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A polyimide cathode with superior stability and rate capability for lithium-ion batteries

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Nano Research 2019年第6期12卷 1355-1360页

作者： Jianghui Zhao Tuo Kang Yanli Chu Peng Chen Feng Jin Yanbin Shen Liwei Chen School of Nano Technology and Nano Bionics University of Science and Technology of ChinaHefei 230026China i-Lab CAS Center for Excellence in NanoscienceSuzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123Chin School of Chemistry and Chemical Engineering Shanghai Jiaotong UniversityShanghai 200240China

Organic-based electrode materials for lithium-ion batteries (LIBs) are promising due to their high theoretical capacity,structure versatility and environmental benignity.However,the poor intrinsic electric conductivity of most polymers results in slow reaction kinetics and hinders their application as electrode materials for LIBs.A binder-free self-supporting organic electrode with excellent redox kinetics is herein demonstrated via in situ polymerization of a uniform thin polyimide (PI) layer on a porous and highly conductive carbonized nanofiber (CNF) framework.The PI active material in the porous PI@CNF film has large physical contact area with both the CNF and the electrolyte thus obtains superior electronic and ionic conduction.As a result,the PI@CNF cathode exhibits a discharge capacity of 170 mAh·g^-1 at 1 C (175 mA·g^-1),remarkable rate-performance (70.5% of 0.5 C capacity can be obtained at a 100 C discharge rate),and superior cycling stability with 81.3% capacity retention after 1,000 cycles at 1 C.Last but not least,a four-electron transfer redox process of the PI polymer was realized for the first time thanks to the excellent redox kinetics of the PI@CNF electrode,showing a discharge capacity exceeding 300 mAh·g^-1 at a current of 175 mA·g^-1.

关键词： polyimide carbonized nanofibers organic electrode material rate capability lithium-ion batteries

In-situ emb e dding zeolitic imidazolate framework derived Co–N–C bifunctional catalysts in carbon nanotube networks for flexible Zn–air batteries

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Journal of Energy Chemistry 2019年第11期28卷 170-176页

作者： Bo Lv Sha Zeng Wei Yang Jian Qiao Chao Zhang Chengfeng Zhu Minghai Chen Jiangtao Di Qingwen Li School of Nano-Technology and Nano-Bionics University of Science and Technology of ChinaHefei 230026AnhuiChina Key Laboratory of Multifunctional Nanomaterials and Smart Systems Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123JiangsuChina

Recently, the development of high-performance bifunctional oxygen catalysts integrated with flexible conductive scaffolds f or rechargeable metal-air batteries has attracted considerable interest, driving by fastgrowing wearable electronics. Herein, we report a flexible bifunctional oxygen catalyst thin film consisting of Co–N–C bifunctional catalysts embedding in carbon nanotube(CNT) networks. The catalyst is readily prepared by pyrolysis of cobalt-based zeolitic imidazolate frameworks(ZIF-67) that are in-situ synthesized in CNT networks. Such catalyst film demonstrates very high catalytic activities for oxygen reduction(onset potential: 0.91 V, and half-wave potential: 0.87 V vs. RHE) and oxygen evolution(10 m Acm^-2 at 1.58 V) reactions, high methanol tolerance property, and long-term stability(97% current retention). Moreover, our integrated catalyst film shows very good structure flexibility and robustness. Based on the obtained film air electrodes, flexible Zn–air batteries demonstrate low charging and discharging overpotentials(0.82 V at 1 m A cm^-1) and excellent structure stability in the bending tests. These results indicate that presently reported catalyst films are potential air electrodes for flexible metal–air batteries.

