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high energy density in ultra-thick and flexible electrodes enabled by designed conductive agent/binder composite

Journal of energy Chemistry 2024年第3期90卷 133-143,I0005页

作者： Xiaoyu Shen Hailong Yu Liubin Ben Wenwu Zhao Qiyu Wang Guanjun Cen Ronghan Qiao Yida Wu Xuejie Huang Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China Songshan Lake Materials Laboratory Dongguan 523808Guangdong China

Thick electrodes can increase incorporation of active electrode materials by diminishing the proportion of inactive constituents,improving the overall energy density of batteries.However,thick electrodes fabricated using the conventional slurry casting approach frequently exhibit an exacerbated accumulation of carbon additives and binders on their surfaces,invariably leading to compromised electrochemical properties.In this study,we introduce a designed conductive agent/binder composite synthesized from carbon nanotube and polytetrafluoroethylene.This agent/binder composite facilitates production of dry-process-prepared ultra-thick electrodes endowed with a three-dimensional and uniformly distributed percolative architecture,ensuring superior electronic conductivity and remarkable mechanical resilience.Using this approach,ultra-thick LiCoO_(2)(LCO) electrodes demonstrated superior cycling performance and rate capabilities,registering an impressive loading capacity of up to 101.4 mg/cm^(2),signifying a 242% increase in battery energy density.In another analytical endeavor,time-of-flight secondary ion mass spectroscopy was used to clarify the distribution of cathode electrolyte interphase(CEI) in cycled LCO electrodes.The results provide unprecedented evidence explaining the intricate correlation between CEI generation and carbon distribution,highlighting the intrinsic advantages of the proposed dry-process approach in fine-tu ning the CEI,with excellent cycling performance in batteries equipped with ultra-thick electrodes.

关键词： Conductive agent/binder composite Dry process Ultra-thick electrodes high energy density CEI reconstruction ToF-SIMS

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An empirical model for high energy density lithium-(ion)batteries with ultra-thick electrodes

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Tungsten 2024年第1期6卷 230-237页

作者： Li-Ming Jin Guang-Guang Xing Nan Qin Yan-Yan Lu Jun-Sheng Zheng Cun-Man Zhang Jim P.Zheng School of Automotive Studies and Clean energy Automotive Engineering Center Tongji UniversityShanghai 201804China Department of Electrical Engineering University at BuffaloThe State University of New YorkBuffaloNY 14260USA

Increasing the electrode thickness is a significant method to decrease the weight and volume ratio of the inactive components for high energy density of the devices.In this contribution,we extracted a repeating unit in the configurations and establish the empirical energy density model based on some assumptions.In this model,the effects of the electrode thickness on the energy density for lithium-ion batteries(LIBs),lithium metal batteries(LMBs),and anode-free lithium batteries(ALBs)are evaluated quantitively with the current parameters of the batteries.The results demonstrate that the structure evolutions from LIBs,LMBs to ALBs with the reduction of the anode weight contribution,the energy density can be well improved exactly.While the increase of the thickness of the electrode provide another route to furthe r enhance the energydensity by decreasing the weight contribution of inactive materials;meanwhile the effects for ALBs are higher than LMBs and LIBs due to the higher weight ratio of inactive materials.This empirical energy density model is also applied into the practical system and provide intuitional results to guide the battery design for higher energy density.

关键词： Empirical model high energy density Lithium batteries Ultra-thick electrodes

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Fluorophosphates and fluorosulfates cathode materials: Progress towards high energy density sodium-ion battery

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Nano Research 2024年第3期17卷 1427-1440页

作者： Mohammed Hadouchi Jingrong Hou Toshinari Koketsu Abdelilah Lahmar Jiwei Ma Laboratoire de Chimie Appliquée des Matériaux Centre des Sciences des MatériauxFaculty of ScienceMohammed V University in RabatAvenue Ibn BattoutaBP 1014RabatMorocco Shanghai Key Laboratory for R&D and Application of Metallic Functional Materials Institute of New Energy for VehiclesSchool of Materials Science and EngineeringTongji UniversityShanghai 201804China Battery Materials Development Section Business Creation Sector R&D CenterMitsui Mining&Smelting Co.Ltd.362-0021 SaitamaJapan Laboratoiry of Condensed Matter Physics University of Picardie Jules Verne33 Rue Saint-Leu 80039AmiensFrance

The rapid diffusion of renewable energy boosts the wide deployment of large-scale energy storage system.With the low cost and high crustal abundance,sodium-ion battery(SIB)technology is expected to become a dominant technology in that area in the future.Toward the practical application,novel cathode materials are urged to develop that show high energy density without sacrificing their cost and benignity to the environment.While the years of many studies,this still remains a huge challenge to battery scientists.In this review,we discuss recent breakthroughs in SIB cathode materials with high energy density,namely fluorphosphates and fluorosulfates.The design of materials,the crystal structure,the electrochemical performance,and the underlaying intercalation mechanism are systematically reviewed.Useful strategies and research directions are also provided to advance future high-energy,low-cost,and ecofriendly cathode materials for next generation SIB.

