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学者姓名：廖灿
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Abstract ：
Passivation of magnesium (Mg) anode in the chloride-free magnesium bis(trifluoromethanesulfonyl)imide (Mg(TFSI)(2)) electrolyte is a key challenge for Mg metal batteries. Tailoring solvation structure and solid electrolyte interphase (SEI) has been considered an effective strategy. Herein, a series of imidazole co-solvents with different branched-chain structures (methyl, ethyl, and propyl) are introduced into the Mg(TFSI)(2)-ether electrolyte to address the passivation issue. The ion-solvent interaction, interfacial adsorption effect, and SEI formation are comprehensively studied by theoretical calculations and experimental characterizations. Through molecular structure analysis, the long-chain 1-propylimidazole (PrIm) exhibits a strong coordination ability to Mg2+ and a favorable parallel adsorption configuration on the Mg surface. As a result, PrIm co-solvent can not only restructure the solvation sheath of Mg2+, but also act as a dynamic protective shield to repel a part of TFSI- and 1,2-dimethoxyethane (DME) away from the Mg surface. Benefiting from the synergistic regulation effect of interfacial chemistry and ion-solvent interactions, the chloride-free Mg(TFSI)(2)-DME + PrIm electrolyte ensures minimal interface passivation and achieves highly reversible Mg plating/stripping. This work provides a guiding strategy for solvation structure regulation and interface engineering for rechargeable Mg metal batteries.
Keyword ：
Adsorption Adsorption Imidazole co-solvent Imidazole co-solvent Magnesium metal battery Magnesium metal battery Mg(TFSI)(2) electrolyte Mg(TFSI)(2) electrolyte Solvation structure Solvation structure
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| GB/T 7714 | Yang, Aoqi , Gao, Xiang , Pei, Maojun et al. Synergistic Effects of Interfacial Chemistry and Ion-Solvent Interactions to Enable Reversible Magnesium Metal Anode in Chloride-Free Mg(TFSI)2 Electrolytes [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 . |
| MLA | Yang, Aoqi et al. "Synergistic Effects of Interfacial Chemistry and Ion-Solvent Interactions to Enable Reversible Magnesium Metal Anode in Chloride-Free Mg(TFSI)2 Electrolytes" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2025) . |
| APA | Yang, Aoqi , Gao, Xiang , Pei, Maojun , Zhou, Jiacong , Wang, Honggang , Liao, Can et al. Synergistic Effects of Interfacial Chemistry and Ion-Solvent Interactions to Enable Reversible Magnesium Metal Anode in Chloride-Free Mg(TFSI)2 Electrolytes . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 . |
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In this study, a novel concept of multipoint anionic bridge (MAB) is proposed and proved, which utilizes anions with different sites to connect with the asymmetric solvation structure (ASS). Compared to usual solvation structures, this study utilizes the multifunctional groups of difluoro(oxalate)borate anion (ODFB-), which can connect with Li+. By tailoring the concentration, the anion serves as a bridge between different solvated structures. The electrolyte is investigated through in situ techniques and simulations to draw correlations between different solvation structures and reaction pathways. The proposed design demonstrates remarkable high-temperature performance on both the anode and cathode sides, enabling stable cycling of LCO||graphite (0.5 Ah, 1.0 C) pouch cell for over 200 cycles at 80 degrees C and facilitating Li||MCMB and Li||LFP cells to deliver stable performance for 200 cycles at 100 degrees C. This work paves the way for the development of high-performance electrolyte systems by designing and using new multipoint anions to construct ASSs.
