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A dual-regulation strategy of B/N codoped CNT-encapsulated Ni nanoparticles as a catalytic host and separator coating promises high-performance Li-S batteries

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Science China(Technological Sciences) 2022年第7期65卷 1567-1577页

作者： XIONG DongGen XU Ling XU Jian ZHANG XiangXiang LI Jia XU YuQing ZHANG Ze YU Ji YANG ZhenYu Key Laboratory of Jiangxi Province for Environment and Energy Catalysis College of ChemistryNanchang UniversityNanchang 330031China Department of Physics Nanchang UniversityNanchang 330031China

A dual-regulation strategy of adopting B/N codoped carbon nanotube-encapsulated nickel nanoparticles(Ni@BNCNT) as a sulfur host and separator coating is proposed for high-performance Li-S batteries. On the cathode side, the 3D conductive network structure of Ni@BNCNT is favorable for high sulfur utilization, and the collaboration between polar metal Ni nanoparticles(NPs) and doped B/N elements facilitates the chemical adsorption of Li polysulfides(Li PSs). In addition, these metal Ni NPs exhibit a satisfactory catalytic effect on the polysulfide conversion. Moreover, using the Ni@BNCNT interlayer can further capture the soluble Li PSs, make them convert quickly, and prevent them from diffusing toward the anode side. The Li-S batteries simultaneously equipped with a S/Ni@BNCNT cathode and Ni@BNCNT interlayer show high reversible capacity and good cycle stability. Additionally, even at a sulfur loading of 3.5 mg cm;and an electrolyte/sulfur ratio of 3 μL mg;, excellent battery performance can be achieved. We believe that this work offers a new strategy based on combining a catalytic host and separator coating to construct high-efficiency Li-S batteries.

关键词： Li-S batteries CNT-encapsulated Ni catalysts dual-regulation strategy catalytic host separator coating

catalytic hosts with strong adsorption strength for long shelf-life lithium-sulfur batteries under lean electrolyte

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Nano Research 2023年第1期16卷 427-438页

作者： Siyuan Zhao Huayu Pei Quan Yang Kangli Liu Yuanyuan Huang Zhuo Wang Guosheng Shao Jinping Liu Junling Guo State Center for International Cooperation on Designer Low-carbon&Environmental Materials School of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001China Zhengzhou Materials Genome Institute Xingyang 450100China School of Chemistry Chemical Engineering and Life ScienceState Key Laboratory of Advanced Technology for Materials Synthesis and ProcessingWuhan University of TechnologyWuhan 430070China

Low electrolyte/sulfur ratio(E/S)is an important factor in increasing the energy density of lithium-sulfur batteries(LSBs).Recently,the E/S has been widely lowered using catalytic hosts that can suppress“shuttle effect”during cycling by relying on a limited adsorption ***,the shelf-lives of these cathodes have not yet received ***,we show that the selfdischarge of sulfur cathodes based on frequently-used catalytic hosts is serious under low E/S because the“shuttle effect”during storage process caused by polysulfides(PSs)disproportionation cannot be suppressed using a limited adsorption *** further prove that the adsorption strength toward PSs,which is unfortunately weak in commonly-used catalytic hosts,is critical for effectively hindering the disproportionation of the ***,to verify this conclusion,we prepare a sulfur-doped titanium nitride(S-TiN)catalytic array *** the adsorption strength and catalytic activity of TiN can be improved by S doping simultaneously,the constructed S/S-TiN cathodes under a low E/S(6.5μL·mg−1)exhibit better shelf-life and cycle-stability than those of S/TiN *** work suggests that enhancing the adsorption strength of catalytic hosts,while maintaining their function to reduce E/S,is crucial for practical LSBs.

