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学者姓名：刘哲源
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The uncontrolled dendritic growth and severe side reactions significantly constrain zinc-ion batteries' further application. This study presents a novel micellar gel electrolyte, innovatively designed through hydrophobic association. The micellar gel electrolyte harmonizes macroscopic and microscopic properties through a rational hierarchical design. At the macroscopic level, the hydrophilic domains as water-absorbing nets and the hydrophobic domains as pillars are intricately interwoven. On the microscopic scale, the copolymerization resulted in a microphase-separated architecture, with hydrophilic and hydrophobic domains establishing distinct micro-regions within the gel matrix. The hydrophilic domains contribute to the stabilization of the hydrogen bond network through amide groups, while the abundant carbonyl groups optimize the solvation structure and migration pathways of Zn2+. The hydrophobic domains provide a robust supporting framework while simultaneously reducing H2O activity and thereby minimizing parasitic reactions. Thus, the enhanced interfacial stability forms a robust and flexible barrier against dendrite formation. The rational hierarchical gel composition and cross-linked network effectively direct Zn deposition preferentially along the (002) plane, ensuring a uniform and stable interface. The assembled Zn & Vert;MnO2 batteries show 80% capacity retention after 1200 cycles at 1C.
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| GB/T 7714 | Chen, Zheming , Lin, Yushuang , Shi, Dehuan et al. Rational hierarchical micellar gel electrolytes with synergistic hydrophobic-hydrophilic integration for dendrite-free zinc-ion batteries [J]. | JOURNAL OF MATERIALS CHEMISTRY A , 2025 , 13 (9) : 6709-6718 . |
| MLA | Chen, Zheming et al. "Rational hierarchical micellar gel electrolytes with synergistic hydrophobic-hydrophilic integration for dendrite-free zinc-ion batteries" . | JOURNAL OF MATERIALS CHEMISTRY A 13 . 9 (2025) : 6709-6718 . |
| APA | Chen, Zheming , Lin, Yushuang , Shi, Dehuan , Song, Kangwei , Luo, Jing , Qiu, Yanbin et al. Rational hierarchical micellar gel electrolytes with synergistic hydrophobic-hydrophilic integration for dendrite-free zinc-ion batteries . | JOURNAL OF MATERIALS CHEMISTRY A , 2025 , 13 (9) , 6709-6718 . |
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Covalent organic frameworks (COFs) are promising semiconductor photocatalysts but are still limited in overall water splitting mainly owing to a lack of clear design approaches with which to ameliorate catalytic activities. Here, we demonstrate a synergy of exciton dipole orientation and dynamic reactivity of COFs that enables water splitting for stoichiometric evolution of H2 and O2. The exciton dipole orientation is responsible for driving the spatial separation of photoinduced charges, while the dynamic reactivity of imine bonds of COFs with water and holes is proven for initiating water oxidation. Accordingly, a rationally designed BtS-COF with benzotrithiophene and sulfone units exhibits a much-improved performance in H2 and O2 evolution in neutral water under visible light. Its catalytic efficiency is even superior to some photocatalysts with metal-based water oxidation cocatalyst.