Keyword ：
asymmetric solvation structure asymmetric solvation structure high-concentration electrolyte high-concentration electrolyte high temperature high temperature lithium difluoro(oxalate)borate lithium difluoro(oxalate)borate lithium metal batteries lithium metal batteries
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| GB/T 7714 | Zheng, Tianle , Xu, Tonghui , Xiong, Jianwei et al. Multipoint Anionic Bridge: Asymmetric Solvation Structure Improves the Stability of Lithium-Ion Batteries [J]. | ADVANCED SCIENCE , 2024 , 11 (48) . |
| MLA | Zheng, Tianle et al. "Multipoint Anionic Bridge: Asymmetric Solvation Structure Improves the Stability of Lithium-Ion Batteries" . | ADVANCED SCIENCE 11 . 48 (2024) . |
| APA | Zheng, Tianle , Xu, Tonghui , Xiong, Jianwei , Xie, Weiping , Wu, Mengqi , Yu, Ying et al. Multipoint Anionic Bridge: Asymmetric Solvation Structure Improves the Stability of Lithium-Ion Batteries . | ADVANCED SCIENCE , 2024 , 11 (48) . |
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Graphite anode materials and carbonate electrolyte have been the top choices for commercial lithium-ion batteries (LIBS) for a long time. However, the uneven deposition and stripping of lithium cause irreversible damage to the graphite structure, and the low flash point and high flammability of the carbonate electrolyte pose a significant fire safety risk. Here, we proposed a multifunctional electrolyte additive diphenylphosphoryl azide (DPPA), which can construct a solid electrolyte interphase (SEI) with high ionic conductivity lithium nitride (Li3N) to ensure efficient transport of Li+. This not only protects the artificial graphite (AG) electrode but also inhibits lithium dendrites to achieve excellent electrochemical performance. Meanwhile, the LIBS with DPPA offers satisfactory flame retardancy performance. The AG//Li half cells with DPPA-0.5M can still maintain a specific capacity of about 350 mAh/g after 200 cycles at 0.2 C. Its cycle performance and rate performance were better than commercial electrolyte (EC/DMC). After cycling, the microstructure surface of the AG electrode was complete and flat, and the surface of the lithium metal electrode had fewer lithium dendrites. Importantly, we found that the pouch cell with DPPA-0.5M had low peak heat release rate. When exposed to external conditions of continuous heating, DPPA significantly improved the fire safety of the LIBS. The research of DPPA in lithium electrolyte is a step towards the development of safe and efficient lithium batteries.
Keyword ：
diphenylphosphoryl azide diphenylphosphoryl azide electrolyte additive electrolyte additive flame retardant flame retardant lithium nitride lithium nitride solid electrolyte interphase solid electrolyte interphase
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| GB/T 7714 | Li, Zhirui , Han, Longfei , Kan, Yongchun et al. Diphenylphosphoryl Azide as a Multifunctional Flame Retardant Electrolyte Additive for Lithium-Ion Batteries [J]. | BATTERIES-BASEL , 2024 , 10 (4) . |
| MLA | Li, Zhirui et al. "Diphenylphosphoryl Azide as a Multifunctional Flame Retardant Electrolyte Additive for Lithium-Ion Batteries" . | BATTERIES-BASEL 10 . 4 (2024) . |
| APA | Li, Zhirui , Han, Longfei , Kan, Yongchun , Liao, Can , Hu, Yuan . Diphenylphosphoryl Azide as a Multifunctional Flame Retardant Electrolyte Additive for Lithium-Ion Batteries . | BATTERIES-BASEL , 2024 , 10 (4) . |
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As the "safety switch" of lithium batteries, the separator controls the electrochemical performance and safety performance of lithium batteries. However, highly flammable and easy to induce lithium dendrite generation of commercial polyolefin pose a huge safety hazard for current commercial lithium-ion batteries. Therefore, developing a flame-retardant, lithium dendrite-inhibiting separator can achieve further leap in the lithium battery industry. A "sandwich" separator (SPS-B) is designed by integrating silk fibroin (SF), decabromodiphenyl ethane, and polyvinyl alcohol through electrospinning. SPS-B shows excellent flame-retardant properties through a free radical trapping mechanism. Moreover, the SPS-B demonstrated satisfactory capability of suppressing lithium dendrites by constructing Li3N-SEI with high ionic conductivity and high strength, and the secondary structure beta-sheets of SF can inhibit the "tip effect" of lithium dendrites, which enables efficient lithium plating/stripping in Li//Li and Li//Cu cells. In addition, the enhanced porosity, electrolyte affinity of SPS-B promotes excellent electrochemical performance with enhanced discharge capacity and reduced concentration polarization. Finally, fire risk of soft-pack batteries are evaluated by continuous external heating. Compared with commercial separator, soft-pack batteries with SPS-B show much lower heat release rate, peak temperature and flue gas release rate, further confirming the effectiveness of SPS-B in reducing fire risk. Overall, the SPS-B provides a satisfactory way to develop high-performance and superior safety lithium batteries.
