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In-situ construction of PDOL electrolyte with dual-reinforced stable interface for high-voltage lithium metal batteries

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Science China Chemistry 2024年第5期67卷 1664-1671页

作者： Yingkang Wu Yuzhou Bai wujie dong Xue Wang Wenqin Ma Fuqiang Huang State Key Lab of Metal Matrix Composites School of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China School of Physical Science and Technology Shanghai Tech UniversityShanghai 201210China Shanghai Institute of Ceramics Chinese Academy of SciencesShanghai 200050China

In-situ polymerized electrolytes significantly enhance the interfacial compatibility of lithium metal batteries(LMBs). Typically,in-situ polymerized 1,3-dioxolane(PDOL) exhibits low interfacial resistance, yet still suffers from low ionic conductivity and a narrow electrochemical stability window(ESW). Here, an ultra-stable PDOL-based polymer electrolyte is developed by incorporating plasticizers of tetramethylene sulfone(TMS) and fluorinated ethylene carbonate(FEC) into the 3D cross-linked network, achieving a significant enhancement in the transport capacity and efficiency of Li-ion. The ionic conductivity reaches3.63×10^(-4)S cm^(-1)even at room temperature, and the transference number(tLi^(+)) is even higher at 0.85. Furthermore, the ESW of this electrolyte can be increased to 4.5 V with the addition of TMS, which forms a thin and robust antioxidant cathode-electrolyte interface(CEI) on the surface of high-voltage LiCoO_(2). FEC generates an inorganic-rich solid-electrolyte interface(SEI) on the Li anode, which effectively inhibits the growth of lithium dendrites. Benefiting from the aforementioned advantages, the highvoltage lithium metal battery demonstrates outstanding long-cycle stability, with 93.2% capacity retention after 200 cycles. This work offers a straightforward and accessible method for the practical implementation of high energy density in-situ polymerized solid-state LMBs.

关键词： solid polymer electrolyte in-situ polymerization PDOL high-voltage LMBs

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Understanding the influence of crystal packing density on electrochemical energy storage materials

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eScience 2024年第1期4卷 17-56页

作者： wujie dong Fuqiang Huang State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China State Key Laboratory of Rare Earth Materials Chemistry and Applications College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

Crystal structure determines electrochemical energy storage characteristics;this is the underlying logic of material *** date,hundreds of electrode materials have been developed to pursue superior ***,it remains a great challenge to understand the fundamental structure–performance relationship and achieve quantitative crystal structure design for efficient energy *** this review,we introduce the concept of crystal packing factor(PF),which can quantify crystal packing *** then present and classify the typical crystal structures of attractive cathode/anode *** PF analyses of different materials,including polymorphs,isomorphs,and others,are performed to clarify the influence of crystal packing density on energy storage performance through electronic and ionic ***,the practical electronic/ionic conductivities of energy storage materials are based on their intrinsic characteristics related to the PF yet are also affected by extrinsic *** PF provides a novel avenue for understanding the electrochemical performance of pristine materials and may offer guidance on designing better *** approaches involve size regulation,doping,carbon additives,and other *** also propose extended PF concepts to understand charge storage and transport behavior at different ***,we provide our insights on the major challenges and prospective solutions in this highly exciting field.

关键词： Packing density Packing factor Energy storage materials Rate capability Crystal structure Structure-activity relationship Electronic conductivity Ionic conductivity

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High‑Entropy Layered Oxide Cathode Enabling High‑Rate for Solid‑State Sodium‑Ion Batteries

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Nano-Micro Letters 2024年第1期16卷 160-171页

作者： Tianxun Cai Mingzhi Cai Jinxiao Mu Siwei Zhao Hui Bi Wei Zhao wujie dong Fuqiang Huang State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050People’s Republic of China State Key Laboratory of Rare Earth Materials Chemistry and Applications College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871People’s Republic of China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049People’s Republic of China Zhongke Institute of Strategic Emerging Materials Yixing 214213JiangsuPeople’s Republic of China

