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学者姓名：雷杰
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Abstract ：
Constructing the continuously-distributed and crystalline-NaF-rich solid electrolyte interface (CC-NaF-SEI) is expected to greatly promote the sodium storage performance of hard carbon (HC) anodes. However, such an impressive concept remains extremely intractable to achieve and lacks an efficiently cost-less strategy. Herein, the application of the commercially available LA133 binder is pioneered to engineer such a CC-NaF-SEI. Through comparative analysis of representative binders with distinct functional groups, reveals the critical role of binder chemistry on SEI regulation. Specifically, the LA133 binder demonstrates a dual-regulation mechanism for CC-NaF-SEI formation. The anion-coordination preferred ─CN bonds induce an anion-enriched interfacial solvation structure, and the ─CONH/─CN groups catalytically cleave P─F bond dissociation in PF6−, synergistically promoting anion decomposition kinetics to form crystalline NaF. Furthermore, robust hydrogen bonds between multiple polar groups in LA133 and HC surface create the spatially anion-confined microenvironments to guide orderly anion decomposition and facilitate continuous NaF growth into a mechanically integrated SEI. The optimized CC-NaF-SEI endows HC anodes with exceptional sodium storage performance: an ultrahigh initial Coulombic efficiency (95.9%), remarkable reversible capacity (356.6 mAh g−1), and stable cycling under extreme conditions (−20–60 °C). This work provides fundamental insights into binder-SEI correlations, establishing a novel paradigm for interfacial optimization in sodium-ion batteries. © 2025 Wiley-VCH GmbH.
Keyword ：
anion decomposition anion decomposition binder binder continuously-distributed continuously-distributed crystalline-NaF-rich SEI crystalline-NaF-rich SEI hard carbon hard carbon
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| GB/T 7714 | Liu, M. , Cai, J. , Zuo, Y. et al. Constructing Continuously-Distributed and Crystalline-NaF-Rich SEI on Hard Carbon Anode Through Binder Chemistry for High-Performance Sodium-Ion Batteries [J]. | Advanced Materials , 2025 . |
| MLA | Liu, M. et al. "Constructing Continuously-Distributed and Crystalline-NaF-Rich SEI on Hard Carbon Anode Through Binder Chemistry for High-Performance Sodium-Ion Batteries" . | Advanced Materials (2025) . |
| APA | Liu, M. , Cai, J. , Zuo, Y. , Luo, W. , Huang, Y. , Qiu, R. et al. Constructing Continuously-Distributed and Crystalline-NaF-Rich SEI on Hard Carbon Anode Through Binder Chemistry for High-Performance Sodium-Ion Batteries . | Advanced Materials , 2025 . |
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The intrinsic clustering behavior and kinetically sluggish conversion process of lithium polysulfides seriously limit the electrochemical reversibility of sulfur redox reactions in lithium-sulfur (Li-S) batteries. Here, we introduce molybdenum pentachloride (MoCl5 ) into the electrolyte which could coordinate with lithium polysulfides and inhibit their intrinsic clustering behavior, subsequently serving as an improved mediator with the bi-functional catalytic effect for Li2 S deposition and activation. Moreover, the coordination bonding and accelerated conversion reaction can also greatly suppress the dissolution and shuttling of polysulfides. Consequently, such polysulfide complexes enable the Li-S coin cell to exhibit good longterm cycling stability with a capacity decay of 0.078 % per cycle after 400 cycles at 2 C, and excellent rate performance with a discharge capacity of 589 mAh/g at 4 C. An area capacity of 3.94 mAh/cm2 is also achieved with a high sulfur loading of 4.5 mg/cm2 at 0.2 C. Even at -20 degrees C, the modified cell maintains standard discharge plateaus with low overpotential, delivering a high capacity of 741 mAh/g at 0.2 C after 80 cycles. The low-cost and convenient MoCl5 additive opens a new avenue for the effective regulation of polysulfides and significant enhancement in sulfur redox conversion. (c) 2025 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.