Keyword ：
battery safety battery safety Li3N-SEI Li3N-SEI lithium batteries lithium batteries lithium dendrite lithium dendrite silk fibroin silk fibroin
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| GB/T 7714 | Li, Zhirui , Liao, Can , Han, Longfei et al. A flame-retardant, dendrite-inhibiting sandwich separator prepared by electrospinning for high-performance and safety lithium batteries [J]. | POLYMERS FOR ADVANCED TECHNOLOGIES , 2024 , 35 (4) . |
| MLA | Li, Zhirui et al. "A flame-retardant, dendrite-inhibiting sandwich separator prepared by electrospinning for high-performance and safety lithium batteries" . | POLYMERS FOR ADVANCED TECHNOLOGIES 35 . 4 (2024) . |
| APA | Li, Zhirui , Liao, Can , Han, Longfei , Cao, Yukun , Huang, Ju , Kan, Yongchun et al. A flame-retardant, dendrite-inhibiting sandwich separator prepared by electrospinning for high-performance and safety lithium batteries . | POLYMERS FOR ADVANCED TECHNOLOGIES , 2024 , 35 (4) . |
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Solid-state electrolytes (SSEs) with flame retardancy and good adaptability to lithium-metal anodes can have great potential in enabling high safety and high energy density lithium-metal batteries. In addition to optimize the composition/structure of current three main types of SSEs including inorganic SSEs, polymeric SSEs, and inorganic/polymer composite SSEs, massive efforts are under way to seek for new SSE formulations. Recently, metal-organic frameworks (MOFs), a type of crystalline inorganic-organic materials with the structural features of rich porous, ordered channels, tunable functionality, are emerging as a research hotspot in the field of SSEs, which have attracted tremendous efforts. Based on the latest investigations, in this paper, a systematic overview of the recent development in MOFs-based SSEs (MSSEs) for lithium-metal batteries is presented. Classification and compositions, development history, fabrication approaches, and recent progress of five main types of MSSEs are comprehensively reviewed, and the roles of MOFs in MSSEs including ionic conductors, ionic transport carriers, and added fillers are highlighted. Moreover, the main challenges are analyzed and the perspectives of MSSEs are also presented for their future research and development. This review not only contributes to the study of new systems of solid-state electrolytes, but also for further development of electrified transportation.
Keyword ：
High ionic conductivity High ionic conductivity Lithium -metal batteries Lithium -metal batteries Metal -organic frameworks Metal -organic frameworks Solid-state electrolytes Solid-state electrolytes
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| GB/T 7714 | Wang, Hongyao , Duan, Song , Zheng, Yun et al. Solid-state electrolytes based on metal-organic frameworks for enabling high-performance lithium-metal batteries: Fundamentals, progress, and perspectives [J]. | ETRANSPORTATION , 2024 , 20 . |
| MLA | Wang, Hongyao et al. "Solid-state electrolytes based on metal-organic frameworks for enabling high-performance lithium-metal batteries: Fundamentals, progress, and perspectives" . | ETRANSPORTATION 20 (2024) . |
| APA | Wang, Hongyao , Duan, Song , Zheng, Yun , Qian, Lanting , Liao, Can , Dong, Li et al. Solid-state electrolytes based on metal-organic frameworks for enabling high-performance lithium-metal batteries: Fundamentals, progress, and perspectives . | ETRANSPORTATION , 2024 , 20 . |
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The uncontrollable growth of lithium dendrites and the flammability of electrolytes are the direct impediments to the commercial application of high-energy-density lithium metal batteries (LMBs). Herein, this study presents a novel approach that combines microencapsulation and electrospinning technologies to develop a multifunctional composite separator (P@AS) for improving the electrochemical performance and safety performance of LMBs. The P@AS separator forms a dense charcoal layer through the condensed-phase flame retardant mechanism causing the internal separator to suffocate from lack of oxygen. Furthermore, it incorporates a triple strategy promoting the uniform flow of lithium ions, facilitating the formation of a highly ion-conducting solid electrolyte interface (SEI), and encouraging flattened lithium deposition with active SiO2 seed points, considerably suppressing lithium dendrites growth. The high Coulombic efficiency of 95.27% is achieved in Li-Cu cells with additive-free carbonate electrolyte. Additionally, stable cycling performance is also maintained with a capacity retention rate of 