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High-safety and high-voltage lithium metal batteries enabled by nonflammable diluted highly concentrated electrolyte

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Nano Research 2024年第4期17卷 2638-2645页

作者： Han Zhang Ziqi Zeng Shuping Wang Yuanke Wu Changhao Li mengchuang liu Xinlan Wang Shijie Cheng Jia Xie State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China State Key Laboratory of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan 430074China State Grid Anhui Electric Power Research Institute Anhui Province Key Laboratory of Electric Fire and Safety Protection(State Grid Laboratory of Fire Protection for Transmission and Distribution Facilities)Hefei 230601China School of Chemistry and Chemical Engineering Huazhong University of Science and TechnologyWuhan 430074China

Lithium metal batteries(LMBs)show great promise for achieving energy densities over 400 Wh·kg^(-1).However,highly flammable organic electrolytes are a long-lasting problem that triggers safety hazards and hinders the commercial application of ***,a nonflammable diluted highly concentrated electrolyte(DHCE)with ethoxy(pentafluoro)cyclotriphosphazene(PFPN)as a diluent is developed to simultaneously achieve high safety and cycling stability of high-voltage *** optimal DHCE not only ensures reversible Li deposition/dissolution behavior with a superior average Coulombic efficiency(CE)over 99.1%on lithium metal anode(LMA),but also suppresses side reactions and stress crack on the LiCoO_(2)(LCO)under high cut-off *** newly developed DHCE exhibits high thermal stability,showing complete nonflammability and reduced heat generation between the electrolyte and delithiated LCO/cycled *** work offers an opportunity for rational designing nonflammable electrolytes toward high-voltage and safe LMBs.

关键词： lithium metal batteries thermal stability nonflammable electrolyte high-voltage phosphazene

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Enhanced Dynamic Phase Stability and Suppressed Mn Dissolution in Low-Tortuosity Spinel LMO Electrode

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Energy Material Advances 2022年第1期2022卷 24-32页

作者： Renjie He Sheng Lei mengchuang liu Mingsheng Qin Wei Zhong Shijie Cheng Jia Xie State Key Laboratory of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan 430074P.R.China State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China School of Chemistry and Chemical Engineering Huazhong University of Science and TechnologyWuhan 430074China

Microspinel LiMn_(2)O_(4)(LMO)is a widely used cathode material in power lithium-ion ***,inevitable Mn dissolution and dynamic phase instability will cause the degradation of microspinel LMO during ***,a low-tortuosity LMO(LMO-LT)electrode is fabricated by an ice-templating method,which exhibits enhanced dynamic phase stability,alleviated Mn dissolution,and rare particle microcracks during *** is shown that the low-tortuosity electrode enables fast lithium-ion diffusion and thus small concentration polarization,leading to uniform electrochemical reaction within microregions of the LMO-LT ***,the fast lithium-ion transport kinetics and even mesoscopic scale reactions of the LMO-LT electrode effectively alleviate irreversible phase transition and Mn dissolution as well as suppress crack generation in LMO *** a result,the full cell[negative-to-positive capacity ratio(N/P)=1.1]with thick LMO-LT cathode(13 mg cm^(−2))and Li_(4)Ti_(5)O_(12) anode sustains 80.0%capacity over 200 *** LMO-LT electrode further delivers 78.9%capacity of that at 0.1 C at the high rate of 5 *** work provides an important strategy to enhance dynamic phase stability and suppress Mn dissolution at the mesoscopic scale,promoting the development of high-performance LMO electrodes.

关键词： electrode lithium kinetics

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“In-N-out” design enabling high-content triethyl phosphate-based non-flammable and high-conductivity electrolytes for lithium-ion batteries

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Science China Chemistry 2024年第2期67卷 724-731页

作者： mengchuang liu Fenfen Ma Zicheng Ge Ziqi Zeng Qiang Wu Hui Yan Yuanke Wu Sheng Lei Yanli Zhu Shijie Cheng Jia Xie State Key Laboratory of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan430074China School of Chemistry and Chemical Engineering Huazhong University of Science and TechnologyWuhan430074China GuSu Laboratory of Materials Suzhou215123China Institute of Metal Research Chinese Academy of SciencesShenyang110000China State Key Laboratory of Explosion Science and Technology Beijing Institute of TechnologyBeijing100081China

