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学者姓名：刘哲源
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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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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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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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As an important interaction among organic cations containing aromatic rings, the pi-pi stacking interaction is a crucial factor determining the crystal structure of organic-inorganic hybrid metal halides (OIMHs). However, the relationship between pi-pi interaction and optical properties of luminescent OIMHs is yet to be studied. (C10H10N2)Cd1-xZnxCl4 (23-Cd1-xZnxCl4) crystals with 0D structures are synthesized by using optically active 2,3 '-bipyridine as the organic ligand. When x <= 0.2, there is no pi-pi interaction among 2,3 '-bipyridinium cations in 23-Cd1-xZnxCl4 crystals. When x > 0.2, pi-pi interaction among organic cations occurs and enhances as the Zn2+ content increases. The tailoring of the pi-pi interaction endows 23-Cd1-xZnxCl4 with tunable light emitting properties, resulting in a broad band emission involving blue and orange species. The blue emission dominates when there is no pi-pi interaction, while the orange emission enhances and finally becomes dominant as the strength of pi-pi interaction increases. The pi-pi interaction promotes the energy transfer from the higher energy valley to the lower one of the S-1 state of the organic cation, resulting in the enhancement of orange emission. Notably, the 23-ZnCl crystal exhibits a photo-luminescence quantum yield (PLQY) of 32%. This is the highest reported value to date among the Zn-based OIMHs, which have optical emission originating from the organic component. The mechanism of pi-pi stacking induced tunable light emission revealed in our work provides new guidance for the design of luminescent OIMHs.
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| GB/T 7714 | Zhang, Qi , Lin, Xinyi , Guo, Shanji et al. Tailoring the π-π stacking interaction among organic cations in hybrid metal halide crystals towards tunable light emission [J]. | JOURNAL OF MATERIALS CHEMISTRY C , 2024 , 12 (19) : 7053-7061 . |
| MLA | Zhang, Qi et al. "Tailoring the π-π stacking interaction among organic cations in hybrid metal halide crystals towards tunable light emission" . | JOURNAL OF MATERIALS CHEMISTRY C 12 . 19 (2024) : 7053-7061 . |
| APA | Zhang, Qi , Lin, Xinyi , Guo, Shanji , Zhang, Yaqing , Jiang, Yan , Zhang, Wei et al. Tailoring the π-π stacking interaction among organic cations in hybrid metal halide crystals towards tunable light emission . | JOURNAL OF MATERIALS CHEMISTRY C , 2024 , 12 (19) , 7053-7061 . |
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Utilizing an interfacial layer to stabilize Zn-metal anodes has been extensively explored, often accompanied by inhibition of Zn dendrites. However, most interfacial layers primarily delay Zn2+ ion transport/transfer, leading to slow Zn deposition due to the ion kinetics hindrance. Basically, this ionic hysteresis effect is inherent to all interfacial layers and will cause unstable Zn deposition over extended cycling periods. Here, we present a simple composite interfacial layer composed of graphene acid (GA) and cellulose nanofibers (CNFs). In the CNF/GA layer, a delicate balance between the rapid Zn2+ transport/transfer and uniform Zn deposition is achieved. The presence of GA not only demonstrates excellent ion selectivity and suppresses corrosion reactions, but also promotes Zn2+ transport/transfer, significantly reducing the desolvation energy of Zn2+ ions. Consequently, the symmetric cell with CNF/GA coatings achieves a highly stable cycling life of 2920 h, surpassing previous reports using graphene-based and CNF-based protecting layers. Moreover, the full cell based on the CNF/GA protected anodes exhibits excellent long-term stability and maintains an ultra-stable self-discharge retention of 99% after 24 h of standing. These findings provide valuable insights for the development of protective layers for Zn-metal anodes and future grid-scale Zn battery deployment. © 2024 The Royal Society of Chemistry
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| GB/T 7714 | Xia, K. , Li, L. , Qiu, Y. et al. Graphene acid-enhanced interfacial layers with high Zn2+ ion selectivity and desolvation capability for corrosion-resistant Zn-metal anodes [J]. | Journal of Materials Chemistry A , 2024 , 12 (36) : 24175-24187 . |
| MLA | Xia, K. et al. "Graphene acid-enhanced interfacial layers with high Zn2+ ion selectivity and desolvation capability for corrosion-resistant Zn-metal anodes" . | Journal of Materials Chemistry A 12 . 36 (2024) : 24175-24187 . |
| APA | Xia, K. , Li, L. , Qiu, Y. , Weng, J. , Shen, S. , Chen, M. et al. Graphene acid-enhanced interfacial layers with high Zn2+ ion selectivity and desolvation capability for corrosion-resistant Zn-metal anodes . | Journal of Materials Chemistry A , 2024 , 12 (36) , 24175-24187 . |
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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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T-2 toxin (T-2), one of the most toxic mycotoxins, has drawn extensive attention due to its universality and persistence in food and the environment. In this study, a novel magnetic ZnO/CaFe2O4 nanocomposite with a p-n based Z-scheme heterojunction was successfully constructed by a hydrothermal method for efficient photodegradation of T-2 toxin. The optimal cubic structure of ZnO/CaFe2O4 endows it with excellent photocatalytic efficiency in removing T-2 toxin, such that near-total degradation was achieved with an exceptionally high mineralization value (64 %) after 180 min of UV radiation. This efficacy was attributed not only to the abundant reaction sites on the binary composites, but also its Z-scheme heterojunction promoting the electron-hole (e--h+) separation and hence favors redox processes. The center dot OH played a major role in the photodegradation, and the decomposition pathway of T-2 was proposed based on the results of UHPLC-Q-TOF-MS/MS data and density functional theory (DFT) calculations. This work provided a green approach for removing the refractory natural pollutants.