关键词： fluorophosphates fluorosulfates crystal structure intercalation mechanism high energy density sodium-ion battery

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3D printing encouraging desired in-situ polypyrrole seed-polymerization for ultra-high energy density supercapacitors

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Journal of energy Chemistry 2024年第8期95卷 117-125页

作者： Tiantian Zhou Shangwen Ling Shuxian Sun Ruoxin Yuan Ziqin Wu Mengyuan Fu Hanna He Xiaolong Li Chuhong Zhang State Key Laboratory of Polymer Materials Engineering Polymer Research Institute Sichuan University

The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered architectures.Polypyrrole（PPy） emerges as an exceedingly conductive polymer and a prospective pseudocapacitive materials for supercapacitors,yet the inferior cyclic stability and unpredictable polymerization patterns severely impede its real-world applicability.Here,for the first time,an innovative seed-induced in-situ polymerization assisted 3D printing strategy is proposed to fabricate PPy-reduced graphene oxide/poly（vinylidene difluoride-cohexafluoropropylene）(PVDF-HFP)（PPy-rGO/PH） electrodes with controllable polymerization behavior and exceptional areal mass loading.The preferred active sites uniformly pre-planted on the 3D-printed graphene substrates serve as reliable seeds to induce efficient polypyrrole deposition,achieving an impressive mass loading of 185.6 mg cm-2(particularly 79.2 mg cm-2for polypyrrole) and a superior areal capacitance of 25.2 F cm-2at 2 mA cm-2for a 12-layer electrode.In agreement with theses appealing features,an unprecedented areal energy density of 1.47 mW h cm-2for a symmetrical device is registered,a rarely achieved value for other PPy/rGO-based supercapacitors.This work highlights a promising route to preparing high energy density energy storage modules for real-world applications.

关键词： 3D printing high energy density Polypyrrole Seed-induced polymerization Supercapacitor

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high-performance Ti_(3)C_(2)T_(x)achieved by polyaniline intercalation and gelatinization as a high-energy cathode for zinc-ion capacitor

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Nano Research 2024年第6期17卷 5305-5316页

作者： Peng Liao ZiYu Geng Xin Zhang Wenjie Yan Zenghui Qiu Haijun Xu College of Mathematics and Physics Beijing University of Chemical TechnologyBeijing 100029China

The actual manufacture of supercapacitors(SCs)is restricted by the inadequate energy density,and the energy density of devices can be properly promoted by assembling zinc-ion capacitors(ZICs)which used capacitive cathode and battery-type anode.Two-dimensional(2D)MXene has brought great focuses in the electrode research on the foundation of large redox-active surface,but the specific capacitance is still affected by the tight stacking of interlaminations.Ti_(3)C_(2)T_(x)@polyaniline(PANI)heterostructures are prepared by uniformly depositing the conductive polymer PANI nanorods as the intercalation agent into the external of Ti_(3)C_(2)T_(x)nanosheets to inhibit stacking.Subsequently,by using graphene oxide(GO)-assisted low-temperature hydrothermal self-assembly manufacture,2D heterostructures are assembled into the three-dimensional(3D)porous crosslinked Ti_(3)C_(2)T_(x)@PANI-reduced graphene oxide(RGO)hydrogels.Attributed to the synergistic work of PANI nanorods,Ti_(3)C_(2)T_(X)nanosheets,and 3D crosslinking frameworks of RGO to match capacitive and battery effects,3D porous hierarchical Ti_(3)C_(2)T_(x)@PANI-RGO heterostructure hydrogels have rich ion transport channels,a large number of active sites,and excellent reaction kinetics.ZIC is assembled by using Ti_(3)C_(2)T_(x)@PANI-RGO heterostructure hydrogels as cathodes and zinc foil as anodes.In this work,Ti_(3)C_(2)T_(x)@PANI-RGO//Zn ZIC exhibits a wide working window(2.0 V),marked specific capacitance(589.89 F·g^(−1)at 0.5 A·g−1),salient energy density(327.71 Wh·kg^(−1)at 513.61 W·kg^(−1)and 192.20 Wh·kg^(−1)at 13,005.87 W·kg^(−1)),and durable cycling stability(97.87%capacitance retention after 10,000 cycles at 10 A·g^(−1)).This study emphasizes the device design of ZICs and the broad prospect of Ti_(3)C_(2)T_(x)-based hydrogels as viable cathodes for ZICs.

