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学者姓名：章永凡
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Abstract ：
A series of novel halogen-functionalized imidazolium halides were successfully designed and synthesized by grafting halogenated hydrocarbons on the side chain of imidazolium and were applied to catalyze the intermolecular dehydration of alcohols. Under metal-free, acid-free, solvent-free, mild conditions and in an air atmosphere, 1-(4-bromobutyl)-3-methylimidazolium bromide was found to efficiently catalyze the etherification of monohydric alcohols and diols, as well as the synthesis of certain unsymmetrical ethers. Interestingly, the immiscibility between ethers and ionic liquids resulted in the spontaneous separation of the catalyst from the product, which made this strategy highly applicable in the etherification. Furthermore, detailed mechanistic studies revealed that [BBrmim]Br formed a unique intermediate with a series of alcohol molecules, in which internal hydrogen atoms successfully underwent hydrogen transfer via hydrogen bonding, thereby ensuring a smooth catalytic process.
Keyword ：
1-(4-Bromobutyl)-3-methyl-imidazolium bromide 1-(4-Bromobutyl)-3-methyl-imidazolium bromide Hydrogen transfer Hydrogen transfer Intermolecular dehydration Intermolecular dehydration Ionic liquid Ionic liquid
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| GB/T 7714 | Wu, Shi , Ai, Zhiwei , Chen, Limei et al. 1-(4-Bromobutyl)-3-methyl-imidazolium Bromide: A Novel Green Ionic Liquid Catalyst for Intermolecular Dehydration of Alcohols [J]. | CHEMISTRYSELECT , 2025 , 10 (2) . |
| MLA | Wu, Shi et al. "1-(4-Bromobutyl)-3-methyl-imidazolium Bromide: A Novel Green Ionic Liquid Catalyst for Intermolecular Dehydration of Alcohols" . | CHEMISTRYSELECT 10 . 2 (2025) . |
| APA | Wu, Shi , Ai, Zhiwei , Chen, Limei , Tao, Huilin , Liu, Jia , Wang, Jia et al. 1-(4-Bromobutyl)-3-methyl-imidazolium Bromide: A Novel Green Ionic Liquid Catalyst for Intermolecular Dehydration of Alcohols . | CHEMISTRYSELECT , 2025 , 10 (2) . |
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Localized surface plasmon resonance (LSPR) on base-metal nanoparticles holds significant potential for applications in diverse fields owing to its capability for electric field enhancement. Nevertheless, the efficiency of single-energy conversion remains a limiting factor for LSPR applications. This study investigated the utilization of hot carriers, generated through the LSPR effect in copper nanoparticles (Cu NPs) supported on ZrO2, to enhance the performance of the thermal catalytic reverse water-gas shift (RWGS) reaction. Finite difference time domain simulations and Kelvin probe force microscopy (KPFM) tests demonstrated that LSPR induces a strong electric field, facilitating the excitation of hot carriers in Cu NPs. In-situ DRIFTS analysis revealed that hot electrons promote the formation of formate species (HCOO*) and their subsequent transformation into CO, identified as the rate-determining step. Furthermore, in-situ H2 pulse and quasi-in situ EPR analyses indicated that photo-assisted thermal conditions enhance the conversion of H2 into active hydrogen species (H* or H + ) on Cu NPs, promoting the generation of oxygen vacancies and the transformation of intermediates. Constrained density functional theory calculations further demonstrated that visible light irradiation reduces energy barriers, thereby increasing reaction efficiency. The findings provide valuable insights into the contribution of LSPR-induced hot electrons in advancing the RWGS reaction.
