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Large-scale manufacturing sulfide superionic conductor for advancing all-solid-state batteries

Matter 2025年

作者： Wang, Shuo Lou, Chenjie Wu, Xinbin Lin, Jing Gautam, Ajay Li, Shenghao Huang, Jielei Cheng, Zhu Zhang, Shengnan Zhang, Xin Strauss, Florian Brezesinski, Torsten Luo, Guoqiang Tang, Mingxue Shen, Yang Lin, Yuanhua Nan, Ce-Wen Center of Smart Materials and Devices State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Material Science and Engineering Wuhan University of Technology Wuhan430070 China Center for High Pressure Science and Technology Advanced Research Beijing100094 China State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing100084 China Kaiserstr. 12 Karlsruhe76131 Germany Department of Radiation Science and Technology Delft University of Technology JB Delft2629 Netherlands

Lithium argyrodites with high ionic conductivities are favorable solid electrolytes (SEs) for all-solid-state batteries (ASSBs). However, their low preparation efficiency and poor cycling performance hinder their large-scale applications. In this work, we demonstrate successful large-scale production (over 1 kg per batch for the first time) of Li5.5PS4.5Cl0.75Br0.75 (LPSCB) by fast dry mixing followed by annealing, which presents high room temperature ionic conductivities of 13 mS cm−1 for cold-pressed and 25 mS cm−1 for sintered pellets. Combining neutron powder diffraction and 6Li → 7Li tracer-exchange nuclear magnetic resonance (NMR) spectroscopy measurements, we show that intercage jumps frequently occur through the 48h-16e-48h pathway in LPSCB, promoting the overall lithium conduction. The assembled ASSBs using LPSCB and a LiNi0.83Co0.11Mn0.06O2 electrode can be cycled for over 2,500 cycles at a 0.5 C rate and 1,800 cycles at a 2 C rate without any capacity degradation. Our results will accelerate the commercialization of sulfide SE for ASSBs. © 2025 Elsevier Inc.

关键词： Neutron powder diffraction

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Optimal design approach of interpenetrating pre-stressed metal-ceramic composites based on deep learning neural network

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Composite Structures 2025年 368卷

作者： Liu, Kun Lai, Xin Liu, Lisheng Zhang, Jinyong Liu, Yifei Hubei Longzhong Laboratory Wuhan University of Technology Demonstration Zone XiangYang537134 China Hubei Key Laboratory of Theory and Application of Advanced Materials Mechanics Wuhan University of Technology Wuhan430070 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China University of Rochester RochesterNY14527 United States

In this work, we proposed a new pre-stressed metal-ceramic interpenetrating structure to improve the apparent tensile strength of ceramic. In addition, an optimization design framework was constructed by integrating machine learning and gradient descent optimization algorithm for the optimization design of ceramic interpenetrating composites. The optimized metal-ceramic interpenetrating structure can achieve a balance of the stress state of the ceramic phase between intensity and distribution by ingeniously control the confinement and topology of the metal phase. More specifically, the surrogate model we constructed through deep neural network (DNN) can efficiently predict the relationship between the structure and its stress state. The final result obtained can achieve excellent pre-stress effect while making the structure lightweight. © 2025 Elsevier Ltd

关键词： Deep neural networks

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Designing polymer nanocomposites with high energy density using machine learning

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npj Computational Materials 2021年第1期7卷 999-1007页

作者： Zhong-Hui Shen Zhi-Wei Bao Xiao-Xing Cheng Bao-Wen Li Han-Xing Liu Yang Shen Long-Qing Chen Xiao-Guang Li Ce-Wen Nan State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Center of Smart Materials and DevicesWuhan University of TechnologyWuhanChina International School of Materials Science and Engineering Wuhan University of TechnologyWuhanChina Hefei National Laboratory for Physical Sciences at the Microscale Department of Physics and CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics University of Science and Technology of China HefeiChina Department of Materials Science and Engineering The Pennsylvania State UniversityUniversity ParkPAUnited States School of Materials Science and Engineering State Key Lab of New Ceramics and Fine ProcessingTsinghua UniversityBeijingChina

Addressing microstructure-property relations of polymer nanocomposites is vital for designing advanced dielectrics for electrostatic energy ***,we develop an integrated phase-field model to simulate the dielectric response,charge transport,and breakdown process of polymer ***,based on 6615 high-throughput calculation results,a machine learning strategy is schemed to evaluate the capability of energy *** find that parallel perovskite nanosheets prefer to block and then drive charges to migrate along with the interfaces in x-y plane,which could significantly improve the breakdown strength of polymer *** verify our predictions,we fabricate a polymer nanocomposite P(VDF-HFP)/Ca_(2)Nb_(3)O_(10),whose highest discharged energy density almost doubles to 35.9 J cm^(−3) compared with the pristine polymer,mainly benefit from the improved breakdown strength of 853 MVm^(−1).This work opens a horizon to exploit the great potential of 2D perovskite nanosheets for a wide range of applications of flexible dielectrics with the requirement of high voltage endurance.