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| GB/T 7714 | Niu, Qing , Deng, Wenfeng , Chen, Yanlei et al. Exciton Dipole Orientation and Dynamic Reactivity Synergistically Enable Overall Water Splitting in Covalent Organic Frameworks [J]. | ACS ENERGY LETTERS , 2024 , 9 (12) : 5830-5835 . |
| MLA | Niu, Qing et al. "Exciton Dipole Orientation and Dynamic Reactivity Synergistically Enable Overall Water Splitting in Covalent Organic Frameworks" . | ACS ENERGY LETTERS 9 . 12 (2024) : 5830-5835 . |
| APA | Niu, Qing , Deng, Wenfeng , Chen, Yanlei , Lin, Qingqing , Li, Liuyi , Liu, Zheyuan et al. Exciton Dipole Orientation and Dynamic Reactivity Synergistically Enable Overall Water Splitting in Covalent Organic Frameworks . | ACS ENERGY LETTERS , 2024 , 9 (12) , 5830-5835 . |
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The structure-activity relationship between the metal center and regio-selectivity is persistently a pivotal scientific issue. To address this, we select the 2-phenylpyridine sulfonylation reactions catalyzed by ruthenium and palladium as research subjects. An extensive theoretical study has been conducted on their reaction mechanisms, the sources of regio-selectivity, and the evolution of electronic structures. The distinct electronic structures lead to completely different catalytic mechanisms and electronic structure evolution processes for ruthenium and palladium. Ruthenium tends to form six-coordinate octahedral complexes, thus undergoing an inner-sphere redox active Ru(II)-Ru(III)-Ru(IV)-Ru(II) catalytic cycle. In contrast, palladium tends to form four-coordinate planar quadrilateral complexes, hence undergoing an outer-sphere redox neutral Pd(II) catalytic cycle. The distinct electronic structure evolution processes fundamentally differentiate the radical attack modes in the sulfonation process, thereby determining the regio-selectivity of the reaction. In the Ru-catalyzed system, the meta-selectivity arises mainly from a more stable Schrock carbene-type meta-intermediate. For the Pd-catalyzed system, the ortho-selectivity mainly comes from the stabilizing effect of the Pd(II) center on the single electron. This study provides novel insights into how the electronic structure of metal centers influences the reaction mechanism and selectivity, making a theoretical contribution to a deeper comprehension of the mechanism and regio-selectivity underlying aromatic functionalization reactions.
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| GB/T 7714 | Lin, Qingqing , Lv, Huan , Lu, Yu et al. Redox Active vs Redox Neutral in Ru/Pd-Catalyzed Sulfonylation: Theoretical Insights into Structure-Activity Relationship between Metal Centers and Regio-Selectivity [J]. | JOURNAL OF ORGANIC CHEMISTRY , 2024 , 89 (24) : 18131-18141 . |
| MLA | Lin, Qingqing et al. "Redox Active vs Redox Neutral in Ru/Pd-Catalyzed Sulfonylation: Theoretical Insights into Structure-Activity Relationship between Metal Centers and Regio-Selectivity" . | JOURNAL OF ORGANIC CHEMISTRY 89 . 24 (2024) : 18131-18141 . |
| APA | Lin, Qingqing , Lv, Huan , Lu, Yu , Yang, Chengkai , Yu, Yan , Liu, Zheyuan . Redox Active vs Redox Neutral in Ru/Pd-Catalyzed Sulfonylation: Theoretical Insights into Structure-Activity Relationship between Metal Centers and Regio-Selectivity . | JOURNAL OF ORGANIC CHEMISTRY , 2024 , 89 (24) , 18131-18141 . |
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Modulating interfacial electrochemistry represents a prevalent approach for mitigating lithium dendrite growth and enhancing battery performance. Nevertheless, while most additives exhibit inhibitory characteristics, the accelerating effects on interfacial electrochemistry have garnered limited attention. In this work, perfluoromorpholine (PFM) with facilitated kinetics is utilized to preferentially adsorb on the lithium metal interface. The PFM molecules disrupt the solvation structure of Li+ and enhance the migration of Li+. Combined with the benzotrifluoride, a synergistic acceleration-inhibition system is formed. The ab initio molecular dynamics (AIMD) and density functional theory (DFT) calculation of the loose outer solvation clusters and the key adsorption–deposition step supports the fast diffusion and stable interface electrochemistry with an accelerated filling mode with C─F and C─H groups. The approach induces the uniform lithium deposition. Excellent cycling performance is achieved in Li||Li symmetric cells, and even after 200 cycles in Li||NCM811 full cells, 80% of the capacity is retained. This work elucidates the accelerated electrochemical processes at the interface and expands the design strategies of acceleration fluorinated additives for lithium metal batteries. © 2024 Wiley-VCH GmbH.
