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High-performance localized high-concentration electrolytes by diluent design for long-cycling lithium metal batteries

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Chinese Chemical Letters 2024年第4期35卷 244-247页

作者： Zhe Wang Li-Peng Hou Qian-Kui Zhang Nan Yao aibing chen Jia-Qi Huang Xue-Qiang Zhang College of Chemical and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuang 050018China Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China School of Materials Science and Engineering Beijing Institute of TechnologyBeijing 100081China

Electrolyte design is essential for stabilizing lithium metal anodes and localized high-concentration electrolyte(LHCE) is a promising one. However, the state-of-the-art LHCE remains insufficient to ensure long-cycling lithium metal anodes. Herein, regulating the solvation structure of lithium ions in LHCE by weakening the solvating power of diluents is proposed for improving LHCE performance. A diluent,1,1,2,2,3,3,4,4-octafluoro-5-(1,1,2,2-tetrafluoroethoxy) pentane(OFE), with weaker solvating power is introduced to increase the proportion of aggregates(an anion interacts with more than two lithium ions,AGG-n) in electrolyte compared with the commonly used 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether(TTE). The decomposition of AGG-n in OFE-based LHCE intensifies the formation of anion-derived solid electrolyte interphase and improves the uniformity of lithium deposition. Lithium metal batteries with OFE-based LHCE deliver a superior lifespan of 190 cycles compared with 90 cycles of TTE-based LHCE under demanding conditions. Furthermore, a pouch cell with OFE-based LHCE delivers a specific energy of 417 Wh/kg and undergoes 49 cycles. This work provides guidance for designing high-performance electrolytes for lithium metal batteries.

关键词： Lithium metal anodes Electrolyte Diluents Solid electrolyte interphase Pouch cells

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A review of solid-state lithium metal batteries through in-situ solidification

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Science China Chemistry 2024年第1期67卷 67-86页

作者： Pan Xu Zong-Yao Shuang chen-Zi Zhao Xue Li Li-Zhen Fan aibing chen Haoting chen Elena Kuzmina Elena Karaseva Vladimir Kolosnitsyn Xiaoyuan Zeng Peng Dong Yingjie Zhang Mingpei Wang Qiang Zhang Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China National and Local Joint Engineering Laboratory for Lithium-ion Batteries and Materials Preparation Technology Key Laboratory of Advanced Battery Materials of Yunnan ProvinceFaculty of Metallurgical and Energy EngineeringKunming University of Science and TechnologyKunming 650093China Institute of Advanced Materials and Technology University of Science and Technology BeijingBeijing 100083China College of Chemical and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuang 050018China Ordos Carbon Neutral Research and Application Co. Ltd.Ordos City 017010China Ufa Institute of Chemistry UFRC RAS Ufa 450054Russia Institute for Carbon Neutrality Tsinghua UniversityBeijing 100084China Shanxi Research Institute for Clean Energy Tsinghua UniversityTaiyuan 030032China

High-energy-density lithium metal batteries are the next-generation battery systems of choice,and replacing the flammable liquid electrolyte with a polymer solid-state electrolyte is a prominent conduct towards realizing the goal of high-safety and high-specific-energy devices.Unfortunately,the inherent intractable problems of poor solid-solid contacts between the electrode/electrolyte and the growth of Li dendrites hinder their practical applications.The in-situ solidification has demonstrated a variety of advantages in the application of polymer electrolytes and artificial interphase,including the design of integrated polymer electrolytes and asymmetric polymer electrolytes to enhance the compatibility of solid–solid contact and compatibility between various electrolytes,and the construction of artificial interphase between the Li anode and cathode to suppress the formation of Li dendrites and to enhance the high-voltage stability of polymer electrolytes.This review firstly elaborates the history of in-situ solidification for solid-state batteries,and then focuses on the synthetic methods of solidified electrolytes.Furthermore,the recent progress of in-situ solidification technology from both the design of polymer electrolytes and the construction of artificial interphase is summarized,and the importance of in-situ solidification technology in enhancing safety is emphasized.Finally,prospects,emerging challenges,and practical applications of in-situ solidification are envisioned.