关键词： polymer energy perovskite

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Defects enriched hollow porous Co-N-doped carbons embedded with ultrafine CoFe/Co nanoparticles as bifunctional oxygen electrocatalyst for rechargeable flexible solid zinc-air batteries

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Nano Research 2021年第3期14卷 868-878页

作者： Zhao Lei Yangyang Tan Zeyi Zhang Wei Wu Niancai Cheng Runzhe Chen Shichun Mu Xueliang Sun College of Materials Science and Engineering Fuzhou UniversityFuzhou350108China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan430070China Department of Mechanical and Materials Engineering The University of Western OntarioLondonONN6A 5B9Canada

The construction and design of highly efficient and inexpensive bifunctional oxygen electrocatalysts substitute for noble-metal-based catalysts is highly desirable for the development of rechargeable Zn-air battery(ZAB).In this work,a bifunctional oxygen electrocatalysts of based on ultrafine CoFe alloy(4-5 nm)dispersed in defects enriched hollow porous Co-N-doped carbons,made by annealing SiO2 coated zeolitic imidazolate framework-67(ZIF-67)encapsulated Fe *** hollow porous structure not only exposed the active sites inside ZIF-67,but also provided efficient charge and mass *** strong synergetic coupling among high-density CoFe alloys and Co-N_(x) sites in Co,N-doped carbon species ensures high oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)***-principles simulations reveal that the synergistic promotion effect between CoFe alloy and Co-N site effectively reduced the formation energy of from O^(*)to OH^(*).The optimized CoFe-Co@PNC exhibits outstanding electrocatalytic stability and activity with the overpotential of only 320 mV for OER at 10 mA·cm^(−2) and the half-wave potential of 0.887 V for ORR,outperforming that of most recent reported bifunctional electrocatalysts.A rechargeable ZAB constructed with CoFe-Co@PNC as the air cathode displays long-term cyclability for over 200 h and high power density(152.8 mW·cm^(−2)).Flexible solid-state ZAB with our CoFe-Co@PNC as the air cathode possesses a high open circuit potential(OCP)up to 1.46 V as well as good bending *** universal structure design provides an attractive and instructive model for the application of nanomaterials derived from MOF in the field of sustainable flexible energy applications device.

关键词： oxygen reduction reaction ultrafine CoFe alloy hollow porous carbons zeolitic imidazolate framework-67 Zn-air battery

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Tuning the dual-active sites of ZIF-67 derived porous nanomaterials for boosting oxygen catalysis and rechargeable Zn-air batteries

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Nano Research 2021年第7期14卷 2353-2362页

作者： Zeyi Zhang Yangyang Tan Tang Zeng Liyue Yu Runzhe Chen Niancai Cheng Shichun Mu Xueliang Sun College of Materials Science and Engineering Fuzhou UniversityFuzhou 350108China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Department of Mechanical and Materials Engineering University of Western OntarioLondonON N6A 5B9Canada

The rational control of the active site of metal-organic frameworks(MOFs)derived nanomaterials is essential to build efficient bifunctional oxygen reduction/evolution reaction(ORR/OER)***,through designing and constructing a Co_(3)O_(4)-Co heterostructure embedded in Co,N co-doped carbon polyhedra derived(Co_(3)O_(4)-Co@NC)from the in-situ compositions of ZIF-67 and cobalt nanocrystals synthesized by the strategy of in-situ NaBH4 reduction,the dual-active site(Co_(3)O_(4)-Co and Co-N_(x))is synchronously realized in a MOFs derived *** formed Co_(3)O_(4)-Co@NC shows excellent bifunctional electrocatalytic activity with ultra-small potential gap(ΔE=E_(j=10)(OER)–E_(1/2)(ORR))of 0.72 V,which surpasses the commercial Pt/C and RuO_(2) *** theory calculation results reveal that the excellent bifunctional electrocatalytic activity can be attributed to the charge redistribution of Co of Co-N_(x) induced by the synergistic effects of well-tuned active sites of Co_(3)O_(4)-Co nanoparticle and Co-N_(x),thus optimizing the rate-determining step of the desorption of O_(2)^(*)intermediate in ORR and OH^(*)intermediate in *** rechargeable Zn-air batteries with our bifunctional catalysts exhibit superior performance as well as high cycling *** simple-effective optimization strategy offers prospects for tuning the active site of MOF derived bifunctional catalyst in electrochemical energy devices.