Keyword ：
acceleration acceleration AIMD AIMD interfacial adsorption interfacial adsorption lithium metal batteries lithium metal batteries outer and inner solvation cluster outer and inner solvation cluster
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| GB/T 7714 | Zheng, X. , Qiu, Y. , Luo, J. et al. Perfluorinated Amines: Accelerating Lithium Electrodeposition by Tailoring Interfacial Structure and Modulated Solvation for High-Performance Batteries [J]. | Small , 2024 , 20 (44) . |
| MLA | Zheng, X. et al. "Perfluorinated Amines: Accelerating Lithium Electrodeposition by Tailoring Interfacial Structure and Modulated Solvation for High-Performance Batteries" . | Small 20 . 44 (2024) . |
| APA | Zheng, X. , Qiu, Y. , Luo, J. , Yang, S. , Yu, Y. , Liu, Z. et al. Perfluorinated Amines: Accelerating Lithium Electrodeposition by Tailoring Interfacial Structure and Modulated Solvation for High-Performance Batteries . | Small , 2024 , 20 (44) . |
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Doping is a recognized method for enhancing catalytic performance. The introduction of strains is a common consequence of doping, although it is often overlooked. Differentiating the impact of doping and strain on catalytic performance poses a significant challenge. In this study, Cu-doped Bi catalysts with substantial tensile strain are synthesized. The synergistic effects of doping and strain in bismuth result in a remarkable CO2RR performance. Under optimized conditions, Cu-1/6-Bi demonstrates exceptional formate Faradaic efficiency (>95%) and maintains over 90% across a wide potential window of 900 mV. Furthermore, it delivers an industrial-relevant partial current density of -317 mA cm(-2) at -1.2 V-RHE in a flow cell, while maintaining its selectivity. Additionally, it exhibits exceptional long-term stability, surpassing 120 h at -200 mA cm(-2). Through experimental and theoretical mechanistic investigations, it has been determined that the introduction of tensile strain facilitates the adsorption of *CO2, thereby enhancing the reaction kinetics. Moreover, the presence of Cu dopants and tensile strain further diminishes the energy barrier for the formation of *OCHO intermediate. This study not only offers valuable insights for the development of effective catalysts for CO2RR through doping, but also establishes correlations between doping, lattice strains, and catalytic properties of bismuth catalysts.
Keyword ：
bismuth bismuth CO2 reduction CO2 reduction doping doping strain strain synergistic effect synergistic effect
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| GB/T 7714 | Wei, Yang , Xu, Xin , Shi, Dehuan et al. Synergistic Effects of Doping and Strain in Bismuth Catalysts for CO2 Electroreduction [J]. | SMALL , 2024 , 20 (34) . |
| MLA | Wei, Yang et al. "Synergistic Effects of Doping and Strain in Bismuth Catalysts for CO2 Electroreduction" . | SMALL 20 . 34 (2024) . |
| APA | Wei, Yang , Xu, Xin , Shi, Dehuan , Jiang, Yaming , Zheng, Chaoyang , Tan, Li et al. Synergistic Effects of Doping and Strain in Bismuth Catalysts for CO2 Electroreduction . | SMALL , 2024 , 20 (34) . |
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Lanthanide ion contained metal-organic frameworks (MOFs) have garnered significant attention in the fields of solid-state lighting and chemical sensing due to their porous structure and distinctive optical properties. However, they also present challenges because of the limited photoluminescence (PL) intensity resulting from the parity-forbidden f-f transitions of lanthanide ions. Herein, the study reports a new heterometallic MOFs Ln3Li2L4 (Li-Ln-MOF, Ln = Y, Eu, Tb and Dy, L = deprotonated 1,3,5-tris(4-carboxyphenyl)benzene) with a Brunauer-Emmett-Teller (BET) surface area of 774.1 