关键词： Air electrodes Carbon nanotube films Bifunctional catalysts Zn-air batteries Zeolitic imidazolate framework

High-pseudocapacitance of porous and square NiO@NC nanosheets for high-performance lithium-ion batteries

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Rare Metals 2021年第6期40卷 1451-1458页

作者： Ze-Lin Cai Zi-Lin Peng Meng-Qi Wang Jia-Yan Wu Hao-Sen Fan Yu-Fei Zhang School of Chemistry and Chemical Engineering Guangzhou UniversityGuangzhou 510006China School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou 510006China

Layered nickel oxides have been focused with intense research interests as high-performance lithium-ion batterie(LIB)anode.However,it is hard to obtain few layered nickel oxides material directly as it easily forms bulk material with the strong interaction between the interlayer.In this work,two-dimensional(2 D)nickel-based coordination polymers were successfully prepared according to aqueous phase copolymerization approach.And then uniform carbondoped NiO nanosheets were successfully obtained from facile solution assembly and post-thermal treatment.The detailed electrochemical testing shows that the uniform NiO nanocrystals encapsulated into porous N-doped carbon(NiO@NC)nanosheets present much higher rate capability with the discharge specific capacity of 782.7 mAh·g^(-1) at high current density of 2.0 A·g^(-1) than pure NiO(690 mAh·g^(-1)).It also shows long-term cycling performance with 91%retention after 50 cycles at 1.0 A·g^(-1).The high rate capability,cycling stability and the easy synthesis make NiO@NC nanosheets as a promising candidate for LIB anode and build up new way for the fabrication of metal oxides anode materials.

关键词： Anode batteries Square NiO@NC nanosheets Pseudocapacitive

Polygonal multi-polymorphed Li4Ti5Oi2@rutile TiO2 as anodes in lithium-ion batteries

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Nano Research 2019年第4期12卷 897-904页

作者： Chang Hyun Hwang Hee-eun Kim Inho Nam Jin Ho Bang Department ofBionano Technology Hanyang University 55 Hanyangdaehak-ro Sangnok-gu Ansan Gyeonggi-do 15588 Republic of Korea School of Chemical Engineering & Materials Science Chung-Ang University 84 Heukseok-ro Dongjak-gu Seoul 06974 Republic of Korea Department of Chemical and Molecular Engineering Hanyang University 55 Hanyangdaehak-ro Sangnok-gu Ansan Gyeonggi-do 15588 Republic of Korea

Li4Ti50i2 (LTO) has attracted considerable attention in lithium-ion battery (LIB) applications because of its favorable characteristics as an anode material. Despite its promise, the widespread use of LTO is still limited primarily due to its intrinsically poor electric and ionic con ductivities and high surface reactivity. To address these issues, we desig ned polyg onal nano architectures composed of various Li-Ti oxide crystal polymorphs by a facile synthesis route. Depending on the pH condition, this synthesis approach yields multi-polymorphed Li-Ti oxides where the interior is dominantly composed of a Li-rich phase and the exterior is a Li-deficient (or Li-free) phase. As one of these variations, a polygonal LTO-rutile TiO2 structure is formed. The rutile TiO2 on the surface of this LTO composite significantly improves the kinetics of Li^+ insertion/extraction because the channel along the o-axis in TQ2 provides a Li^+ highway due to the significantly low energy barrier for Li^+ diffusion. Moreover, the presenee of rutile TiO2, which is less reactive with a carbonate-based electrolyte, ensures Iong-term stability by suppress)ng the undesirable interfacial reaction on LTO.

关键词： micro-polygon structure Li-Ti oxide multi-polymorphs Li4Ti5Oi2@ rutile TiO2 anode lithium-ion batteries

Thickness evolution of graphite-based cathodes in the dual ion batteries via in operando optical observation

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Journal of Energy Chemistry 2019年第2期28卷 122-128页

作者： Na Li Yaoda Xin Haosen Chen Shuqiang Jiao Hanqing Jiang Wei-Li Song Daining Fang Institute of Advanced Structure Technology Beijing Institute of Technology Beijing Key Laboratory of Lightweight Multi-Functional Composite Materials and Structures Beijing Institute of Technology Overseas Education College Nanjing University of Technology Collaborative Innovation Center of Electric Vehicles in Beijing Beijing Institute of Technology State Key Laboratory of Advanced Metallurgy University of Science and Technology Beijing School for Engineering of Matter Transport and EnergyArizona State University State Key Laboratory for Turbulence and Complex Systems College of EngineeringPeking University

