (32) : 15512-15522 . |
MLA | Fang, Junjie et al. "Synergistic Radical and Nonradical Dual Pathways Enable High-Efficiency Tetracycline Degradation over Hierarchical Nitrogen-Doped Carbon" . | Industrial and Engineering Chemistry Research 64 . 32 (2025) : 15512-15522 . |
APA | Fang, Junjie , Wu, Shuchang , Li, Shuchun , Zhang, Xiaomin , Chen, Yiquan , Xie, Zailai . Synergistic Radical and Nonradical Dual Pathways Enable High-Efficiency Tetracycline Degradation over Hierarchical Nitrogen-Doped Carbon . | Industrial and Engineering Chemistry Research , 2025 , 64 (32) , 15512-15522 . |
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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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