Keyword ：
Photocatalytic degradation Photocatalytic degradation p-n heterojunction p-n heterojunction T-2 toxin T-2 toxin Z-scheme Z-scheme
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| GB/T 7714 | Huang, Qingwen , Lou, Xiuping , Nie, Dongxia et al. Perspective Accelerated photodegradation of T-2 toxin over magnetic recyclable ZnO/ CaFe 2 O 4 nanocomposite with a p-n based Z-scheme heterojunction architecture [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 347 . |
| MLA | Huang, Qingwen et al. "Perspective Accelerated photodegradation of T-2 toxin over magnetic recyclable ZnO/ CaFe 2 O 4 nanocomposite with a p-n based Z-scheme heterojunction architecture" . | SEPARATION AND PURIFICATION TECHNOLOGY 347 (2024) . |
| APA | Huang, Qingwen , Lou, Xiuping , Nie, Dongxia , Zhao, Zhihui , Fan, Kai , Guo, Wenbo et al. Perspective Accelerated photodegradation of T-2 toxin over magnetic recyclable ZnO/ CaFe 2 O 4 nanocomposite with a p-n based Z-scheme heterojunction architecture . | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 347 . |
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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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Supramolecular systems consisting of covalent organic frameworks (COFs) and Ni complex are designed for robust photocatalytic reduction of CO2. Multiple heteroatom-hydrogen bonding between the COF and Ni complex is identified to play a decisive role in the photoexcited electron transfer across the liquid-solid interface. The diminution of steric groups on COF or metal complex can optimize catalytic performance, which is more attributable to the enhanced hydrogen-bond interaction rather than their intrinsic activity. The photosystem with relatively strong strength of hydrogen bonds exhibits remarkable photocatalytic CO2-to-CO conversion, far superior to photosystems with supported atomic Ni or metal complex alone in the absence of hydrogen-bond effect. Such heteroatom-hydrogen bonds bridging electron transport pathway confers supramolecular system with high photocatalytic performance, providing an avenue to rationally design efficient and steadily available photosystems.
Keyword ：
Covalent Organic Framework Covalent Organic Framework Electron Transport Electron Transport Heteroatom-Hydrogen Bond Heteroatom-Hydrogen Bond Photoreduction of CO2 Photoreduction of CO2
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| GB/T 7714 | He, Yajun , Zhao, Yun , Wang, Xiaofeng et al. Multiple Heteroatom-Hydrogen Bonds Bridging Electron Transport in Covalent Organic Framework-Based Supramolecular System for Photoreduction of CO2 [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 , 62 (31) . |
| MLA | He, Yajun et al. "Multiple Heteroatom-Hydrogen Bonds Bridging Electron Transport in Covalent Organic Framework-Based Supramolecular System for Photoreduction of CO2" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 62 . 31 (2023) . |
| APA | He, Yajun , Zhao, Yun , Wang, Xiaofeng , Liu, Zheyuan , Yu, Yan , Li, Liuyi . Multiple Heteroatom-Hydrogen Bonds Bridging Electron Transport in Covalent Organic Framework-Based Supramolecular System for Photoreduction of CO2 . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 , 62 (31) . |
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