m2/g. The porous crystal structure of Li-Ln-MOF is characterized by three kinds of channels interpenetrating with each other. By employing ligand alternation and lanthanide ion alloying strategies, Li-Y1-xEux-MOF1 crystal isostructural with Li-Ln-MOF is synthesized by using 2,4,6-tris(4-carboxyphenyl)-1,3,5-triazine (H3TATB) as ligand. The Li-Y0.7Eu0.3-MOF1 crystal excels in the comprehensive performance with a BET surface area of 858.8 m2 g-1 and a near-unity PL quantum yield. The time density functional theory and natural transition orbitals calculations unravel that the outstanding optical properties Li-Y0.7Eu0.3-MOF1 originates from the charge transfer between TATB3- and Eu3+. Benefiting from the excellent comprehensive performance of Li-Y1-xEux-MOF1, the study reveals their potentials as single-composition white-light emission and fluorescent sensing probe for the detection of nitrobenzene. A strategy via ligand alteration is developed to achieve a near-unity photoluminescence quantum yield in lanthanide metal-organic frameworks (Ln-MOFs) with a porosity of up to 53.6%. Mechanistic investigation through theoretical calculation and time-resolved spectra unravel that Ln-MOF displayed outstanding optical properties ascribed to the charge transfer from the triple excited state of ligand to the Ln3+. image
Keyword ：
fluorescent sensing fluorescent sensing lanthanide-organic frameworks lanthanide-organic frameworks ligand alteration ligand alteration photoluminescence photoluminescence white-light emission white-light emission
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| GB/T 7714 | Zhang, Wei , Wang, En-Ting , Li, Xinhao et al. Lithium-Lanthanide Heterometallic Organic Frameworks with Near-Unity Photoluminescence Quantum Yields for Single-Composition White-Light Emission and Fluorescent Sensing on Nitrobenzene [J]. | ADVANCED OPTICAL MATERIALS , 2024 , 12 (21) . |
| MLA | Zhang, Wei et al. "Lithium-Lanthanide Heterometallic Organic Frameworks with Near-Unity Photoluminescence Quantum Yields for Single-Composition White-Light Emission and Fluorescent Sensing on Nitrobenzene" . | ADVANCED OPTICAL MATERIALS 12 . 21 (2024) . |
| APA | Zhang, Wei , Wang, En-Ting , Li, Xinhao , Huang, Weixin , Sun, Yakun , Liu, Zheyuan et al. Lithium-Lanthanide Heterometallic Organic Frameworks with Near-Unity Photoluminescence Quantum Yields for Single-Composition White-Light Emission and Fluorescent Sensing on Nitrobenzene . | ADVANCED OPTICAL MATERIALS , 2024 , 12 (21) . |
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To meet the demand for higher energy density in lithium-ion batteries, extensive research has focused on advanced cathodes and metallic lithium anodes. However, Ni-rich cathodes suffer from the inactive phase-transition and side reactions at the cathode-electrolyte interfaces (CEI). In this study, we propose a novel approach to enhance the solubility of LiNO3 in carbonate electrolyte systems using a local high-concentrated addition strategy with triethyl phosphate as a co-solvent. Rather than the traditional solvent-dominated solvation clusters, the NO3− dominated electrolyte is examined to elucidate unique complexation phenomena. Two distinct clusters in NO3− dominated electrolyte arising from as a consequence of intramolecular interactions intrinsic to the constituents. This promotes the formation of a homogeneous oxynitride interphase and facilitates more expeditious lithium ion diffusion kinetics. Hence, the less stress fragmentation and irreversible phase transformation occur on the cathode surface with the homogeneous oxynitridation interface. This innovative design enables efficient cycling of the Li || NCM811 cell, offering a promising strategy to improve lithium-ion batteries performance. © 2024 Elsevier B.V.