Keyword ：
Cu/ZrO 2 Cu/ZrO 2 Hot carriers Hot carriers Localized surface plasmon resonance Localized surface plasmon resonance Oxygen vacancies Oxygen vacancies Reverse water gas shift reaction Reverse water gas shift reaction
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| GB/T 7714 | Ni, Wenkang , Zhang, Xiaoyan , Yue, Xuanyu et al. Visible light enhanced thermocatalytic reverse water gas shift reaction via localized surface plasmon resonance of copper nanoparticles [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2025 , 361 . |
| MLA | Ni, Wenkang et al. "Visible light enhanced thermocatalytic reverse water gas shift reaction via localized surface plasmon resonance of copper nanoparticles" . | SEPARATION AND PURIFICATION TECHNOLOGY 361 (2025) . |
| APA | Ni, Wenkang , Zhang, Xiaoyan , Yue, Xuanyu , Zhang, Zizhong , Zhang, Yongfan , Wang, Ke et al. Visible light enhanced thermocatalytic reverse water gas shift reaction via localized surface plasmon resonance of copper nanoparticles . | SEPARATION AND PURIFICATION TECHNOLOGY , 2025 , 361 . |
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Electrochemical interfaces between polymer electrolytes and electrodes are central to electrochemical devices in the global transition towards renewable energy. Here we show that the adsorption and desorption of sulfonates in Nafion on Pt(111) involve distinct elementary steps, with the latter proceeding through a coupled cation-electron transfer. Adsorbed sulfonates not only block a fraction of surface Pt sites but, more importantly, generate two additional types of surface adsorbate, OHNafion and ONafion, which exhibit distinct kinetic properties from adsorbed OH and O on bare Pt(111), respectively. The impact of the adsorption of sulfonate groups in Nafion on the activity of the oxygen reduction reaction (ORR) on Pt cannot be rationalized by existing thermodynamic descriptors. The reduced ORR activity on the Nafion-covered Pt(111) is caused by the kinetically hindered *O ->*OH conversion and *OH reduction on sites close to adsorbed sulfonates.
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| GB/T 7714 | Zhao, Kaiyue , Luo, Mingchuan , Zhang, Yongfan et al. Coupled cation-electron transfer at the Pt(111)/perfluoro-sulfonic acid ionomer interface and its impact on the oxygen reduction reaction kinetics [J]. | NATURE CATALYSIS , 2025 , 8 (1) : 46-57 . |
| MLA | Zhao, Kaiyue et al. "Coupled cation-electron transfer at the Pt(111)/perfluoro-sulfonic acid ionomer interface and its impact on the oxygen reduction reaction kinetics" . | NATURE CATALYSIS 8 . 1 (2025) : 46-57 . |
| APA | Zhao, Kaiyue , Luo, Mingchuan , Zhang, Yongfan , Chang, Xiaoxia , Xu, Bingjun . Coupled cation-electron transfer at the Pt(111)/perfluoro-sulfonic acid ionomer interface and its impact on the oxygen reduction reaction kinetics . | NATURE CATALYSIS , 2025 , 8 (1) , 46-57 . |
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3,4-ethylenedioxythiophene (EDOT) unit featuring electron donor and self-structuring properties, has been considered as the conducting polymers resources for organic electronic devices. However, construction of covalent organic frameworks (COFs) with EDOT building blocks has not been reported. Herein, a novel conductive EDOT-based COF (EDOT-Por-COF) with enhanced chemical interaction and conductivity was synthesized as the electrocatalysts accelerating the conversion kinetics of soluble polysulfides. The corresponding EDOT-Por-COF with electron-rich conjugated microenvironment generates higher sulfur affinity and polysulfides catalytic activity, which is further verified by experimental data and density functional theory (DFT) calculations. The introduction of an electron-rich surrounding environment alleviates the tendency of charge loss at Co sites and guarantees an optimized electronic structure around the Co sites, thus improving the adsorption strength and electron transfer between the Co sites and polysulfides, contributing to an improved catalytic capability on polysulfides. As a result, the assembled cell displays a ultrahigh discharge capacity of 1585.9 mAh g- 1 at 0.1 C, a low the capacity decay rate of 0.031 % per cycle for 2000 cycles at 1 C and a high rate capacity of 763.9 mAh g- 1 at 5 C. This work supports a new insight into electrocatalyst structural regulation to boost the electrochemical performance of Li-S batteries.
