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Conducting polymer-functionalized mesoporous metal-organic frameworks for high-performance Li-S battery

Nano Research 2023年第4期16卷 4867-4873页

作者： Xiao-Fei liu Ya-Rui Wang Hong Chen Bo li shuang-Quan Zang Henan Key Laboratory of Crystalline Molecular Functional Materials Henan International Joint Laboratory of Tumor Theranostical Cluster MaterialsGreen Catalysis Center and College of ChemistryZhengzhou UniversityZhengzhou 450001China Collaborative Innovation Center of Water security for Water source Region of Mid-line of south-to-North Diversion Project of Henan Province College of Chemistry and Pharmacy EngineeringNanyang Normal UniversityNanyang 473061China

It was known that mesoporous metal-organic frameworks(MOFs)with hierarchical pores and unsaturated metal sites can effectively inhibit the shuttle effect of lithium polysulfides in lithium-sulfur battery,however,the unsatisfactory structural stability and electrical conductivity limit the application of mesoporous MOFs(MMOFs)in li-s batteries.Aiming at sensible solutions,the conductive polyaniline(PANI)was incorporated into the MMOF to enhance the discharge capacity and the cycling stability of proposed li-s batteries,as the stability and the conductivity of the MMOF cathode was improved simultaneously.The activated MMOF-PANI provides physical and chemical adsorption of polysulfides against their shuttle effect.Moreover,the introduction of PANI into the channels of MMOF effectively improves the conductivity of MMOF,thus improving the electrochemical performance of the MMOF-PANI-based batteries.Benefiting from these synergetic effects,the s@MMOF-PANI cathode delivers improved electrochemical performance including excellent rate performance and cycling stability.The battery shows an initial capacity of 777.7 mAh·g^(−1)at 2.0 C and a low decay rate of 0.06%per cycle in 1,000 cycles and approximately a repeatable rate performance.

关键词： metal-organic framework conductivity mesoporous shuttle effect Li-S battery

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Isolated diatomic Zn-Co metal–nitrogen/oxygen sites with synergistic effect on fast catalytic kinetics of sulfur species in Li-S battery

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Journal of Energy Chemistry 2023年第4期79卷 505-514页

作者： Chun-Lei song Qiao-Tong He Zhongyi Zeng Jing-Yan Chen Tian Wen Yu-Xiao Huang liu-Chun Zhuang Wei Yi Yue-Peng Cai Xu-Jia Hong school of Chemistry South China Normal UniversityGuangzhou 510006GuangdongChina Guangzhou Municipal and Guangdong Provincial Key Laboratory of Molecular Target&Clinical Pharmacology the NMPA and State Key Laboratory of Respiratory DiseaseSchool of Pharmaceutical Sciences&the Fifth Affiliated Hospital Guangzhou Medical UniversityGuangzhou 511436GuangdongChina

lithium-sulfur batteries are severely restricted by low electronic conductivity of sulfur and li_(2)s,shuttle effect,and slow conversion reaction of lithium polysulfides(liPss).Herein,we report a facile and highyield strategy for synthesizing dual-core single-atom catalyst(ZnCoN_(4)O_(2)/CN)with atomically dispersed nitrogen/oxygen-coordinated Zn-Co sites on carbon nanosheets.Based on density functional theory(DFT)calculations and liPss conversion catalytic ability,ZnCoN_(4)O_(2)/CN provides dual-atom sites of Zn and Co,which could facilitate li^(+)transport and li_(2)s diffusion,and catalyze liPss conversion more effectively than homonuclear bimetallic single-atom catalysts or their simple mixture and previously reported singleatom catalysts.li-s cell with ZnCoN_(4)O_(2)/CN modified separator showed excellent rate performance(789.4 mA h g^(-1)at 5 C)and stable long cycle performance(0.05%capacity decay rate at 6C with 1000cycles,outperforming currently reported single atomic catalysts for liPss conversion.This work highlights the important role of metal active centers and provides a strategy for producing multifunctional dual-core single atom catalysts for high-performance li-s cells.