关键词： in-situ solidification polymer electrolyte artificial solid electrolyte interphase rechargeable lithium metal batteries dendrite-free lithium metal anode

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A three-way electrolyte with ternary solvents for high-energy-density and long-cycling lithium-sulfur pouch cells

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SusMat 2024年第2期4卷 1-12页

作者： Zheng Li Legeng Yu chen-Xi Bi Xi-Yao Li JinMa Xiang chen Xue-Qiang Zhang aibing chen Haoting chen Zuoru Zhang Li-Zhen Fan Bo-Quan Li cheng Tang Qiang Zhang Tsinghua Center for Green Chemical Engineering Electrification Beijing Key Laboratory of Green Chemical Reaction Engineering and TechnologyDepartment of Chemical EngineeringTsinghua UniversityBeijingChina School of Materials Science and Engineering Beijing Institute of TechnologyBeijingChina Institute of Advanced Materials and Technology University of Science and TechnologyBeijingChina Shanxi Research Institute for Clean Energy Tsinghua UniversityTaiyuanChina Center for Next-Generation Energy Materials and School of Chemical Engineering Sungkyunkwan UniversityJangan-GuSuwon-SiGyeonggi-DoRepublic of Korea College of Chemical and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuangChina Ordos Carbon Neutral Research and Application Co. Ltd.Kangbashi DistrictOrdos CityInner MongoliaChina Institute for Carbon Neutrality Tsinghua UniversityBeijingChina

Lithium–sulfur(Li–S)batteries promise high-energy-density potential to exceed the commercialized lithiumion batteries but suffer from limited cycling lifespan due to the side reactions between lithium polysulfides(LiPSs)and Li metal anodes.Herein,a three-way electrolyte with ternary solvents is proposed to enable high-energy-density and long-cycling Li–S pouch cells.Concretely,ternary solvents composed of 1,2-dimethoxyethane,di-isopropyl sulfide,and 1,3,5-trioxane are employed to guarantee smooth cathode kinetics,inhibit the parasitic reactions,and construct a robust solid electrolyte interphase,respectively.The cycling lifespan of Li–S coin cells with 50μm Li anodes and 4.0 mg cm^(−2) sulfur cathodes is prolonged from88 to 222 cycles using the three-way electrolyte.Nano-heterogeneous solvation structure of LiPSs and organic-rich solid electrolyte interphase are identified to improve the cycling stability of Li metal anodes.Consequently,a 3.0 Ah-level Li–S pouch cell with the three-way electrolyte realizes a high energy density of 405 Wh kg^(−1) and undergoes 27 cycles.Thiswork affords a three-way electrolyte recipe for suppressing the side reactions of LiPSs and inspires rational electrolyte design for practical high-energy-density and long-cycling Li–S batteries.

关键词： lithium metal anodes lithium-sulfur batteries pouch cells solid electrolyte interphase three-way electrolyte

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Ni nanoparticles confined by yolk-shell structure of CNT-mesoporous carbon for electrocatalytic conversion of CO_(2): Switching CO to formate

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Journal of Energy Chemistry 2022年第7期31卷 224-229,I0006页

作者： Juan Du aibing chen College of Chemical and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuang 050018HebeiChina

Electrochemical reduction of CO_(2)(CO_(2)ER) to formate has been a promising route to produce value-added chemicals.Developing low-cost and efficient electrocatalysts with high product selectivity is still a grand challenge.Herein,a novel Ni nanoparticles-anchored CNT coated by mesoporous carbon with yolk-shell structure (CNT/Ni@mC) catalysis was designed for CO_(2)ER.Ni nanoparticles were confined in the cavity between CNT and mesoporous carbon shell and the confined space can be controlled by tuning the amount of silica precursor.The mesoporous carbon shell and confined space are beneficial to charge transmission during CO_(2)ER.In contrast to previous studies,the CNT/Ni@mC catalyst presents selectivity toward formate rather than CO.Electrochemical in situ attenuated total reflection Fourier transform infrared spectroscopy measurements indicate the presence of a COO* intermediate that converts to formate under CO_(2)ER conditions.The well-defined structural feature of the confined space of the Ni-based catalyst for selective CO_(2)ER to formate may facilitate in-depth mechanistic understandings on structural factors that affect CO_(2)ER performance.