Na-ion O3-type layered oxides are prospective cathodes for Na-ion batteries due to high energy density and ***,such cathodes usually suffer from phase transitions,sluggish kinetics and air instability,making it difficult to achieve high performance solid-state sodium-ion ***,the high-entropy design and Li doping strategy alleviate lattice stress and enhance ionic conductivity,achieving high-rate performance,air stability and electrochemically thermal stability for Na_(0.95)Li_(0.06)Ni_(0.25)Cu_(0.05)Fe_(0.15)Mn_(0.49)O_(2).This cathode delivers a high reversible capacity(141 mAh g^(−1)at 0.2C),excellent rate capability(111 mAh g^(−1)at 8C,85 mAh g^(−1)even at 20C),and long-term stability(over 85%capacity retention after 1000 cycles),which is attributed to a rapid and reversible O3–P3 phase transition in regions of low voltage and suppresses phase ***,the compound remains unchanged over seven days and keeps thermal stability until 279℃.Remarkably,the polymer solid-state sodium battery assembled by this cathode provides a capacity of 92 mAh g^(−1)at 5C and keeps retention of 96%after 400 *** strategy inspires more rational designs and could be applied to a series of O3 cathodes to improve the performance of solid-state Na-ion batteries.

关键词： High-entropy High-rate performance Li-TM interaction Air stability O3 layered oxide cathode

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Ultrafast sodium storage of alkylamine molecule tailored MnPSenabled by quasi-topological intercalation mechanism

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Science China Chemistry 2024年

作者： Xueyang Tu Ke Fan Baixin Peng Zhuoran Lv Yiran Hao wujie dong Wei Zhao Zuocheng Wang Haitao Huang Yuqiang Fang Fuqiang Huang State Key Laboratory of High-Performance Ceramics and Superfine Microstructure Shanghai Institute of Ceramics Chinese Academy of Sciences Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Research Institute for Smart Energy The Hong Kong Polytechnic University State Key Lab of Metal Matrix Composites School of Materials Science and Engineering Shanghai Jiao Tong University Zhangjiang Institute for Advanced Study Shanghai Jiao Tong University Jiangxi Far East Battery Co. Ltd.

Two-dimensional transition metal trithiophosphates （TMPS3,TM=Mn,Fe,Co,etc.） are competitive anode materials for sodium-ion batteries （SIBs） due to their high theoretical capacity (>1,300 mAh g-1) but suffer from limited practical capacity(～300 mAh g-1) and inferior rate capability caused by sluggish Na+intercalation/deintercalation kinetics and severe structural ***,alkylamine molecules are first proposed as intercalation guests to significantly boost the electrochemical activity and stability of *** to MnPS3,C3H9N-MnPS3enlarges the interlayer spacing from 6.48 to 10.23?and shows a 10～5times higher electrical conductivity,which provides fast ion/electron transport and high strain adaptability,realizing a quasi-topological Na+intercalation ***,C3H9N-MnPS3exhibits an ultrahigh reversible capacity of 775m Ah g-1at 0.5 A g-1and superior high-rate cycling stability with～100%capacity retention after 2,500 cycles at 15 A g-1,ranking it among the top metal trithiophosphate-based anode materials *** calculations indicate that the improved sodium storage performance of C3H9N-MnPS3results from the reduced bonding energy of P–S bonds and increased adsorption energy of Na+.This work is expected to provide an efficient strategy for the design of high-performance layered anode materials for SIBs.

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Electrodes with Electrodeposited Water-excluding Polymer Coating Enable High-Voltage Aqueous Supercapacitors

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Research 2020年第1期2020卷 711-723页

作者： wujie dong Tianquan Lin Jian Huang Yuan Wang Zhichao Zhang Xin Wang Xiaotao Yuan Jie Lin I-Wei Chen Fuqiang Huang State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China State Key Laboratory of Rare Earth Materials Chemistry and Applications College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Department of Materials Science and Engineering University of PennsylvaniaPhiladelphiaPA 19104USA

Aqueous supercapacitors are powerful energy sources,but they are limited by energy density that is much lower than lithium-ion *** raising the voltage beyond the thermodynamic potential for water splitting(1.23 V)can boost the energy density,there has been much effort on water-stabilizing salvation additives such as Li_(2)SO_(4) that can provide an aqueous electrolyte capable of withstanding~1.8 *** by the first-principles calculations that reveal water can promote hydrogen and oxygen evolution reactions,here,we pursue a new strategy of covering the electrode with a dense electroplated polymerized polyacrylic acid,which is an electron insulator but a proton conductor and proton *** combined effect of salvation and coating expands the electrochemical window throughout pH 3 to pH 10 to 2.4V for both fast and slow proton-mediated redox *** allows activated carbon to quadruple the energy density,a kilogram of nitrogen-doped graphene to provide 127 Watt-hour,and both to have improved endurance because of suppression of water-mediated ***,aqueous supercapacitors can now achieve energy densities quite comparable to that of a lithium-ion battery,but at 100 times the charging/discharging speed and cycle durability.