关键词： dual-active sites bifunctional oxygen electrocatalysts metal−organic frameworks Zn-air batteries density functional theory(DFT)

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Sulfur-linked carbonyl polymer as a robust organic cathode for rapid and durable aluminum batteries

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Journal of Energy Chemistry 2021年第12期30卷 320-327,I0007页

作者： Liang Fang Limin Zhou Lianmeng Cui Peixin Jiao Qinyou An Kai Zhang Department of Energy and Materials Engineering Dongguk University-SeoulSeoul 04620Republic of Korea Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Engineering Research Center of High-efficiency Energy Storage(Ministry of Education)Renewable Energy Conversion and Storage Center(RECAST)College of ChemistryNankai UniversityTianjin 300071China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070HubeiChina Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Foshan 528200GuangdongChina

Rechargeable aluminum batteries are believed as a promising next-generation energy-storage system due to abundant low-cost Al sources and high volumetric specific *** Al-storage cathodes,however,are plagued by strong electrostatic interaction between host materials and carrier ions,leading to large overpotential and undesired cycling stability as well as sluggish ion diffusion ***,sulfur-linked carbonyl polymer based on perylene-3,4,9,10-tetracarboxylic dianhydride(PTCDA) as the cathode materials for ABs is proposed,which demonstrates a small voltage polarization(135 mV),a reversible capacity of 110 mAh g^(-1) at 100 mA g^(-1) even after 1200 cycles,and rapid Al-storage *** with PTCDA,the sulfide polymer possesses higher working voltage because of its lower LUMO energy level according to theoretical *** ordered carbonyl active sites in sulfide polymer contribute to the maximized material utilization and rapid ion coordination and dissociation,resulting in superior rate ***,the bridged thioether bonds endow the polysulfide with robust and flexible structure,which inhibits the dissolution of active materials and improves cycling *** work implies the importance of ordered arrangement of redox active moieties for organic electrode,which provides the theoretical direction for the structural design of organic materials applied in multivalent-ion batteries.

关键词： Aluminum batteries Organic materials Carbonyl polymer Electrochemical active sites Ordered arrangement

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Scalable Assembly of Layered Dielectric Nanocomposites Filled with Perovskite Nanosheets for Flexible Electronics

SSRN

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SSRN 2024年

作者： Fu, Si Ren, Lele Wang, Jian Liu, Hexing Zhang, Pengchao Shen, Zhonghui Zhang, Xin Tu, Rong Zhang, Song Nan, Ce-Wen Li, Bao-Wen State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China School of Materials Science and Engineering Wuhan University of Technology Wuhan430070 China State Key Lab of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing100084 China

Polymer-based dielectrics have attracted much attention in the field of flexible electronics due to their excellent flexibility, dielectric and mechanical properties. However, the rational design of nanofiller-polymer nanocomposite for improving dielectric and mechanical properties remains challenging. Herein, layered nanocomposites filled with high-κ Ca2Nb3O10 perovskite nanosheets were fabricated via shear-flow induced alignment of nanosheets. The hierarchical structure and good dispersion of nanosheets endowed the layered nanocomposites with an outstanding modulus of 12.7 GPa and toughness of 1.8 MJ/m3. Meanwhile, the layered nanocomposites exhibited a high dielectric constant of 14.7, a low dielectric loss of 4.2%, and low leakage current density -7 A/cm2. The layered high-κ nanocomposites designed in this work will have broad application prospects in th flexible electronics. © 2024, The Authors. All rights reserved.

关键词： Perovskite

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Articular cartilage and osteochondral tissue engineering techniques:Recent advances and challenges

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Bioactive Materials 2021年第12期6卷 4830-4855页

作者： Wenying Wei Honglian Dai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Biomedical Materials and Engineering Research Center of Hubei ProvinceWuhan University of TechnologyWuhan430070China International School of Materials Science and Engineering Wuhan University of TechnologyWuhan430070China Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu Hydrogen ValleyFoshan528200China

In spite of the considerable achievements in the field of regenerative medicine in the past several decades,osteochondral defect regeneration remains a challenging issue among diseases in the musculoskeletal system because of the spatial complexity of osteochondral units in composition,structure and *** order to repair the hierarchical tissue involving different layers of articular cartilage,cartilage-bone interface and subchondral bone,traditional clinical treatments including palliative and reparative methods have showed certain improvement in pain relief and defect *** is the development of tissue engineering that has provided more promising results in regenerating neo-tissues with comparable compositional,structural and functional characteristics to the native osteochondral *** in this review,some basic knowledge of the osteochondral units including the anatomical structure and composition,the defect classification and clinical treatments will be first *** we will highlight the recent progress in osteochondral tissue engineering from perspectives of scaffold design,cell encapsulation and signaling factor incorporation including bioreactor *** products for osteochondral defect repair will be analyzed and summarized ***,we will discuss the current obstacles and future directions to regenerate the damaged osteochondral tissues.