Keyword ：
Battery separators Battery separators Chemical microenvironment Chemical microenvironment Covalent organic frameworks Covalent organic frameworks High-performance Li-S batteries High-performance Li-S batteries Polysulfides Polysulfides
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| GB/T 7714 | Han, Diandian , Qin, Wenliang , Qiu, Mei et al. Covalent organic frameworks with conductive EDOT unit for superior lithium-sulfur batteries [J]. | NANO ENERGY , 2025 , 134 . |
| MLA | Han, Diandian et al. "Covalent organic frameworks with conductive EDOT unit for superior lithium-sulfur batteries" . | NANO ENERGY 134 (2025) . |
| APA | Han, Diandian , Qin, Wenliang , Qiu, Mei , Zhu, Zhiqiang , Zhang, Lin , Li, Haojie et al. Covalent organic frameworks with conductive EDOT unit for superior lithium-sulfur batteries . | NANO ENERGY , 2025 , 134 . |
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Piezo-photocatalysis is a frontier technology for converting mechanical and solar energies into crucial chemical substances and has emerged as a promising and sustainable strategy for N-2 fixation. Here, for the first time, defects and piezoelectric field are synergized to achieve unprecedented piezo-photocatalytic nitrogen reduction reaction (NRR) activity and their collaborative catalytic mechanism is unraveled over BaTiO3 with tunable oxygen vacancies (OVs). The introduced OVs change the local dipole state to strengthen the piezoelectric polarization of BaTiO3, resulting in a more efficient separation of photogenerated carrier. Ti3+ sites adjacent to OVs promote N-2 chemisorption and activation through d-pi back-donation with the help of the unpaired d-orbital electron. Furthermore, a piezoelectric polarization field could modulate the electronic structure of Ti3+ to facilitate the activation and dissociation of N-2, thereby substantially reducing the reaction barrier of the rate-limiting step. Benefitting from the synergistic reinforcement mechanism and optimized surface dynamics processes, an exceptional piezo-photocatalytic NH3 evolution rate of 106.7 mu mol g(-1) h(-1) is delivered by BaTiO3 with moderate OVs, far surpassing that of previously reported piezocatalysts/piezo-photocatalysts. New perspectives are provided here for the rational design of an efficient piezo-photocatalytic system for the NRR.
Keyword ：
defect engineering defect engineering nitrogen fixation nitrogen fixation piezoelectric field piezoelectric field piezo-photocatalysis piezo-photocatalysis
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| GB/T 7714 | Yuan, Jie , Feng, Wenhui , Zhang, Yongfan et al. Unraveling Synergistic Effect of Defects and Piezoelectric Field in Breakthrough Piezo-Photocatalytic N2 Reduction [J]. | ADVANCED MATERIALS , 2024 , 36 (5) . |
| MLA | Yuan, Jie et al. "Unraveling Synergistic Effect of Defects and Piezoelectric Field in Breakthrough Piezo-Photocatalytic N2 Reduction" . | ADVANCED MATERIALS 36 . 5 (2024) . |
| APA | Yuan, Jie , Feng, Wenhui , Zhang, Yongfan , Xiao, Jianyu , Zhang, Xiaoyan , Wu, Yinting et al. Unraveling Synergistic Effect of Defects and Piezoelectric Field in Breakthrough Piezo-Photocatalytic N2 Reduction . | ADVANCED MATERIALS , 2024 , 36 (5) . |
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The understanding of electron transfer pathways and orbital interactions between analytes and adsorption sites in gas-sensitive studies, especially at the atomic level, is currently limited. Herein, we have designed eight isoreticular catechol-metalloporphyrin scaffolds, FeTCP-M and InTCP-M (TCP = 5,10,15,20tetrakis-catechol-porphyrin, M = Fe, Co, Ni and Zn) with adjustable charge transfer schemes in the coordination microenvironment and precise tuning of orbital interactions between analytes and adsorption sites, which can be used as models for exploring the influence of these factors on gas sensing. Our experimental findings indicate that the sensitivity and selectivity can be modulated using the type of metals in the metal-catechol chains (which regulate the electron transfer routes) and the metalloporphyrin rings (which fine-tune the orbital interactions between analytes and adsorption sites). Among the isostructures, InTCP-Co demonstrates the highest response and selectivity to NO2 under visible light irradiation, which could be attributed to the more favorable transfer pathway of charge carriers in the coordination microenvironment under visible light illumination, as well as the better electron spin state compatibility, higher orbital overlap and orbital symmetry matching between the N(2)s2pz hybrid orbital of NO2 and the Co-3d(z)(2) orbital of InTCP-Co.