关键词： Carbon dioxide electrochemical reduction Nickel-based catalyst Formate Yolk-shell CNT

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Self-deposition for mesoporous carbon nanosheet with supercapacitor application

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Chinese Journal of Chemical Engineering 2023年第3期55卷 34-40页

作者： Juan Du aibing chen Senlin Hou Xueqing Gao College of Chemical and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuang 050018China The Second Hospital of Hebei Medical University Shijiazhuang 050000China

Porous carbon sheets have wide application prospects in many fields,especially in energy storage of supercapacitor due to the features combining both 2D structure and porous architectures.Herein,a self-deposition approach is proposed to obtain N-doped mesoporous carbon nanosheets (N-MCNs),using 3-aminophenol (3-AF) as precursor and Mg(OH)_(2) sheet as hard template.This process realizes the direct carbon formation using 3-AF monomer as carbon precursor under the catalysis of hard template avoiding the polymerization and utilization of solvent.The mass ratio of 3-AF to Mg(OH)_(2) plays an important role in determining the pore structures and the resulting capacitance behavior.The results show that N-MCNs with a mass ratio of 3-AF and Mg(OH)_(2) of 1:1 have good electrochemical behavior for supercapacitors.This N-MCNs based electrode exhibits a high capacitance of 240 F·g^(-1)at 1 A·g^(-1),good rate performance(75.4%retention ratio at 20 A·g^(-1)),and high cycling stability with 98.3% initial capacitance retained after 10000 cycles.Symmetric supercapacitors on N-MCNs achieve energy density of 18.2 W·h·kg^(-1) and power density of 0.4 kW·kg^(-1) operated within a wide potential range of 0–1.6 V in 1.0 mol·L^(-1) Na_(2)SO_(4) solution,exhibiting its potential for electrode materials with high performance.

关键词： Monomer self-deposition Mg(OH)_(2)catalysis Hard template Carbon nanosheet Supercapacitor

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CNT modified by mesoporous carbon anchored by Ni nanoparticles for CO_(2) electrochemical reduction

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Carbon Energy 2022年第6期4卷 1274-1284页

作者： Juan Du aibing chen Senlin Hou Jing Guan College of Chemical and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuangHebeiChina The Second Hospital of Hebei Medical University ShijiazhuangHebeiChina School of Environmental and Municipal Engineering Qingdao University of TechnologyQingdaoShandongChina

The design of novel catalysts for efficient electroreduction of CO_(2) into valueadded chemicals is a promising approach to alleviate the energy crisis.Herein,we successfully modify the carbon nanotube by a layer of mesoporous carbon shell anchored by nickel(Ni)nanoparticles.Ni species effectively enable carbon deposition derived from pyrolysis of surfactant 1-hexadecyl trimethyl ammonium bromide to form a mesoporous carbon shell.At the same time,Ni nanoparticles can be embedded in the mesoporous carbon shell due to the confinement effect.Owing to the dispersive Ni nanoparticles and N-doping active sites of mesoporous carbon,the as-prepared electrocatalyst exhibits exciting catalytic performance for the selective reduction of CO_(2) to carbon monoxide(CO)with a maximum Faradaic efficiency of 98%at a moderate overpotential of−0.81 V(vs.reversible hydrogen electrode)and a high partial current density of 60 mA cm^(−2) in H-cell with an aqueous electrolyte.