Keyword ：
Ab initio molecular dynamics Ab initio molecular dynamics Lithium batteries Lithium batteries Ni-rich cathodes Ni-rich cathodes NO3− dominated weakly dissociated solvation clusters NO3− dominated weakly dissociated solvation clusters Solvent-dominated solvation clusters Solvent-dominated solvation clusters
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| GB/T 7714 | Xiao, Y. , Zhang, W. , Dong, W. et al. Enhancing the Cathode/Electrolyte interface in Ni-Rich Lithium-Ion batteries through homogeneous oxynitridation enabled by NO3− dominated clusters [J]. | Chemical Engineering Journal , 2024 , 494 . |
| MLA | Xiao, Y. et al. "Enhancing the Cathode/Electrolyte interface in Ni-Rich Lithium-Ion batteries through homogeneous oxynitridation enabled by NO3− dominated clusters" . | Chemical Engineering Journal 494 (2024) . |
| APA | Xiao, Y. , Zhang, W. , Dong, W. , Yang, K. , Chao, Y. , Xi, C. et al. Enhancing the Cathode/Electrolyte interface in Ni-Rich Lithium-Ion batteries through homogeneous oxynitridation enabled by NO3− dominated clusters . | Chemical Engineering Journal , 2024 , 494 . |
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The serious dendrite formation and safety hazards associated with side reactions hinder the practical application of lithium metal batteries. A molecular customization strategy based on both physical and chemical properties is reported. A copolymer of acrylamide and hexafluorobutyl acrylate molecules is used as an artificial solid electrolyte interface(ASEI) for lithium metal to achieve dynamic interface protection during cycling. The amide group serves as the rigid unit, while the hexafluorobutyl group serves as the flexible unit, and imparts excellent mechanical properties to the copolymer. Synergistically abundant CF bonds exhibit excellent water and oxygen resistance and have good electrolyte affinity. The ester and amide groups serve as amphiphilic sites for Li+ and PF6-, regulating the ion flux at the interface and achieving dendrite-free lithium deposition. During cycling, the organic-inorganic composite SEI dynamically evolves to safeguard the lithium metal, preventing undue electrolyte consumption. The copolymer achieves stable cycling for 1500 and 950 h at 1 and 2 mA cm-2, respectively. It demonstrates excellent performance with LiNi0.8Co0.1Mn0.1O2 and LiFePO4 cathodes. This study introduces a new approach to designing polymers at the molecular level to optimize the physical properties/chemical activity of lithium metal interfaces. The serious dendrite formation and safety hazards associated with side reactions hinder the practical application of lithium metal batteries. A molecular customization polymer based on physicochemical properties as ASEI is reported. The copolymer has excellent mechanical properties and water and oxygen resistance. The ester and amide groups serve as amphiphilic sites, regulating the ion flux and achieving dendrite-free lithium deposition. image
Keyword ：
binary copolymer binary copolymer dendrite suppression dendrite suppression interface engineering interface engineering lithium metal anode lithium metal anode
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| GB/T 7714 | Luo, Jing , Huang, Qinzhui , Shi, Dehuan et al. Dynamic Interfacial Protection via Molecularly Tailored Copolymer for Durable Artificial Solid Electrolyte Interphase in Lithium Metal Batteries [J]. | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (39) . |
| MLA | Luo, Jing et al. "Dynamic Interfacial Protection via Molecularly Tailored Copolymer for Durable Artificial Solid Electrolyte Interphase in Lithium Metal Batteries" . | ADVANCED FUNCTIONAL MATERIALS 34 . 39 (2024) . |
| APA | Luo, Jing , Huang, Qinzhui , Shi, Dehuan , Qiu, Yanbin , Zheng, Xinyu , Yang, Sisheng et al. Dynamic Interfacial Protection via Molecularly Tailored Copolymer for Durable Artificial Solid Electrolyte Interphase in Lithium Metal Batteries . | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (39) . |