Keyword ：
Coordinating reaction Coordinating reaction Improved mediator Improved mediator Lithium-sulfur (Li-S) battery Lithium-sulfur (Li-S) battery Polysulfide clustering Polysulfide clustering Shuttle effect Shuttle effect
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| GB/T 7714 | Li, Qihou , Liu, Jiamin , Chu, Fulu et al. Coordinating lithium polysulfides to inhibit intrinsic clustering behavior and facilitate sulfur redox conversion in lithium-sulfur batteries [J]. | CHINESE CHEMICAL LETTERS , 2025 , 36 (5) . |
| MLA | Li, Qihou et al. "Coordinating lithium polysulfides to inhibit intrinsic clustering behavior and facilitate sulfur redox conversion in lithium-sulfur batteries" . | CHINESE CHEMICAL LETTERS 36 . 5 (2025) . |
| APA | Li, Qihou , Liu, Jiamin , Chu, Fulu , Zhou, Jinwei , Chen, Jieshuangyang , Guan, Zengqiang et al. Coordinating lithium polysulfides to inhibit intrinsic clustering behavior and facilitate sulfur redox conversion in lithium-sulfur batteries . | CHINESE CHEMICAL LETTERS , 2025 , 36 (5) . |
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The use of p-block metals to accelerate the sulfur reduction reaction (SRR) in lithium-sulfur (Li-S) batteries is emerging. However, the d-electrons inertia of p-block metal endows the weak adsorption and catalytic ability for SRR, limiting catalyst design. Herein, we fabricate an asymmetrically coordinated p-block indium trisulfide by coordination engineering with P doping and sulfur vacancies (P-In2S3-x) for SRR. The unique coordination engineering induces the rearrangement of electrons in the s/p/d hybrid orbital, causing that P-In2S3-x shifts electron states from low to high spin, generating more unpaired electrons. The obtained high-spin configuration achieves that electron transition to a higher energy level to activate d-electrons of p-block metals, which enables a novel dp coupling between d orbitals of In atoms and the p orbitals of S atoms in LiPSs, improving adsorption and catalytic ability of p-block metals for SRR. Consequently, cell with P-In2S3-x achieves excellent capacity retention, with a very low decay rate (0.036 % per cycle at 5 C over 1000 cycles) and high performance at 0 degrees C (760 mAh g- 1 at 1 C). This study offers a strategy for modulation d-electrons activity p-block metals by tailoring electron spin to boost catalytic efficiency in Li-S batteries.
Keyword ：
Catalytic mechanism Catalytic mechanism d -Electrons d -Electrons Electronic spin Electronic spin Lithium-sulfur batteries Lithium-sulfur batteries P -Block metals P -Block metals
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| GB/T 7714 | Huang, Zheng , Jiao, Xuechao , Lei, Jie et al. Activated d-electrons of p-block metals by reconfigured electron spin for kinetically boosting sulfur conversion of lithium-sulfur batteries [J]. | NANO ENERGY , 2025 , 139 . |
| MLA | Huang, Zheng et al. "Activated d-electrons of p-block metals by reconfigured electron spin for kinetically boosting sulfur conversion of lithium-sulfur batteries" . | NANO ENERGY 139 (2025) . |
| APA | Huang, Zheng , Jiao, Xuechao , Lei, Jie , Zuo, Yinze , Wang, Zheng , Lu, Linlong et al. Activated d-electrons of p-block metals by reconfigured electron spin for kinetically boosting sulfur conversion of lithium-sulfur batteries . | NANO ENERGY , 2025 , 139 . |
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Modulating the electron delocalization of catalysts can improve the activation and conversion capabilities of lithium polysulfides (LiPSs) in lithium-sulfur batteries, while the precise mechanism underlying this enhancement remains unclear. Herein, a p-block In single-atom catalysts (In-N4) is constructed with moderate electron delocalization via axial coordination engineering of gallium nitride (GaN), which exhibits the best adsorption and electrocatalytic activity toward LiPSs. In situ characterization analysis combined with advanced theoretical calculations demonstrate that the axial In-N-Ga coordination induces the electron transfer from In sites toward the N sites of GaN and the unconventional sp3d2 hybridization interactions of In sites. This further helps to optimize adsorption configuration through the orbital hybridization between sp3d2 hybrid orbital of In sites and p orbital of S atoms in LiPSs, namely the sp3d2 - p orbital hybridization, which can weaken S-S covalent bonds of LiPSs and significantly accelerate the sulfur reduction reaction. Accordingly, the capacity decay of lithium-sulfur battery with In-SA/GaN catalyst is only 0.040% per cycle over 800 cycles at 5 C. The stacked pouch cell delivers a reversible capacity of 600 mAh after 100 cycles. This work elaborates on the activity origin of p-block metal catalysts and provides a new perspective on designing advanced catalysts for other catalytic systems.