Graphite has been currently considered as a promising cathode material in dual ion batteries(DIBs)due to its unique features of sp2 hybridized carbon and stacked two-dimensional layered structures.However,unexpected volume/thickness changes in the graphite cathodes,induced by the intercalation/deintercalation of anions with large molecular size have been known to be a critical problem in designing DIB cells.To understand the volume/thickness changes in the DIB electrodes,in operando optical observing apparatus has been employed to observe the cross-section view of a graphite-based cathode upon cycles in the present work.The observation suggests that the cathode initially presented a huge irreversible thickness change(60%),and such thickness variation was prone to reduce and remain <20% in the following cycles.The results from both in operando observation and electrochemical characterizations collectively indicate that the greater thickness variation at initial cycle should be attributed to both anion intercalation into graphite-based cathodes and irreversible decomposition of chemical components in the DIB system.The method here highlights a universal route for fundamentally understanding the electrodes of huge volume variation.

关键词： Dual ion batteries In operando optical observation Graphite Cathode Thickness evolution

A scalable synthesis of silicon nanoparticles as high-performance anode material for lithium-ion batteries

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Rare Metals 2019年第3期38卷 199-205页

作者： Jin Li Juan-Yu Yang Jian-Tao Wang Shi-Gang Lu China Automotive Battery Research Institute Co. Ltd.General Research Institute for Nonferrous Metals

In this work, a scalable and cost-effective method including mechanical milling, centrifugation and spray drying was developed to fabricate Si nanoparticles.The synthesized Si nanoparticles show an average size of 62 nm and exhibit a narrow particle size distribution. The influence of particle sizes on electrochemical performance of Si-based electrode was investigated, and it is found that as the particle size decreases in the studied range, the Si particles show a lower specific capacity and a higher irreversible capacity loss(ICL). Furthermore, an oxide layer with thickness of ～3 nm was detected on the surface of the as-received Si nanoparticles, and this layer can be effectively removed by hydrofluoric acid(HF) etching,resulting in much improved electrochemical performance over the as-received samples.

关键词： Lithium-ion batteries Anode Silicon nanoparticles Wet grinding mill

Biomass-derived nitrogen-doped hierarchical porous carbon as efficient sulfur host for lithium–sulfur batteries

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Journal of Energy Chemistry 2020年第5期29卷 61-67页

作者： Qinghuiqiang Xiao Gaoran Li Minjie Li Ruiping Liu Haibo Li Pengfei Ren Yue Dong Ming Feng Zhongwei Chen Department of Materials Science and Engineering China University of Mining&Technology(Beijing)Beijing 100083China Department of Chemical Engineering University of WaterlooWaterloo N2L3G1OntarioCanada Key Laboratory of Functional Materials Physics and Chemistry of the Ministry of Education Jilin Normal UniversityChangchun 130103JilinChina

Lithium-sulfur(Li-S) battery is a potential energy storage technology with high energy density and low cost. However, the gap between theoretical expectation and practical performance limits its wide implementation. Herein, we report a nitrogen-doped porous carbon derived from biomass pomelo peel as sulfur host material for Li-S batteries. The hierarchical porous architecture and the polar surface introduced by N-doping render a favorable combination of physical and chemical sulfur confinements as well as an expedite electron/ion transfer, thus contributing to a facilitated and stabilized sulfur electrochemistry. As a result, the corresponding sulfur composite electrodes exhibit an ultrahigh initial capacity of 1534.6 mAh g^-1, high coulombic efficiency over 98% upon 300 cycles, and decent rate capability up to 2 C. This work provides an economical and effective strategy for the fabrication of advanced carbonaceous sulfur host material as well as the significant improvement of Li-S battery performance.