关键词： Osteochondral tissue engineering Cartilage tissue engineering Gradient scaffold Bioreactors

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Non‑Enzyme,Temperature Calibrating,and Bioactive Fiber‑based Flexible Sensors for Dopamine and Lactic Acid Detection

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advanced Fiber Materials 2024年第2期6卷 501-511页

作者： Maowen Xie Guang Yao Xingyi Gan Chunhong Zhang Tianyao Zhang Qian Wang Xinqin Li Chenzheng Zhou Kangning Zhao Min Gao Taisong Pan Yuan Lin School of Materials and Energy University of Electronic Science and Technology of ChinaChengdu 610054SichuanChina State Key Laboratory of Electronic Thin Films and Integrated Devices University of Electronic Science and Technology of ChinaChengdu 610054SichuanChina Medico‑Engineering Cooperation on Applied Medicine Research Center University of Electronic Science and Technology of ChinaChengdu 610054SichuanChina Shenzhen Institute for Advanced Study University of Electronic Science and Technology of ChinaShenzhen 518110China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing International School of Materials Science and EngineeringWuhan University of TechnologyWuhan 430070HubeiChina

Flexible electrochemical biosensors enable the in-situ monitoring and quantification of human biochemical constituents in molecular scale,spearheading and thriving the field toward precision ***,specific biorecognition elements for multiplexed biomarkers detection,temperature stability and versatility need to be improved for higher ***,we propose a bioactive sensor patch comprising a non-enzyme Co_(3)O_(4)/carbon fiber-based biorecognition element and a temperature calibration *** optimized serpentine configuration renders the sensor intimate and seamless attachment with skin,operating robustly even subjected to 40%tensile *** fiber-based sensor could selectively monitor dopa-mine and lactic acid contents based on cyclic voltammetry and amperometry,*** bioanalytical results at room temperature indicate that the electrochemical biosensor has a wide detection range(0.001–1.100 mM for dopamine and 2–35 mM for lactic acid),excellent selectivity and reproducibility(maximum error 3.2%for dopamine and 5.6%for lactic acid).In addition,temperature calibration contour maps of these two biomarkers are established in an ambient temperature range from 25 to 45℃.The continuously collected data could be aggregated and wirelessly transmitted to portable devices using an electrochemical signal transducer and an acquisition module,promising personalized and preventative health care in various scenarios.

关键词： Bioactive fiber Electrochemical selectivity Dopamine Lactic acid Temperature calibration Sensor

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Biomimetic brain-like nanostructures for solid polymer electrolytes with fast ion transport

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Science China Materials 2022年第6期65卷 1476-1484页

作者： Ahmed Eissa Abdelmaoula Lulu Du Lin Xu Yu Cheng Amir AMahdy Muhammad Tahir Ziang Liu Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and EngineeringWuhan University of TechnologyWuhan 430070China Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu Hydrogen ValleyFoshan 528200China Mining and Metallurgical Department Faculty of EngineeringAl-Azhar UniversityCairo 11884Egypt

The intrinsic drawbacks of electrolytes and the growth of lithium dendrites limit the development of commercial lithium *** address the aforementioned challenges,a novel biomimetic brain-like nanostructure(BBLN)solid polymer electrolyte was created by manipulating the shape of the incorporated *** designed BBLN solid polymer electrolyte was created by incorporating spherical core-shell(UIO-66@67)fillers into polymer electrolyte,which is significantly different from traditional polymer-based composite ***-66@67 spherical nanoparticles are highly favorable to eliminating polymer electrolyte stress and deformation during solidification,indicating a great potential for fabricating highly uniform BBLN solid polymer electrolytes with a substantial number of continuous ***,spherical nanoparticles can significantly reduce the crystalline structure of polymer electrolytes,improving polymer chain segmental movement and providing continuous pathways for rapid ion *** a result,BBLN solid polymer electrolyte shows excellent ionic conductivity(9.2×10^(−4)S cm^(−1)),a high lithium transference number(0.74),and outstanding cycle stability against lithium electrodes over 6500 h at room *** concept of biomimetic brain-like nanostructures in this work demonstrates a novel strategy to enhance ion transport in polymerbased electrolytes for solid-state batteries.

关键词： brain structure spherical nanoparticles continuous interphase nanophase separation MOF-in-MOF

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