关键词： lithium durability battery

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Achieving highly stable Sn-based anode by a stiff encapsulation heterostructure

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Science China Materials 2022年第3期65卷 695-703页

作者： Ruizhe Li Jijian Xu Zhuoran Lv wujie dong Fuqiang Huang State Key Laboratory of High Performance Ceramics and Superfine Mincrostructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China Center of Materials Science and Optoelectronics Engineering University of Chinese of Academy of SciencesBeijing 100049China State Key Laboratory of Rare Earth Materials Chemistry and Applications College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

Rationally designed heterostructures provide attractive prospects for energy storage electrodes by combining different active materials with distinct electrochemical ***,through a phase separation strategy,a heterostructure of SnO_(2) encapsulated by amorphous Nb_(2)O_(5) is spontaneously ***-type anode Nb_(2)O_(5) outer shell,playing as reaction containers and fast ionic pathways,physically inhibits the Sn atoms’migration and enhances the reaction ***,strong chemical interactions are found at the SnO_(2)/Nb_(2)O_(5) interfaces,which ensure the solid encapsulation of the SnO_(2) cores even after 500 *** used for lithium-ion batteries,this heterostructured anode exhibits high cycling stability with a capacity of 626 mAhg^(-1) after 1000 cycles at 2Ag^(-1)(85% capacity retention)and good rate performance with the capacity of 340 mAhg^(-1) at 8Ag^(-1).

关键词： heterostructure encapsulation SnO2/Nb2O5 interface chemical interaction atom migration

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Two-dimensional TiNCl for capacitive-like lithium-ion storage

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Science China Materials 2022年第11期65卷 2942-2948页

作者： Linggang Fan Shaoning Zhang wujie dong Jijian Xu Xiangli Che Ruizhe Li Hui Bi Fuqiang Huang State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China State Key Laboratory of Rare Earth Materials Chemistry and Applications College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

In this study,TiNCl was designed and applied in high-rate lithium-ion batteries(LIBs),and the mechanism of the energy storage in TiNCl was *** Ti-N layer serves as the electronic conductive unit for its high conductivity,while the polyhedral channels constructed with Cl facilitate the transmission of Li ions serving as the ionic conductive *** addition,due to the negatively charged nature of Cl,the TiNCl anode has a capacitive contribution up to 99.5%at 1 mV *** at a high rate of 50 C,it still retains a remarkable reversible capacity of 202 mA h gafter 1000 *** concept based on the structure design develops new electrode materials with desired properties.

关键词： lithium-ion battery high-rate performance TiNCl titanium-based anode

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基于结构调节碳材料的掺氮种类和含量及其超级电容器储能应用

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无机材料学报 2021年第7期36卷 766-772,I0007-I0011页

作者：孙鹏张绍宁毕辉董武杰黄富强中国科学院上海硅酸盐研究所高性能陶瓷和超微结构国家重点实验室上海200050 中国科学院大学材料科学与光电技术学院北京100049 上海科技大学物理科学与技术学院上海200031 北京大学化学与分子工程学院稀土材料化学及应用国家重点实验室北京100871

碳材料是极具潜力的超级电容器电极材料,但是其容量较低。异质原子掺杂,尤其是氮掺杂,是大幅度提高碳材料电化学性能的有效方法。但是在碳材料中实现高含量的活性氮掺杂仍极具挑战。本研究通过Si–O–Si网络和氧化铝之间的相互作用成功... 详细信息