关键词： lithium-sulfur battery low electrolyte/sulfur ratio(E/S) self-discharge catalytic host adsorption strength

High-Entropy Alloys to Activate the Sulfur Cathode for Lithium-Sulfur Batteries

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Energy & Environmental Materials 2023年第3期6卷 40-49页

作者： Zhenyu Wang Hailun Ge Sheng Liu Guoran Li Xueping Gao Institute of New Energy Material Chemistry School of Materials Science and EngineeringRenewable Energy Conversion and Storage CenterNankai UniversityTianjin 300350China

Sulfur element possesses an ultrahigh theoretical specific capacity,while the utilization of sulfur in the whole cathode is lower obviously owing to the sluggish kinetics of sulfur and discharged products,limiting the enhancement on energy density of lithium-sulfur ***,for the first time,Fe_(0.24)Co_(0.26)Ni_(0.10)Cu_(0.15)Mn_(0.25)high-entropy alloy is introduced as the core catalytic host to activate the electrochemical performance of the sulfur cathode for lithium-sulfur *** is manifested that Fe_(0.24)Co_(0.26)Ni_(0.10)Cu_(0.15)Mn_(0.25)high-entropy alloy nanocrystallites distributed on nitrogen-doped carbon exhibit high electrocatalytic activity toward the conversion of solid sulfur to solid discharged products across soluble intermediate lithium *** particular,benefiting from the accelerated kinetics by high-entropy alloy nanocrystallites and synergistic adsorption by nitrogen-doped carbon,the cathode exhibits high reversible capacity of 1079.5 mAh g_(-cathode)^(-1)(high utilization of 89.4%)with the whole cathode as active material,instead of sulfur ***,under both lean electrolyte(3μmg^(-1))and ultrahigh sulfur loading(27.0 mg cm^(-2))condition,the high discharge capacity of 868.2 mAh g_(-cathode)^(-1)can be still achieved for the sulfur *** strategy opens up a new path to explore catalytic host materials for enhancing the utilization of sulfur in the whole cathode for lithium-sulfur batteries.

关键词： catalytic host electrochemical performance high-entropy alloy lithium–sulfur batteries sulfur cathode

High-Entropy Spinel Oxide Nanofibers as catalytic Sulfur hosts Promise the High Gravimetric and Volumetric Capacities for Lithium–Sulfur Batteries

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Energy & Environmental Materials 2022年第2期5卷 645-654页

作者： Liyuan Tian Ze Zhang Sheng Liu Guoran Li Xueping Gao Institute of New Energy Material Chemistry School of Materials Science and EngineeringRenewable Energy Conversion and Storage CenterNankai UniversityTianjin 300350China

The exploration of new catalytic hosts is highly important to tackle the sluggish electrochemical kinetics of sulfur redox for achieving high energy density of lithium–sulfur ***,for the first time,we present high-entropy oxide(HEO,(Mg_(0.2)Mn_(0.2)Ni_(0.2)Co_(0.2)Zn_(0.2))Fe_(2)O_(4))nanofibers as catalytic host of *** HEO nanofibers show a synergistic effect among multiple metal cations in spinel structure that enables strong chemical confinement of soluble polysulfides and fast kinetics for polysulfide ***,the S/HEO composite displays the high gravimetric capacity of 1368.7 mAh g^(−1) at 0.1 C rate,excellent rate capability with the discharge capacity of 632.1 mAh g^(−1) at 5 C rate,and desirable cycle ***,the S/HEO composite shows desirable sulfur utilization and good cycle stability under a harsh operating condition of high sulfur loading(4.6 mg cm^(−2))or low electrolyte/sulfur ratio(5μL mg^(−1)).More impressively,the high volumetric capacity of 2627.9 mAh cm^(−3) is achieved simultaneously for the S/HEO composite due to the high tap density of 1.92 g cm^(−3),nearly 2.5 times of the conventional sulfur/carbon ***,based on high-entropy oxide materials,this work affords a fresh concept of elevating the gravimetric/volumetric capacities of sulfur cathodes for lithium–sulfur batteries.

关键词： catalytic host high-entropy oxide lithium-sulfur battery polysulfide conversion spinel oxide nanofibers