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| GB/T 7714 | Chen, Er-Xia , He, Liang , Qiu, Mei et al. Regulating electron transfer and orbital interaction within metalloporphyrin-MOFs for highly sensitive NO2 sensing [J]. | CHEMICAL SCIENCE , 2024 , 15 (18) : 6833-6841 . |
| MLA | Chen, Er-Xia et al. "Regulating electron transfer and orbital interaction within metalloporphyrin-MOFs for highly sensitive NO2 sensing" . | CHEMICAL SCIENCE 15 . 18 (2024) : 6833-6841 . |
| APA | Chen, Er-Xia , He, Liang , Qiu, Mei , Zhang, Yongfan , Sun, Yayong , Li, Wen-Hua et al. Regulating electron transfer and orbital interaction within metalloporphyrin-MOFs for highly sensitive NO2 sensing . | CHEMICAL SCIENCE , 2024 , 15 (18) , 6833-6841 . |
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Optimizing friction materials based on molecular diversity in a molecular framework system is an effective method to improve the output performance of triboelectric nanogenerators (TENGs). In this study, three cadmium(II) metal-organic frameworks (Cd-MOFs) with different cavities were synthesized solvothermally by the assembly of cadmium nitrate (Cd(NO3)2 & sdot;4H2O), 4 ',4 '''-carbonylbis(([1,1 '-biphenyl]-3,5-dicarboxylic acid)) (H4CBBD), and trans-1,2-bis(4-pyridyl)ethylene (4,4 '-bpe) via a solvent-regulated strategy. The topology and porosity of Cd-MOFs could be controlled effectively by the solvent constituents and were demonstrated to be closely related to their triboelectric behaviors. Theoretical calculations and experimental characterizations revealed that the TENGs fabricated by the Cd-MOF with maximum porosity exhibited the best triboelectric performance owing to the enhanced specific surface area and surface potential. In the applications, the highoutput TENGs can be successfully used as an efficient power supply for electrochemical systems, enabling the direct bromination of aromatic compounds in high yields with good regioselectivity. This study provides a simple and feasible method to optimize positive friction materials at the molecular level and develops the practical applications of TENGs in electrochemical systems.
Keyword ：
Bromination Bromination Electrochemical system Electrochemical system Metal-organic frameworks Metal-organic frameworks Solvent-regulated strategy Solvent-regulated strategy Triboelectric nanogenerator Triboelectric nanogenerator
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| GB/T 7714 | Huang, Chao , Zhang, Qiang , Zhang, Yue et al. Self-driven electrochemical system using solvent-regulated structural diversity of cadmium(II) metal-organic frameworks [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2024 , 662 : 953-961 . |
| MLA | Huang, Chao et al. "Self-driven electrochemical system using solvent-regulated structural diversity of cadmium(II) metal-organic frameworks" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 662 (2024) : 953-961 . |
| APA | Huang, Chao , Zhang, Qiang , Zhang, Yue , Wang, Fei , Zhang, Ying-Ying , Qiu, Mei et al. Self-driven electrochemical system using solvent-regulated structural diversity of cadmium(II) metal-organic frameworks . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2024 , 662 , 953-961 . |
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The inherent structural flexibility and reversibility of non-covalent organic frameworks have enabled them to exhibit switchable multistate structures under external stimuli, providing great potential in the field of resistive switching (RS), but not well explored yet. Herein, we report the 0D+1D hydrogen-bonded polycatenation non-covalent organic framework (HOF-FJU-52), exhibiting diverse and reversible RS behaviors with the high performance. Triggered by the external stimulus of electrical field E at room temperature, HOF-FJU-52 has excellent resistive random-access memory (RRAM) behaviors, comparable to the state-of-the-art materials. When cooling down below 200 K, it was transferred to write-once-read-many-times memory (WORM) behaviors. The two memory behaviors exhibit reversibility on a single crystal device through the temperature changes. The RS mechanism of this non-covalent organic framework has been deciphered at the atomic level by the detailed single-crystal X-ray diffraction analyses, demonstrating that the structural dual-flexibility both in the asymmetric hydrogen bonded dimers within the 0D loops and in the infinite pi-pi stacking column between the loops and chains contribute to reversible structure transformations between multi-states and thus to its dual RS behaviors. Hydrogen-bonded organic frameworks as stimuli responsive multistate structures show potential in the field of resistive switching. Here, the authors report a 0D+1D hydrogen-bonded polycatenation non-covalent organic framework showing reversible transformation of multistate-structures triggered by electrical field and temperature, enabling reversibly switchable resistive random-access memory and write-once-read-many-times memory behavior.