Keyword ：
electron delocalization electron delocalization orbital hybridization orbital hybridization p-block metal p-block metal single-atom catalyst single-atom catalyst sulfur reduction reaction sulfur reduction reaction
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| GB/T 7714 | Jiao, Xuechao , Lei, Jie , Huang, Zheng et al. Axial Coordination Regulating Electronic Delocalization of p-Block In-N4 Sites to Accelerate Sulfur Reduction Reaction [J]. | ADVANCED FUNCTIONAL MATERIALS , 2025 . |
| MLA | Jiao, Xuechao et al. "Axial Coordination Regulating Electronic Delocalization of p-Block In-N4 Sites to Accelerate Sulfur Reduction Reaction" . | ADVANCED FUNCTIONAL MATERIALS (2025) . |
| APA | Jiao, Xuechao , Lei, Jie , Huang, Zheng , Zuo, Yinze , Zhuang, Zewen , Luo, Yiyuan et al. Axial Coordination Regulating Electronic Delocalization of p-Block In-N4 Sites to Accelerate Sulfur Reduction Reaction . | ADVANCED FUNCTIONAL MATERIALS , 2025 . |
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The application of zinc-metal-based batteries is hindered by the low thermodynamic stability of zinc anodes and the sluggish desolvation kinetics of the interfacial [Zn(H2O)6]2+ complex, which can induce serious side reactions and exacerbate dendrite formation. Herein, an innovative catalytic desolvation mechanism is proposed to manipulate the interfacial solvation structure by engineering a pi-electron-rich (C 00000000 00000000 00000000 00000000 11111111 00000000 11111111 00000000 00000000 00000000 O/CN configurations) covalent organic polymer (COP) layer as an interfacial catalyst. It was revealed that the pi-electrons can trigger dissociation of the [Zn(H2O)6]2+ complex through an ortho-synergistic reaction process, which includes a nucleophilic reaction between electron-accepting C atoms at CO/CN sites and H2O molecules and an electrophilic reaction between electron-donating sites near O and N heteroatoms and Zn2+. In situ characterization analysis combined with advanced theoretical calculations confirmed that such a catalytic desolvation process can dynamically induce contact ion pairs and aggregate dominated interfacial solvation structures, boosting Zn2+ diffusion and deposition kinetics. Consequently, suppressed side reactions and homogenous (002)-crystal-preferred Zn2+ deposition can be simultaneously achieved. Therefore, an excellent cycling lifespan of 2500 h was obtained for the symmetric Zn cell and an ultra-stable cycling lifespan of 28 000 cycles for full cells. We believe that this catalytic desolvation strategy will pave a new avenue in the interfacial design of Zn anodes.