关键词： Dual-core single-atom catalysts lithium polysulfides Fast catalytic kinetics li_(2)s diffusion Li-S battery

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Three-in-one LaNiO_(3) functionalized separator boosting electrochemical stability and redox kinetics for high-performance Li-S battery

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Journal of Energy Chemistry 2023年第7期82卷 581-591,I0013页

作者： Weiyu Wang Mingxiu Hou Fangqian Han Di Yu Jie liu Qian Zhang Fengli Yu Lei Wang Maoshuai He state Key Laboratory Base of Eco-chemical Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina College of Chemistry and Molecular Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina College of Chemical Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina Weifang Key Laboratory of Green Processing of separator for Chemical Power sources School of Chemistry and EngineeringWeifang Vocational CollegeWeifang 261108ShandongChina shandong Engineering Research Center for Marine Environment Corrosion and safety Protection College of Environment and Safety EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina

The lithium-sulfur(li-s)battery,as one of the energy storage devices,has been in the limelight due to its high theoretical energy density.However,the poor redox kinetics and the"shuttle effect"of polysulfides severely restrict the use of li-s batteries in practical applications.Herein,a novel bimetallic LaNiO_(3) functional material with high electrical conductivity and catalytic property is prepared to act as a high-efficiency polysulfide shuttling stopper.The three LaNiO_(3) samples with different physical/chemical characteristics are obtained by controlling the calcination temperature.In conjunction with the high electrical conductivity and excellent catalytic properties of the as-prepared materials,the appropriate chemisorption toward polysulfides offers great potential to enhance electrochemical stability for highperformance li-s batteries.Particularly,the li-s cell with the separator modified by such functional material gives a specific capacity of 658 mA h g^(-1) after 500 cycles at a high current density of 2 C.Even with high sulfur loading of 6.05 mg cm^(-2),the Li-S battery still exhibits an areal specific capacity of 2.81 m A h cm^(-2)after 150 cycles.This work paves a new avenue for the rational design of materials for separator modification in high-performance li-s batteries.

关键词： Li-S battery Functional separator Catalytic property Electrochemical stability Redox kinetics

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Tuning of interactions between cathode and lithium polysulfide in Li-S battery by rational halogenation

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Journal of Energy Chemistry 2020年第10期29卷 147-152页

作者： samson O.Olanrele Zan lian Chaowei si shuo Chen Bo li shenyang National Laboratory for Materials science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016LiaoningChina school of Materials science and Engineering University of Science and Technology of ChinaShenyang 110016LiaoningChina Key Laboratory of Functional Inorganic Material Chemistry(Ministry of Education of China) School of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080HeilongjiangChina Chemical sciences Department Mountain Top UniversityOgun StateNigeria

li-s batteries have aroused intense interests as one of the most promising high-energy-density storage technology.However,the complex undesired shuttle effect induced by dissolution and diffusion of lithium polysulfide intermediates remains the major setback of this technology.Chemical modification of carbon cathode through heteroatom-doping is widely accepted as an effective method to inhibit the shuttle effect in Li-S battery cathode.Herein,using first principle calculations,we systematically examined the interaction between halogenated graphene and lithium polysulfide species.It is found that the halogen dopants(F,Cl,Br,I)significantly modify the local electronic structure of adsorption site and further induce a polarization to trap the polysulfides.Interestingly,a concave curve is observed from F to I for lithium polysulfide adsorption rather than a linear relation.The exceptions demonstrated from iodine dopant is carefully analyzed and attributed to its unique charge state.Moreover,boron as second dopant further strengthens the interaction between halogenated graphene and polysulfide molecule.Based on halogenation strategy,lithium polysulfide/cathode interactions are tuned in a wide range,which can also be of great importance to accelerate redox reaction in Li-S battery.Overall,an effective method by halogenation is verified to regulate the adsorption of lithium polysulfide and also enhance the reaction kinetics of the Li-S battery system.

关键词： Li-S battery Halogenation shuttle effect Co-doping

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Engineering strategies for suppressing the shuttle Effect in lithium–sulfur Batteries

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Nano-Micro Letters 2024年第1期16卷 187-221页

作者： Jiayi li li Gao Fengying Pan Cheng Gong limeng sun Hong Gao Jinqiang Zhang Yufei Zhao Guoxiu Wang Hao liu Joint International Laboratory On Environmental and Energy Frontier Materials School of Environmental and Chemical EngineeringShanghai UniversityShanghaiPeople’s Republic of China Centre for Clean Energy Technology University of Technology SydneyBroadwaySydneyNSW 2007Australia

lithium–sulfur(li–s)batteries are supposed to be one of the most potential next-generation batteries owing to their high theoretical capacity and low cost.Nevertheless,the shuttle effect of firm multi-step two-electron reaction between sulfur and lithium in liquid electrolyte makes the capacity much smaller than the theoretical value.Many methods were proposed for inhibiting the shuttle effect of polysulfide,improving corresponding redox kinetics and enhancing the integral performance of li–s batteries.Here,we will comprehensively and systematically summarize the strategies for inhibiting the shuttle effect from all components of li–s batteries.First,the electrochemical principles/mechanism and origin of the shuttle effect are described in detail.Moreover,the efficient strategies,including boosting the sulfur conversion rate of sulfur,confining sulfur or lithium polysulfides(LPs)within cathode host,confining LPs in the shield layer,and preventing LPs from contacting the anode,will be discussed to suppress the shuttle effect.Then,recent advances in inhibition of shuttle effect in cathode,electrolyte,separator,and anode with the aforementioned strategies have been summarized to direct the further design of efficient materials for li–s batteries.Finally,we present prospects for inhibition of the LPs shuttle and potential development directions in li–s batteries.