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| GB/T 7714 | Chen, Shimin , Ju, Yan , Yang, Yisi et al. Multistate structures in a hydrogen-bonded polycatenation non-covalent organic framework with diverse resistive switching behaviors [J]. | NATURE COMMUNICATIONS , 2024 , 15 (1) . |
| MLA | Chen, Shimin et al. "Multistate structures in a hydrogen-bonded polycatenation non-covalent organic framework with diverse resistive switching behaviors" . | NATURE COMMUNICATIONS 15 . 1 (2024) . |
| APA | Chen, Shimin , Ju, Yan , Yang, Yisi , Xiang, Fahui , Yao, Zizhu , Zhang, Hao et al. Multistate structures in a hydrogen-bonded polycatenation non-covalent organic framework with diverse resistive switching behaviors . | NATURE COMMUNICATIONS , 2024 , 15 (1) . |
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Two novel vanadoborate compounds, [Cu(en)2]3[Li(H2O)]4[Li(H2O)3]2[V12B18O50(OH)10(H2O)]2 & sdot;33.5H2O (1) and (H2en)4[Li(H2O)]4[V12B18O55(OH)5(H2O)]& sdot;14H2O (2), were synthesized via hydrothermal synthesis under identical conditions except for temperature. Structural analysis revealed that although both contain [V12B18O60]n- cluster anion, the different countercations potentially lead to variations in the [V12B18O60]ncluster anion skeletons. In compound 1, the V4+/V5+ ratio was 10:2; while in compound 2 the ratio was 11:1. It is speculated that different countercations may influence the valence states of cluster anions. In this study, quantum chemical calculations revealed that the aromaticity and activity of the two compounds were different, and twodimensional correlation infrared spectroscopy (2D-COS-IR) under magnetic perturbation confirmed that distinct response peaks of functional group vibrations to the magnetic field due to the different V4+/V5+ ratios and aromaticity of the two compounds. An electrochemical analysis revealed that compound 2 exhibits higher electrocatalytic activity. The results of quantum chemical calculations are aligned not only with the changes in the 2D-COS-IR spectra but also with the conclusions obtained from experiments on electrochemical properties. Overall, this work proposes a novel strategy for interpreting the alteration of vanadoborate anionic skeleton due to the introduction of different countercations by combining 2D-COS-IR with quantum chemical calculations.
Keyword ：
Electrocatalyst Electrocatalyst Quantum chemical calculation Quantum chemical calculation spectroscopy spectroscopy Two-dimensional correlation infrared Two-dimensional correlation infrared Vanadoborate Vanadoborate
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| GB/T 7714 | Meng, Ming-Ze , Shi, Gui-Dong , Cheng, Ling-Ling et al. Two-dimensional correlation infrared spectroscopy study on vanadoborate anionic skeleton regulated by countercations [J]. | SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY , 2024 , 311 . |
| MLA | Meng, Ming-Ze et al. "Two-dimensional correlation infrared spectroscopy study on vanadoborate anionic skeleton regulated by countercations" . | SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY 311 (2024) . |
| APA | Meng, Ming-Ze , Shi, Gui-Dong , Cheng, Ling-Ling , Chen, Yi-Ping , Zhang, Yong-Fan , Lin, Wei . Two-dimensional correlation infrared spectroscopy study on vanadoborate anionic skeleton regulated by countercations . | SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY , 2024 , 311 . |
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Correction to: Nature Communications, published online 5 January 2024 In this article the grant number 22271046 relating to Natural Science Foundation of China was omitted. The original article has been corrected. © 2024, The Author(s).
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| GB/T 7714 | Chen, S. , Ju, Y. , Yang, Y. et al. Author Correction: Multistate structures in a hydrogen-bonded polycatenation non-covalent organic framework with diverse resistive switching behaviors (Nature Communications, (2024), 15, 1, (298), 10.1038/s41467-023-44214-x) [未知]. |
| MLA | Chen, S. et al. "Author Correction: Multistate structures in a hydrogen-bonded polycatenation non-covalent organic framework with diverse resistive switching behaviors (Nature Communications, (2024), 15, 1, (298), 10.1038/s41467-023-44214-x)" [未知]. |
| APA | Chen, S. , Ju, Y. , Yang, Y. , Xiang, F. , Yao, Z. , Zhang, H. et al. Author Correction: Multistate structures in a hydrogen-bonded polycatenation non-covalent organic framework with diverse resistive switching behaviors (Nature Communications, (2024), 15, 1, (298), 10.1038/s41467-023-44214-x) [未知]. |
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