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| GB/T 7714 | Zuo, Yinze , Wang, Zheng , Liu, Mingquan et al. Enhanced interfacial Zn2+ desolvation kinetics by a π-electron-rich Janus catalyst for robust Zn-metal batteries [J]. | ENERGY & ENVIRONMENTAL SCIENCE , 2025 , 18 (15) : 7490-7503 . |
| MLA | Zuo, Yinze et al. "Enhanced interfacial Zn2+ desolvation kinetics by a π-electron-rich Janus catalyst for robust Zn-metal batteries" . | ENERGY & ENVIRONMENTAL SCIENCE 18 . 15 (2025) : 7490-7503 . |
| APA | Zuo, Yinze , Wang, Zheng , Liu, Mingquan , Lu, Linlong , Jiang, Yidong , Lei, Jie et al. Enhanced interfacial Zn2+ desolvation kinetics by a π-electron-rich Janus catalyst for robust Zn-metal batteries . | ENERGY & ENVIRONMENTAL SCIENCE , 2025 , 18 (15) , 7490-7503 . |
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Alloy catalyst is considered to be an important strategy to solve the shuttle effect and sluggish kinetics of lithium-sulfur batteries (LSBs). However, the effect of the electronic structure of the alloy catalyst on the sulfur conversion process has not been effectively analyzed. In this paper, based on alloying strategy, the electronic structure of such a FeCoNi catalyst is regulated and optimized, and the sulfur adsorption configuration and catalytic conversion process are defined. The in situ Raman spectroscopy and the density functional theory (DFT) are employed to deeply understand the catalytic mechanism of such a sulfur conversion. A cell with FeCoNi modified separator delivers an ultra-low capacity attenuation of 0.056% per cycle over 1000 cycles at 3 C. The outstanding anti-self-discharge performance of 8.1% over 7 days is also achieved. Furthermore, the obtained cell with a high sulfur loading of 9.7 mg cm-2 and lean electrolyte of 5.6 mu L mgs-1 exhibits 81% capacity retention after 100 cycles, providing a research prospect for the practical application of lithium-sulfur batteries. Based on the intrinsic electronic structure of the alloy catalyst, the surface electronic reconstruction process of the alloy catalyst is analyzed, and its catalytic mechanism in the sulfur conversion process is elucidated, which provides a new idea for the development of alloy catalyst and lithium sulfur battery. image
Keyword ：
chemisorption chemisorption electrocatalyst electrocatalyst electrochemical kinetics electrochemical kinetics FeCoNi FeCoNi lithium-sulfur batteries lithium-sulfur batteries
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| GB/T 7714 | Zuo, Yinze , Jiao, Xuechao , Huang, Zheng et al. Surface Electron Reconstruction of Catalyst Through Alloying Strategy for Accelerating Sulfur Conversion in Lithium-Sulfur Batteries [J]. | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (44) . |
| MLA | Zuo, Yinze et al. "Surface Electron Reconstruction of Catalyst Through Alloying Strategy for Accelerating Sulfur Conversion in Lithium-Sulfur Batteries" . | ADVANCED FUNCTIONAL MATERIALS 34 . 44 (2024) . |
| APA | Zuo, Yinze , Jiao, Xuechao , Huang, Zheng , Lei, Jie , Liu, Mingquan , Dong, Li et al. Surface Electron Reconstruction of Catalyst Through Alloying Strategy for Accelerating Sulfur Conversion in Lithium-Sulfur Batteries . | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (44) . |
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Wide operation temperature is the crucial objective for an energy storage system that can be applied under harsh environmental conditions. For lithium-sulfur batteries, the "shuttle effect" of polysulfide intermediates will aggravate with the temperature increasing, while the reaction kinetics decreases sharply as the temperature decreasing. In particular, sulfur reaction mechanism at low temperatures seems to be quite different from that at room temperature. Here, through in situ Raman and electrochemical impedance spectroscopy studies, the newly emerged platform at cryogenic temperature corresponds to the reduction process of Li2S8 to Li2S4, which will be another rate-determining step of sulfur conversion reaction, in addition to the solid-phase conversion process of Li2S4 to Li2S2/Li2S at low temperatures. Porous bismuth vanadate (BiVO4) spheres are designed as sulfur host material, which achieve the rapid snap-transfer-catalytic process by shortening lithium-ion transport pathway and accelerating the targeted rate-determining steps. Such promoting effect greatly inhibits severe "shuttle effect" at high temperatures and simultaneously improves sulfur conversion efficiency in the cryogenic environment. The cell with the porous BiVO4 spheres as the host exhibits excellent rate capability and cycle performance under wide working temperatures.