关键词： shuttle effect Designed strategies Li-S battery lithium polysulfides

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Unfolding the structure-property relationships of li_(2)s anchoring on two-dimensional materials with high-throughput calculations and machine learning

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Journal of Energy Chemistry 2023年第7期82卷 31-39,I0002页

作者： Lujie Jin Hongshuai Wang Hao Zhao Yujin Ji Youyong li Institute of Functional Nano&soft Materials(FUNsOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123China Macao Institute of Materials science and Engineering Macao University of Science and TechnologyTaipa 999078MacaoChina

lithium-sulfur(li-s)batteries are notable for their high theoretical energy density,but the‘shuttle effect’and the limited conversion kinetics of li-s species can downgrade their actual performance.An essential strategy is to design anchoring materials(AMs)to appropriately adsorb li-s species.Herein,we propose a new three-procedure protocol,named InfoAd(Informative Adsorption)to evaluate the anchoring of li_(2)s on two-dimensional(2D)materials and disclose the underlying importance of material features by combining high-throughput calculation workflow and machine learning(ML).In this paradigm,we calculate the anchoring of li_(2)s on 12552D A_(x)B_(y)(B in the VIA/VIIA group)materials and pick out 44(un)reported nontoxic 2D binary A_(x)B_(y)AMs,in which the importance of the geometric features on the anchoring effect is revealed by ML for the first time.We develop a new Infograph model for crystals to accurately predict whether a material has a moderate binding with li_(2)s and extend it to all 2D materials.Our InfoAd protocol elucidates the underlying structure-property relationship of li_(2)s adsorption on 2D materials and provides a general research framework of adsorption-related materials for catalysis and energy/substance storage.

关键词： Adsorption Anchoring material Li-S battery Extreme gradient boosting Graph neural network Material geometry semi-supervised learning

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Low-temperature li-s batteries enabled by all amorphous con version process of organosulfur cathode

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Journal of Energy Chemistry 2022年第1期31卷 496-502,I0013页

作者： Zhenkang Wang Xiaowei shen sijie li Yuxuan Wu Tingzhou Yang Jie liu Tao Qian Chenglin Yan College of Energy Key Laboratory of Advanced Carb on Materials and Wearable Energy Technologies of Jiangsu ProvinceSoochow UniversitySuzhou 215006JiangsuChina College of Chemistry and Chemical Engineering.Nantong University Seyuan 9Nantong 226000JiangsuChina

The high degree of crystallinity of discharging in termediates of li-s batteries(li_(2)s_(2)/li_(2)s)causes a severe capacity attenuation at low temperatures.Herein,a sulfur-rich polymer is fabricated,which enables all the discharging in termediates to exist in an amorphous state without long-range order,promoti ng the substantial conversion of discharging intermediates and enhancing li-s batteries'performance at low temperatures greatly.This cathode material exhibits excellent performance both at room and low temperatures.Even under an extremely low temperature(-40℃),the discharge capacity can remain 67% of that at room temperature.Besides,in-situ UV/Vis spectroscopy and density functional theory calculations reveal that this organosulfur cathode undergoes a new mechanism during discharge.li_(2)s_(6) and li_(2)s_(3) are the primary discharging intermediates that are quite different from conventional li-s batteries.These results provide a new directi on for a broader range of applications of li-s batteries.

关键词： Low temperature Organosulfur polymers Li-S battery Crystallinity

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Atomically Dispersed Fe-N_(4) sites and Fe_(3)C Particles Catalyzing Polysulfides Conversion in li-s Batteries

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Chemical Research in Chinese Universities 2022年第5期38卷 1232-1238页

作者： CHEN Weijie XIA Huicong GUO Kai JIN Wangzhe DU Yu YAN Wenfu QU Gan ZHANG Jianan College of Materials science and Engineering Zhengzhou UniversityZhengzhou 450001P.R.China state Key Laboratory of Inorganic synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012P.R.China

lithium-sulfur(li-s)batteries have been puzzled by the“shuttle effect”.In the recent years,catalytic materials present a huge potential for solving this problem.However,the exploitation for catalytic activity was still challenging in li-s batteries.In this article,we put forward a single atom catalyst(sAC)of FeN_(4) coupled with Fe_(3)C on the N-doped carbon(FeN_(4)/Fe_(3)C@NC)by one-step pyrolysis method.The FeN_(4) and Fe_(3)C synergistically catalyze the polysulfides conversion when the N-doped carbon provides the high conductive three-dimensional skeleton in li-s batteries.As a result,the FeN_(4)/Fe_(3)C@NC shows a specific capacity of 1100 mA·h/g at 0.2 C(1 C=1675 mA/g).In addition,the FeN_(4)/Fe_(3)C@NC maintains 99.01%of the pristine specific capacity after 100 cycles at 0.5 C,indicating the improved electrochemical performance in li-s batteries.This work sheds new lights on the design of engineering catalysts for developing high-performance li-s batteries.

