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学者姓名：雷杰
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Abstract ：
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 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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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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