关键词： Biomass-derived material Porous carbon Lithium sulfur batteries Electrochemical performance

Grafting polymeric sulfur onto carbon nanotubes as highly-active cathode for lithium–sulfur batteries

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Journal of Energy Chemistry 2020年第3期29卷 27-33页

作者： Junfeng Wu Siyu Ding Shihai Ye Chao Lai Institute of New Energy Material Chemistry School of Materials Science and EngineeringNational Institute for Advanced MaterialsNankai UniversityTianjin 300350China School of Chemistry and Materials Science Jiangsu Normal UniversityXuzhou 221116JiangsuChina

Lithium–sulfur(Li–S)batteries are being explored as promising advanced energy storage systems due to their ultra-high energy density.However,fast capacity fading and low coulombic efficiency,resulting from the dissolution of polysulfides,remain a serious challenge.Compared to weak physical adsorptions or barriers,chemical confinement based on strong chemical interaction is a more effective approach to address the shuttle issue.Herein,we devise a novel polymeric sulfur/carbon nanotube composite for Li–S battery,for which 2,5-dithiobiurea is chosen as the stabilizer of long-chain sulfur.This offers chemical bonds which bridge the polymeric sulfur and carbon nanotubes.The obtained composite can deliver an ultra-high reversible capacity of 1076.2 m Ahg^-1(based on the entire composite)at the rate of 0.1 C with an exceptional initial Coulombic efficiency of 96.2%,as well as remarkable cycle performance.This performance is mainly attributed to the reaction reversibility of the obtained polymeric sulfur-based composite during the discharge/charge process.This was confirmed by density functional theory calculations for the first time.

关键词： Lithium–sulfur batteries Polymeric sulfur Carbon nanotubes DFT calculations High capacity

Controlled synthesis of nanosized Si by magnesiothermic reduction from diatomite as anode material for Li-ion batteries

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International Journal of Minerals,Metallurgy and Materials 2020年第4期27卷 515-525页

作者： Li-fen Guo Shi-yun Zhang Jian Xie Dong Zheng Yuan Jin Kang-yan Wang Da-gao Zhuang Wen-quan Zheng Xin-bing Zhao State Key Laboratory of Silicon Materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027China Key Laboratory of Advanced Materials and Applications for batteries of Zhejiang Province Hangzhou 310027China Hangzhou Branch Zhejiang Zotye Automobile Corporation LimitedHangzhou 310018China Shanghai Han Xing Science and Technology Co. Ltd.Shanghai 201322China

Li-ion batteries(LIBs)have demonstrated great promise in electric vehicles and hybrid electric vehicles.However,commercial graphite materials,the current predominant anodes in LIBs,have a low theoretical capacity of only 372 mAh·g?1,which cannot meet the everincreasing demand of LIBs for high energy density.Nanoscale Si is considered an ideal form of Si for the fabrication of LIB anodes as Si–C composites.Synthesis of nanoscale Si in a facile,cost-effective way,however,still poses a great challenge.In this work,nanoscale Si was prepared by a controlled magnesiothermic reaction using diatomite as the Si source.It was found that the nanoscale Si prepared under optimized conditions(800°C,10 h)can deliver a high initial specific capacity(3053 mAh·g?1 on discharge,2519 mAh·g?1 on charge)with a high first coulombic efficiency(82.5%).When using sand-milled diatomite as a precursor,the obtained nanoscale Si exhibited a well-dispersed morphology and had a higher first coulombic efficiency(85.6%).The Si–C(Si:graphite=1:7 in weight)composite using Si from the sand-milled diatomite demonstrated a high specific capacity(over 700 mAh·g?1 at 100 mA·g?1),good rate capability(587 mAh·g?1 at 500 mA·g?1),and a long cycle life(480 mAh·g?1 after 200 cycles at 500 mA·g?1).This work gives a facile method to synthesize nanoscale Si with both high capacity and high first coulombic efficiency.

关键词： silicon anode magnesiothermic reduction diatomite Li-ion batteries