碳材料是极具潜力的超级电容器电极材料,但是其容量较低。异质原子掺杂,尤其是氮掺杂,是大幅度提高碳材料电化学性能的有效方法。但是在碳材料中实现高含量的活性氮掺杂仍极具挑战。本研究通过Si–O–Si网络和氧化铝之间的相互作用成功调节碳材料的掺氮种类及其含量。除此之外,通过调节前驱体组成,碳材料的结构可以从珊瑚状转变为三维结构。在反应中,氧化物中的氧原子可以和碳材料中氮原子成键,氮原子不易逃离,从而实现高含量氮掺杂(5.29at%@1000℃)。另一方面,相互作用使碳材料孔体积增大(1.78 m^(3)·g^(-1))和孔径分布加宽(0.5~60 nm)。因此,获得的富氮掺杂碳材料具有302 F·g^(-1)@1 A·g^(-1)的高容量和177 F·g^(-1)@120 A·g^(-1)的杰出倍率性能。此独特的固氮方法是一种有潜力的制备高性能超级电容器电极材料的策略。

关键词：碳材料氮原子固定相互作用形貌设计超级电容器

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Nitrogen-doped black titania for high performance supercapacitors

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Science China Materials 2020年第7期63卷 1227-1234页

作者： Chongyin Yang Xin Wang wujie dong I-Wei Chen Zhou Wang Jijian Xu Tianquan Lin Hui Gu Fuqiang Huang State Key Laboratory of High Performance Ceramics and Superfine Microstructures Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China Department of Materials Science and Engineering University of PennsylvaniaPennsylvaniaPA 19104-6272USA State Key Laboratory of Rare Earth Materials Chemistry and Applications and National Laboratory College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China College of Chemistry and Molecular Engineering Zhengzhou UniversityZhengzhou 450001China

For energy storage system,it is still a huge challenge to achieve high energy density and high power density *** potential solution is to fabricate electrochemical capacitors(ECs),which store electric energy through surface ion adsorption or redox *** we report a new electrode material,heavy nitrogen-doped(9.29 at.%)black titania(TiO2-x:N).This unique hybrid material,consisting of conductive amorphous shells supported on nanocrystalline cores,has rapid N-mediated redox reaction(TiO2-xNy+zH++ze■-TiO2-xNyHz),especially in acidic solutions,providing a specific capacitance of 750 Fg-1at 2 m V s-1(707 Fg-1at 1 A g-1),great rate capability(503 F g-1at 20 Ag-1),and maintain stable after initial *** a new developed supercapacitor material,nitrogen-doped black titania may revive the oxide-based supercapacitors.

关键词： black titania supercapacitor nitrogen-dopant N-mediated redox reactions

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金属富磷化物储能研究进展与展望

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硅酸盐学报 2023年第6期51卷 1626-1639页

作者：陈文胡克艳董武杰黄富强景德镇陶瓷大学江西景德镇333403 中国科学院上海硅酸盐研究所高性能陶瓷与超细微结构国家重点实验室上海200050

磷基负极材料具有较高的理论容量和中等的氧化还原电位,且原料在储量和成本方面有极大的优势,因此其在钠、锂离子电池负极材料方面具有重要的应用前景。但红磷由于极低的电子电导率和过大的体积膨胀导致电化学活性衰减速度快,循环性能差... 详细信息

磷基负极材料具有较高的理论容量和中等的氧化还原电位,且原料在储量和成本方面有极大的优势,因此其在钠、锂离子电池负极材料方面具有重要的应用前景。但红磷由于极低的电子电导率和过大的体积膨胀导致电化学活性衰减速度快,循环性能差,而黑磷导电性可达105 S/m,结构致密导致其本征倍率性能较差,两者的缺点限制了单质磷作为负极材料的实际应用。通过向单质磷中引入少量金属元素可以形成性质独特的金属富磷化物MPx(x≥2),一方面可以通过金属元素电子注入实现金属富磷化物电子导电性的跨越式提升,另一方面还可以形成较为空旷的晶体结构提供更快的反应动力学并有效地抑制体积膨胀,因此兼具高容量和优异电子/离子输运特性的金属富磷化物MPx是极具潜力的钠、锂离子电池负极材料。主要综述了金属富磷化物材料的组成结构特点,重点阐述金属富磷化物在储能机理和改性策略方面的最新进展。

关键词：金属富磷化物负极材料锂离子电池钠离子电池

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