关键词： carbon dioxide electrochemical reduction carbon monoxide CNT highly dispersed nickel nanoparticles

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Continuous Fabrication of Ti_(3)C_(2)T_x MXene-Based Braided Coaxial Zinc-Ion Hybrid Supercapacitors with Improved Performance

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Nano-Micro Letters 2022年第2期14卷 206-215页

作者： Bao Shi La Li aibing chen Tien-Chien Jen Xinying Liu Guozhen Shen Hebei University of Science and Technology 70 Yuhua RoadShijiazhuang 050018People’s Republic of China State Key Laboratory for Superlattices and Microstructures Institute of Semiconductors Chinese Academy of Sciences&Center of Materials Science and Optoelectronic Engineering University of Chinese Academy of SciencesBeijing 100083People’s Republic of China Department of Mechanical Engineering Science Kingsway CampusUniversity of JohannesburgAuckland ParkJohannesburg 2006South Africa Institute for Development of Energy for African Sustainability University of South AfricaPrivate Bag X6Florida 1710South Africa

Zinc-ion hybrid fiber supercapacitors(FSCs)are promising energy storages for wearable electronics owing to their high energy density,good flexibility,and weavability.However,it is still a critical challenge to optimize the structure of the designed FSC to improve energy density and realize the continuous fabrication of super-long FSCs.Herein,we propose a braided coaxial zinc-ion hybrid FSC with several meters of Ti_(3)C_(2)T_x MXene cathode as core electrodes,and shell zinc fiber anode was braided on the surface of the Ti_(3)C_(2)T_x MXene fibers across the solid electrolytes.According to the simulated results using ANSYS Maxwell software,the braided structures revealed a higher capacitance compared to the spring-like structures.The resulting FSCs exhibited a high areal capacitance of 214 mF cm^(-2),the energy density of 42.8μWh cm^(-2)at 5 mV s^(-1),and excellent cycling stability with 83.58%capacity retention after 5000 cycles.The coaxial FSC was tied several kinds of knots,proving a shape-controllable fiber energy storage.Furthermore,the knitted FSC showed superior stability and weavability,which can be woven into watch belts or embedded into textiles to power smart watches and LED arrays for a few days.

关键词： Ti_(3)C_(2)T_x MXene Fiber supercapacitor Coaxial structure Zinc-ion

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Study on the occurrence state of indium in sphalerite of Dulong Sn–Zn–In polymetallic deposit,Southwest China

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Acta Geochimica 2023年第3期42卷 572-582页

作者： Lisheng Gao Hanjie Wen Chuanwei Zhu Xin Nie aibing chen Guangshu Yang Faculty of Land Resources Engineering Kunming University of Science and TechnologyKunming 650093YunnanChina State Key Laboratory of Ore Deposit Geochemistry Institute of GeochemistryChinese Academy of SciencesGuiyang 550081GuizhouChina School of Earth Sciences and Resources Changan UniversityXi’an 710054ShanxiChina College of Earth and Planetary Sciences University of Chinese Academy of SciencesBeijing 100049China

The Dulong deposit,located in the Laojunshan area of southeastern Yunnan,China,is an important polymetallic deposit due to its high reserves of tin,zinc,and indium.The occurrence state of indium is critical for understanding its supernormal enrichment mechanism.Previous studies investigated the occurrence state of indium(including the valence state)based on the indium content in sphalerite and the correlation between metal concentrations.However,more evidence is needed to better constrain indium occurrence at the micro-,nano-,or even atomic scale.In this study,EPMA-FIB-SEM-TEM and XPS techniques were employed to investigate the indium distribution characteristics and occurrence state in sphalerite from the Dulong Sn–Zn–In polymetallic deposit.The maximum concentration of indium in the indium-rich sphalerite samples is 0.37%,and the results of the EPMA analysis showed a relatively homogeneous distribution of indium in sphalerite.The FIB-SEM-TEM results demonstrated that the lattice stripes of sphalerite were periodically and continuously distributed at the nanoscale,confirming that sphalerite in the deposit was an excellent single crystal structure,and the peak heights of the various characteristic peaks of indium in the EDX spectra were relatively close to each other,with no distinct peaks of high indium content.In addition,the XPS results indicate that the element valence state of indium in sphalerite is In^(3+),and it combines with S^(2-)to form a bond.These results indicate that indium in sphalerite of the Dulong deposit is uniformly distributed at both the micro-and nanoscale,and there is no indium-independent mineral.In^(3+)enters the crystal lattice of sphalerite by replacing Zn2+in the form of isomorphic substitution.