关键词： polyaniline(PANI) Ti_(3)C_(2)T_(x)@PANI heterostructure intercalation process three-dimensional(3D)porous hydrogel high energy density zinc-ion capacitor

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Thin NASICON Electrolyte to Realize high energy density Solid-State Sodium Metal Battery

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energy & Environmental Materials 2023年第6期6卷 419-426页

作者： Jin An Sam Oh Xiaoyu Xu Zhihan Zeng Kexin Wang Nicholas Yew Jin Tan Eugene Kok Jiemin Huang Li Lu Singapore Institute of Manufacturing Technology A^(*)STAR(Agency for ScienceTechnology and Research)2 Fusionopolis WayInnovisSingapore City 138634Singapore Department of Mechanical Engineering National University of SingaporeSingapore City 117575Singapore

The solid-state electrolyte in a solid-state battery acts as an electrons'barrier and an ions'bridge between the two electrodes.As solid-state electrolyte does not store the mobile ions,it is necessary to achieve a thin solid-state electrolyte to reduce the internal resistance and enhance the energy density.In this work,a thin NASICON solid-state electrolyte,with a stoichiometry of Na_(3)Zr_(2)Si_(2)PO_(12),is fabricated by the tape-casting method and its thickness can be easily controlled by the gap between substrate and scraper.The areal-specific resistance and the flexural strength increase with the electrolyte thickness.A solid-state sodium metal battery with 86 pm thick Na_(3)Zr_(2)Si_(2)PO_(12)exhibits a reversible specific capacity of 73-78 mAh g^(-1)with a redox potential of 3.4 V at 0.2 C.This work presents the importance of electrolyte thickness to reduce internal resistance and achieve a high energy density for sodium batteries.

关键词： high energy density NASICON solid-state battery solid-state electrolyte tape casting

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Pathway for high-energy density LiMnFePO4 cathodes

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Progress in Natural Science:Materials International 2023年第1期33卷 126-131页

作者： Shaoluan Huang Wenzhong Lin Liewu Li Pei Liu Tao Huang Zhencheng Huang Jinli kong Wei Xiong Wenwei Yu Shenghua Ye Jiangtao Hu Qianling Zhang Jianhong Liu Graphene Composite Research Center College of Chemistry and Environmental Engineering Shenzhen University Shenzhen Eigen–Equation Graphene Technology Co.Ltd.

Polyanion cathodes are credited for its thermal stability and better safety, no matter in lithium ion batteries or sodium ion batteries. Polyanion oxides with phosphate groups came to the public’s attention in 1997, and the representative material is LiFePO4, which has been widely applied and plays a huge role in the field of powder batteries and energy storage system. However, owing to the low lithiation potentials and storage sites, the energy densities of polyanion cathodes have been restricted, resulting of low-endurance and limited application scenarios. Accordingly, here, we use cheap and environmental friendly raw materials as precursors to synthesis high energy density LiMn0.6Fe0.4PO4@C cathode by a simple spray-drying and high temperature calcination process.The self-designed liquid polyacrylonitrile(LPAN) is added for the intention of nanoparticle coating, conductive network construction and particle granulation. The low-cost and carbon-coated LiMn0.6Fe0.4PO4cathode exhibits excellent reversible capacity, low electrochemical polarization and excellent rate capacity, which maintains93.5% capacity retention after cycling 1000 times at 5C. The work introduces a new avenue to fabricate olivine structure cathodes with outstanding electrochemical performance for the high energy density lithium ion batteries.

关键词： Polyanion cathode Liquid polyacrylonitrile Cost effective high energy density high stability

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Fluorobenzene diluted low-density electrolyte for high-energy density and high-performance lithium-sulfur batteries

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Journal of energy Chemistry 2022年第5期31卷 752-761页

作者： Zhilong Han Shuping Li Mengjun Sun Renjie He Wei Zhong Chuang Yu Shijie Cheng Jia Xie State Key Laboratory of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina School of Physics Huazhong University of Science and TechnologyWuhan 430074HubeiChina State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina

The mass fraction of electrolytes is the crucial factor affecting the energy density of lithium-sulfur(Li-S)batteries. Due to the high porosity within the C/S cathode, high concentration of polysulfides, and side reaction in lithiun metal anode under lean electrolyte, it is extremely challenging to improve performance while reducing the electrolyte volume. Here, we report a novel electrolyte with relatively low density(1.16 g cm^(-2)), low viscosity(1.84 m Pa s), and high ionic conductivity, which significantly promotes energy density and cyclability of Li-S batteries under practical conditions. Moreover, such electrolyte enables a hybrid cathode electrolyte interphase(CEI) and solid electrolyte interface(SEI) layer with plentiful Li F, which leads to fast kinetics of ions transport and stable cyclability even under low temperatures.Compared to Li-S batteries in electrolyte employing 1,1,2,2-tetrafluoroethyl 2,2,3,3-tetrafluoropropyl ether(TTE) diluent, the ultra-thick cathode(20 mg cm^(-2)) shows a high capacity of 9.48 m Ah cm^(-2)and excellent capacity retention of 80.3% over 191 cycles at a low electrolyte-to-sulfur ratio(E/S = 2) and negative-to-positive capacity ratio(N/P = 2.5), realizing a 19.2% improvement in energy density in coin cells(from 370 to 441 Wh kg^(-1)) and a high energy density up to 467 Wh kg^(-1) in pouch cells. This study not only provides guidance for the electrolyte design but also paves the way for the development of high performance Li-S batteries under practical conditions.

关键词： high energy density Lithium-sulfur battery Thick sulfur electrode Lean electrolyte Low-density electrolyte

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Application-oriented hydrolysis reaction system of solid-state hydrogen storage materials for high energy density target:A review

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Journal of energy Chemistry 2022年第11期31卷 218-238,I0007页

作者： Jing Yao Zhen Wu Huan Wang Fusheng Yang Jianwei Ren Zaoxiao Zhang School of Chemical Engineering and Technology Xi’an Jiaotong UniversityXi’an 710049ShaanxiChina Department of Mechanical Engineering Science University of JohannesburgJohannesburg 2092South Africa State Key Laboratory of Multiphase Flow in Power Engineering Xi’an Jiaotong UniversityXi’an 710049ShaanxiChina

Hydrogen storage and delivery technology is still a bottleneck in the hydrogen industry chain.Among all kinds of hydrogen storage methods,light-weight solid-state hydrogen storage(LSHS)materials could become promising due to its intrinsic high hydrogen capacity.Hydrolysis reaction of LSHS materials occurs at moderate conditions,indicating the potential for portable applications.At present,most of review work focuses on the improvement of material performance,especially the catalysts design.This part is important,but the others,such as operation modes,are also vital to to make full use of material potential in the practical applications.Different operation modes of hydrolysis reaction have an impact on hydrogen capacity to various degrees.For example,hydrolysis in solution would decrease the hydrogen capacity of hydrogen generator to a low value due to the excessive water participating in the reaction.Therefore,application-oriented operation modes could become a key problem for hydrolysis reaction of LSHS materials.In this paper,the operation modes of hydrolysis reaction and their practical applications are mainly reviewed.The implements of each operation mode are discussed and compared in detail to determine the suitable one for practical applications with the requirement of high energy density.The current challenges and future directions are also discussed.

关键词： Solid-state hydrogen storage high energy density Hydrogen generator Hydrolysis reaction Portable applications

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MXene-based symmetric supercapacitors with high voltage and high energy density

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Materials Reports(energy) 2022年第1期2卷 105-111页

作者： Wei Zheng Joseph Halim Per O.Å.Persson Johanna Rosen Michel W.Barsoum Department of Physics Chemistry and Biology(IFM)Linkoping University58183LinkopingSweden Department of Materials Science and Engineering Drexel University19104PhiladelphiaPAUSA

MXene-based aqueous symmetric supercapacitors(SSCs)are attractive due to their good rate performances and green nature.However,it remains a challenge to reach voltages much over 1.2 V,which significantly diminishes their energy density.Herein,we report on Mo_(1.33)CTz MXene-based SSCs possessing high voltages in a 19.5 M LiCl electrolyte.Benefiting from the vacancy-rich structure and high stable potential window of Mo_(1.33)CTz,the obtained SSCs deliver a maximum energy density of>38.2 mWh cm^(-3) at a power density of 196.6 mW cm^(-3) under an operating voltage of 1.4 V,along with excellent rate performance and impressive cycling stability.This highly concentrated LiCl electrolyte is also applicable to Ti_(3)C_(2)Tz,the most widely studied MXene,achieving a maximum energy density of>41.3 mWh cm^(-3) at a power density of 165.2 mW cm^(-3) with an operating voltage of 1.8 V.The drop in energy density with increasing power in the Ti_(3)C_(2)Tz cells was steeper than for the Mo-based cells.This work provides a roadmap to develop superior SSCs with high voltages and high energy densities.

关键词： MXene Symmetric supercapacitor high voltage high energy density highly concentrated electrolyte

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