关键词： FeN_(4) Fe_(3)C Li-S battery shuttle effect

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Enhancing lithium-sulfur battery performance with In_(2)O_(3)-In_(2)s_(3)@NsC heterostructures:synergistic effects of double barrier and catalytic transformation

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Journal of Materials science & Technology 2024年第2期169卷 105-114页

作者： Deqing He Chunyu Zhu Yutao Huo Zhonghao Rao school of Energy and Environmental Engineering Hebei University of TechnologyTianjin 300401China Hebei Key Laboratory of Thermal science and Energy Clean Utilization Hebei University of TechnologyTianjin 300401China school of Low-carbon Energy and Power Engineering China University of Mining and TechnologyXuzhou 221116China

The sluggish redox reaction kinetics of lithium polysulfides(liPss)are considered the main obstacle to the commercial application of lithium-sulfur(li-s)batteries.To accelerate the conversion by catalysis and inhibit the shuttling of soluble liPss in li-s batteries,a solution is proposed in this study.The solution involves fabrication of N,s co-doped carbon coated In_(2)O_(3)/In_(2)s_(3)heterostructure(In_(2)O_(3)-In_(2)s_(3)@NsC)as a multifunctional host material for the cathode.The In_(2)O_(3)-In_(2)s_(3)@NsC composite can reduce the Gibbs free energy for the conversion reactions of liPss,which results in superior performance.The synergy between different components in In_(2)O_(3)-In_(2)s_(3)@NsC and the unique 3D structure facilitate ion and electron transport in li-s batteries.The In_(2)O_(3)-In_(2)s_(3)@NsC/li 2 s 6 cathode exhibits excellent rate capacity,with a capacity of 599 mAh g−1 at 5.5 C,and good cycle stability,with a capacity of 436 mAh g^(−1)after 1000 cycles at 1 C.Overall,this study proposes a promising solution to improve the energy storage properties of li-s batteries,which could potentially facilitate the commercialization of li-s batteries.

关键词： Li-S battery Multifunctional host material synergy Heterostructures Energy storage properties

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Rational synthesis of chitin-derived nitrogen-doped porous carbon nanofibers for efficient polysulfide confinement

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Nano Research 2023年第6期16卷 8478-8487页

作者： shanfeng Yang shuiping Luo Xinji Dong li Tian Pei Kang shen Jinliang Zhu school of Resources Environment and MaterialsCollaborative Innovation Centre of Sustainable Energy MaterialsCollege of Chemistry and Chemical EngineeringGuangxi UniversityNanning 530004China Department of Chemistry and Academy for Advanced Interdisciplinary studies Southern University of Science and Technology(SUSTech)Shenzhen 518055China Hunan Provincial Key Laboratory of Advanced Materials for New Energy storage and Conversion Hunan University of Science and TechnologyXiangtan 411201China

Principles of inexpensive biotechnology are being increasingly used to address the problems posed by the use of lithium-sulfur batteries.We used chitin,a low-cost marine biowaste product,as a precursor for the in-situ preparation of chitin-derived nitrogendoped hierarchical porous carbon fibers(CNHPCFs)containing abundant pores.These materials are characterized by varying morphologies and high specific surface areas and present a hierarchical porous structure.CNHPCFs adsorb polysulfides,exhibit good ionic conductivity,and can be potentially used to generate green energy.These properties help address the problems of volume expansion and slow transport.The CNHPCF-1@s cathode exhibits excellent cycling performance and high capacity(1368.80 mAh·g^(−1)at 0.2 C;decay rate:0.011%per turn at 5 C).The high electrochemical reversibility recorded for CNHPCF-1@s and the stepwise reaction mechanism followed were studied using the in-situ X-ray diffraction and in-situ Raman spectroscopy techniques.The results reported herein can potentially help develop new ideas for the recycling and treatment of marine biofertilizers.The results can also provide a platform to improve the application prospects of lithium-sulfur batteries.

关键词： chitin carbon fiber Li-S battery in-situ Raman in-situ X-ray diffraction

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