关键词： Sphalerite Indium Occurrence state Dulong Sn–Zn–In polymetallic deposit

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Strong interaction between phosphorus and wrinkle carbon sphere promote the performance of phosphorus anode material for lithium-ion batteries

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Nano Research 2023年第7期16卷 9273-9279页

作者： Xin Li Shaojie Zhang Juan Du Lele Liu Chong Mao Jie Sun aibing chen College of Chemical and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuang 050018China Department of Chemical Engineering University of JohannesburgJohannesburg 2028South Africa Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Zhuhai Smoothway Electronic Materials Co. Ltd.Zhuhai 519050China

The durable red phosphorus(RP)anode for lithium-ion batteries(LIBs)has attracted great attention owing to its high theoretical specific capacity(2596 mA·h·g^(-1))and moderate lithiation potential(~0.7 V vs.Li^(+)/Li).However,its intrinsic poor electrical conductivity,enormous volume expansion,and soluble intermediates(lithium polyphosphides,Li_(x)PP_(s))lead to poor cycling performance.To overcome these issues,we introduce a new type of wrinkle carbon spheres as the host for loading phosphorus through a vaporization-condensation strategy.Density functional theory calculations reveal that the wrinkle carbon sphere shows strong binding energy with P4 molecule,accelerating the adsorption and polymerization of P4,thus enhancing RP conversion in the preparation process.In the lithiation/delithiation process,the wrinkle carbon has strong bonding with phosphorus and strong adsorption with Li_(x)PP_(s),resulting in excellent cycling performance.The design strategy to modify RP polymerization via reforming the interaction between wrinkle carbon spheres and phosphorus expands the application of RP for LIBs and beyond.

关键词： red phosphorus high wrinkle carbon spheres vaporization-condensation strategy lithium-ion batteries

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Fast and extensive intercalation chemistry in Wadsley-Roth phase based high-capacity electrodes

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Journal of Energy Chemistry 2022年第6期31卷 601-611,I0017页

作者： Miao Wang Zhenpeng Yao Qianqian Li Yongfeng Hu Xiuping Yin aibing chen Xionggang Lu Jiujun Zhang Yufeng Zhao Institute for Sustainable Energy&College of Sciences Shanghai UniversityShanghai 200444China Department of Chemistry and Chemical Biology Harvard University12 Oxford StreetCambridgeMA 02138United States Materials Genome Institute Shanghai UniversityShanghai 200444China Canadian Light Source 44 Innovation BoulevardSaskatoonSK S7N 2 V3Canada College of Chemical and Pharmaceutical Engineering Hebei University of Science and Technology70 Yuhua RoadShijiazhuang 050018China State Key Laboratory of Advanced Special Steel Shanghai Key Laboratory of Advanced FerrometallurgyShanghai UniversityShanghai 200444 China Key Laboratory of Applied Chemistry Yanshan UniversityQinhuangdao 066004HebeiChina School of Resource and Environmental Sciences Wuhan UniversityWuhan 430072HubeiChina

Wadsley-Roth (W-R) structured oxides featured with wide channels represent one of the most promising material families showing compelling rate performance for lithium-ion batteries.Herein,we report an indepth study on the fast and extensive intercalation chemistry of phosphorus stabilized W-R phase PNb_(9)O_(25) and its application in high energy and fast-charging devices.We explore the intercalation geometry of PNb_(9)O_(25) and identify two geometrical types of stable insertion sites with the total amount much higher than conventional intercalation-type electrodes.We reveal the ion transportation kinetics that the Li ions initially diffuse along the open type Ⅲ channels and then penetrate to edge sites with low kinetic barriers.During the lithiation,no remarkable phase transition is detected with nearly intact host phosphorous niobium oxide backbone.Therefore,the oxide framework of PNb_(9)O_(25) keeps almost unchanged with all the fast diffusion channels and insertion cavities well-maintained upon cycling,which accomplishes the unconventional electrochemical performance of W-R structured electrodes.

关键词： Wadsley-Roth phase PNb_(9)O_(25) Intercalation chemistry Ion transportation kinetics Lithium-ion batteries

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