93.56% after 300 cycles in LFP//Li cells. Importantly, utilizing P@AS separator delays the ignition of pouch batteries under continuous external heating by 138 s, causing a remarkable reduction in peak heat release rate and total heat release by 23.85% and 27.61%, respectively, substantially improving the fire safety of LMBs. An advanced multifunctional separator with an extremely high electrolyte adsorption energy of surface silica microencapsulated ammonium polyphosphate particles anchored in an environmentally friendly polyvinyl alcohol fiber matrix is designed and constructed. The advanced separator demonstrates excellent electrochemical performances, lithium dendrite inhibition, and flame-retardant properties to drive the development of high-performance and high-safety lithium mental batteries. image
Keyword ：
dendrite-free dendrite-free fire safety fire safety flame retardant flame retardant lithium metal batteries lithium metal batteries multifunctional separator multifunctional separator
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| GB/T 7714 | Liao, Can , Li, Wanqing , Han, Longfei et al. Microcapsule Modification Strategy Empowering Separator Multifunctionality to Enhance Safety of Lithium-Metal Batteries [J]. | SMALL , 2024 , 20 (43) . |
| MLA | Liao, Can et al. "Microcapsule Modification Strategy Empowering Separator Multifunctionality to Enhance Safety of Lithium-Metal Batteries" . | SMALL 20 . 43 (2024) . |
| APA | Liao, Can , Li, Wanqing , Han, Longfei , Chu, Fukai , Zou, Bin , Qiu, Shuilai et al. Microcapsule Modification Strategy Empowering Separator Multifunctionality to Enhance Safety of Lithium-Metal Batteries . | SMALL , 2024 , 20 (43) . |
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Lithium metal batteries (LMBs) are considered as one type of the most promising next-generation energy storage devices with high-energy-density, and stabilizing the lithium metal anodes (LMAs) to overcome LMBs' safety concerns and performance degradation has attracted extensive attention. Introducing advanced polymer materials into the critical components of LMBs has proven to be an effective and promising approach for stabilizing LMAs toward practical application of LMBs. In addressing the lack of a timely review on the emerging progress of advanced polymer materials in LMBs for stabilizing LMAs, a comprehensive article summarizing the most recent developments of multiscale cellulose materials, including micron cellulose (MC) and nanocellulose (NC), in LMBs is reviewed. First, the basic structures of cellulose, characteristics comparison, and the development history of introducing cellulose into LMBs are presented. Furthermore, the roles of multiscale cellulose materials and functional mechanisms in various components of LMBs for stabilizing LMAs are summarized. A general conclusion and a perspective on the current limitations and future research directions of cellulose-based stable LMBs are proposed. The aim of this review is not only to summarize the recent progress of multiscale cellulose materials in stabilizing LMAs but also to lighten the pathways for realizing LMBs' practical application. This review aims to provide an in-depth summary of the roles of multiscale cellulose materials (i.e., micron cellulose (MC) and nanocellulose (NC)) in various components of lithium-metal batteries (LMBs), including separators, electrolytes, interfaces, and anode current collectors. Additionally, a general conclusion and a perspective on the current limitations and future research directions of cellulose-based stable LMBs are proposed. image
Keyword ：
advanced polymer materials advanced polymer materials lithium metal batteries lithium metal batteries micron cellulose micron cellulose nanocellulose nanocellulose stabilizing lithium metal anodes stabilizing lithium metal anodes
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| GB/T 7714 | Li, Zhenghao , Zheng, Yun , Liao, Can et al. Advanced Polymer Materials for Protecting Lithium Metal Anodes of Liquid-State and Solid-State Lithium Batteries [J]. | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (42) . |
| MLA | Li, Zhenghao et al. "Advanced Polymer Materials for Protecting Lithium Metal Anodes of Liquid-State and Solid-State Lithium Batteries" . | ADVANCED FUNCTIONAL MATERIALS 34 . 42 (2024) . |
| APA | Li, Zhenghao , Zheng, Yun , Liao, Can , Duan, Song , Liu, Xiang , Chen, Guohui et al. Advanced Polymer Materials for Protecting Lithium Metal Anodes of Liquid-State and Solid-State Lithium Batteries . | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (42) . |
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