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Organic electrode materials are promising for next-generation energy storage materials due to their environmental friendliness and sustainable renewability. However, problems such as their high solubility in electrolytes and low intrinsic conductivity have always plagued their further application. Polymerization to form conjugated organic polymers can not only inhibit the dissolution of organic electrodes in the electrolyte, but also enhance the intrinsic conductivity of organic molecules. Herein, we synthesized a new conjugated organic polymer (COPs) COP500-CuT2TP (poly [5,10,15,20-tetra(2,2 '-bithiophen-5-yl) porphyrinato] copper (II)) by electrochemical polymerization method. Due to the self-exfoliation behavior, the porphyrin cathode exhibited a reversible discharge capacity of 420 mAh g-1, and a high specific energy of 900 Wh Kg-1 with a first coulombic efficiency of 96 % at 100 mA g-1. Excellent cycling stability up to 8000 cycles without capacity loss was achieved even at a high current density of 5 A g-1. This highly conjugated structure promotes COP500-CuT2TP combined high energy density, high power density, and good cycling stability, which would open new opportunity for the designable and versatile organic electrodes for electrochemical energy storage. A new porphyrin conjugated polymer cathode, COP500-CuT2TP is achieved under electrochemical polymerization. Self-exfoliation of polymer cathode promotes charge storage, leading to a specific capacity of 420 mAh g-1 and 900 Wh Kg-1. Excellent cycling stability up to 8000 cycles at 5 A g-1 is achieved. Mechanistic insights by combining experimental and computational investigations supports the charge storage performance. image
Keyword ：
conjugated organic polymers conjugated organic polymers lithium-ion batteries lithium-ion batteries porphyrin porphyrin thiophene thiophene
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| GB/T 7714 | Wu, Xing , Zhou, Wang , Ye, Chao et al. Porphyrin-Thiophene Based Conjugated Polymer Cathode with High Capacity for Lithium-Organic Batteries [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (14) . |
| MLA | Wu, Xing et al. "Porphyrin-Thiophene Based Conjugated Polymer Cathode with High Capacity for Lithium-Organic Batteries" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 14 (2024) . |
| APA | Wu, Xing , Zhou, Wang , Ye, Chao , Zhang, Jiahao , Liu, Zheyuan , Yang, Chengkai et al. Porphyrin-Thiophene Based Conjugated Polymer Cathode with High Capacity for Lithium-Organic Batteries . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (14) . |
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Studying lithium growth on diverse substrates with unique crystal structures is crucial for linking atomic and macroscopic views, which ensures a long cycle life and safety in lithium metal batteries. This work provides explanations on (1) the stages of nucleation, which are influenced by the adsorption-relaxation mechanism, (2) acquiring evolved traits of dendritic morphology from the embryo, and (3) the integration of the atomic and macroscopic perspectives through a variety of techniques at different scales to validate dendrite evolution. The heteroepitaxial growth process of the embryos is divided into two principal stages: nucleation and growth. The adsorption-type substrates exhibit characteristics of relatively lower average interaction energy and specific stress energy during the nucleation stage. At the growth stage, the adsorption-type substrate tends to facilitate multilayer growth. This work provides potential to design and material selection for lithium metal batteries, contributing to the development of safer, more efficient, and longer-lasting energy storage systems. © 2024 American Chemical Society.
Keyword ：
Crystal atomic structure Crystal atomic structure Epitaxial growth Epitaxial growth Indium phosphide Indium phosphide Lithium batteries Lithium batteries
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| GB/T 7714 | Li, Borong , Zhang, Weicheng , Yang, Kang et al. Bridging Atomic and Macroscopic Perspectives on Heteroepitaxial Growth in Lithium Metal Anodes [J]. | ACS Energy Letters , 2024 , 9 (10) : 5215-5224 . |
| MLA | Li, Borong et al. "Bridging Atomic and Macroscopic Perspectives on Heteroepitaxial Growth in Lithium Metal Anodes" . | ACS Energy Letters 9 . 10 (2024) : 5215-5224 . |
| APA | Li, Borong , Zhang, Weicheng , Yang, Kang , Li, Long , Luo, Jing , Lin, Qingqing et al. Bridging Atomic and Macroscopic Perspectives on Heteroepitaxial Growth in Lithium Metal Anodes . | ACS Energy Letters , 2024 , 9 (10) , 5215-5224 . |
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