Keyword ：
bismuth vanadate bismuth vanadate lithium-sulfur batteries lithium-sulfur batteries rate-determinate step rate-determinate step reaction mechanism reaction mechanism wide temperature range wide temperature range
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| GB/T 7714 | Deng, Ding-Rong , Xiong, Hai-Ji , Luo, Yu-Lin et al. Accelerating the Rate-Determining Steps of Sulfur Conversion Reaction for Lithium-Sulfur Batteries Working at an Ultrawide Temperature Range [J]. | ADVANCED MATERIALS , 2024 , 36 (39) . |
| MLA | Deng, Ding-Rong et al. "Accelerating the Rate-Determining Steps of Sulfur Conversion Reaction for Lithium-Sulfur Batteries Working at an Ultrawide Temperature Range" . | ADVANCED MATERIALS 36 . 39 (2024) . |
| APA | Deng, Ding-Rong , Xiong, Hai-Ji , Luo, Yu-Lin , Yu, Kai-Min , Weng, Jian-Chun , Li, Gui-Fang et al. Accelerating the Rate-Determining Steps of Sulfur Conversion Reaction for Lithium-Sulfur Batteries Working at an Ultrawide Temperature Range . | ADVANCED MATERIALS , 2024 , 36 (39) . |
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The development of electrocatalysts with high catalytic activity is conducive to enhancing polysulfides adsorption and reducing activation energy of polysulfides conversion, which can effectively reduce polysulfide shuttling in Li-S batteries. Herein, a novel catalyst NiCo-MoOx/rGO (rGO = reduced graphene oxides) with ultra-nanometer scale and high dispersity is derived from the Anderson-type polyoxometalate precursors, which are electrostatically assembled on the multilayer rGO. The catalyst material possesses dual active sites, in which Ni-doped MoOx exhibits strong polysulfide anchoring ability, while Co-doped MoOx facilitates the polysulfides conversion reaction kinetics, thus breaking the Sabatier effect in the conventional electrocatalytic process. In addition, the prepared NiCo-MoOx/rGO modified PP separator (NiCo-MoOx/rGO@PP) can serve as a physical barrier to further inhibit the polysulfide shuttling effect and realize the rapid Li+ migration. The results demonstrate that Li-S coin cell with NiCo-MoOx/rGO@PP separator shows excellent cycling performance with the discharge capacity of 680 mAhg-1 after 600 cycles at 1 C and the capacity fading of 0.064% per cycle. The rate performance is also impressive with the remained capacity of 640 mAhg-1 after 200 cycles even at 4 C. When the sulfur loading is 4.0 mgcm-2 and electrolyte volume/sulfur mass ratio (E/S) ratio is 6.0 mu Lmg-1, a specific capacity of 830 mAhg-1 is achieved after 200 cycles with a capacity decay of 0.049% per cycle. More importantly, the cell with NiCo-MoOx/rGO@PP separator exhibits cycling performance under wide operating temperature with the reversible capacities of 518, 715, and 915 mAhg-1 after 100 cycles at -20, 0, and 60 degrees C, respectively. This study provides a new design approach of highly efficient catalysts for sulfur conversion reaction in Li-S batteries.
Keyword ：
adsorption and catalysis dual-sites adsorption and catalysis dual-sites doped molybdenum oxide doped molybdenum oxide lithium-sulfur batteries lithium-sulfur batteries separator modification separator modification wide temperature wide temperature
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| GB/T 7714 | Chen, Jieshuangyang , Lei, Jie , Zhou, Jinwei et al. Polysulfides adsorption and catalysis dual-sites on metal-doped molybdenum oxide nanoclusters for Li-S batteries with wide operating temperature [J]. | NANO RESEARCH , 2024 , 17 (11) : 9651-9661 . |
| MLA | Chen, Jieshuangyang et al. "Polysulfides adsorption and catalysis dual-sites on metal-doped molybdenum oxide nanoclusters for Li-S batteries with wide operating temperature" . | NANO RESEARCH 17 . 11 (2024) : 9651-9661 . |
| APA | Chen, Jieshuangyang , Lei, Jie , Zhou, Jinwei , Chen, Xuanfeng , Deng, Rongyu , Qian, Mingzhi et al. Polysulfides adsorption and catalysis dual-sites on metal-doped molybdenum oxide nanoclusters for Li-S batteries with wide operating temperature . | NANO RESEARCH , 2024 , 17 (11) , 9651-9661 . |
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