Safety issues related to flammable electrolytes in lithium-ion batteries(LIBs) remain a major challenge for their extended *** use of non-flammable phosphate-based electrolytes has proved the validity in inhibiting the combustion of ***,the strong interaction between Li^(+) and phosphate leads to a dominant solid electrolyte interphase(SEI) with limited electronic shielding,resulting in the poor Li^(+) intercalation at the graphite(Gr) anode when using high-phosphate-content *** mitigate this issue and improve Li^(+) insertion,we propose an “In-N-Out” strategy to render phosphates “noncoordinative”.By employing a combination of strongly polar solvents for a “block effect” and weakly polar solvents for a “drag effect”,we reduce the Li^(+)–phosphate *** a result,phosphates remain in the electrolyte phase(“In”),minimizing their impact on the incompatibility with the Gr electrode(“Out”).We have developed a non-flammable electrolyte with high triethyl phosphate(TEP) content(>60 wt.%),demonstrating the excellent ion conductivity(5.94 mS cm^(-1) at 30 ℃) and reversible Li^(+) intercalation at a standard concentration(~1 mol L^(-1)).This approach enables the manipulation of multiple electrolyte functions and holds the promise for the development of safe electrochemical energy storage systems using non-flammable electrolytes.

关键词： lithium-ion batteries graphite anode high-phosphate-content electrolytes non-flammable electrolyte excellent ion conductivity standard concentration

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高比能钠离子电池预钠化技术研究进展

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物理化学学报 2023年第3期39卷 27-42页

作者：徐铭礼刘猛闯杨泽洲吴晨钱江锋湖北省化学电源材料与技术重点实验室武汉大学化学与分子科学学院武汉430072

钠离子电池有望取代锂离子电池实现大规模储能应用。然而,储钠负极材料具有较低的初始库伦效率,制约了高比能钠离子电池的开发。预钠化技术被认为是补偿负极活性钠损失、提升电池能量密度的最直接有效的方法,对于钠离子电池的商业化应... 详细信息

钠离子电池有望取代锂离子电池实现大规模储能应用。然而,储钠负极材料具有较低的初始库伦效率,制约了高比能钠离子电池的开发。预钠化技术被认为是补偿负极活性钠损失、提升电池能量密度的最直接有效的方法,对于钠离子电池的商业化应用具有重要意义。本文全面总结近年来预钠化技术的最新研究进展,包括短接法预钠化、电化学预钠化、钠金属物理预钠化、化学预钠化和正极补钠添加剂等,并从反应原理、安全性、可操作性、处理效率和可放大性等角度分析讨论现有各技术方案的优势及面临的挑战;着重介绍化学预钠化和正极补钠添加剂,这两类最具应用前景的预钠化技术的最新成果,进而从实用化角度深入探讨仍待解决的科学问题和技术难点。本文可为预钠化技术的进一步优化和高比能钠离子电池的开发提供思路。

关键词：钠离子电池预钠化技术初始库伦效率化学补钠法正极补钠添加剂

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从废旧电池中直接提取锂实现锂的高效回收

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Science Bulletin 2024年第11期69卷 1697-1705页

作者：刘威刘猛闯马纷纷覃明盛钟伟陈忻曾子琪程时杰谢佳 State Key Laboratory of Advanced Electromagnetic Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan 430074China State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China School of Chemistry and Chemical Engineering Huazhong University of Science and TechnologyWuhan 430074China GuSu Laboratory of Materials Suzhou 215123China Suzhou Laboratory Suzhou 215123China

The flourishing expansion of the lithium-ion batteries(LIBs) market has led to a surge in the demand for lithium resources. Developing efficient recycling technologies for imminent large-scale retired LIBs can significantly facilitate the sustainable utilization of lithium resources. Here, we successfully extract active lithium from spent LIBs through a simple, efficient, and low-energy-consumption chemical leaching process at room temperature, using a solution comprised of polycyclic aromatic hydrocarbons and ether solvents. The mechanism of lithium extraction is elucidated by clarifying the relationship between the redox potential and extraction efficiency. More importantly, the reclaimed active lithium is directly employed to fabricate LiFePO_(4) cathode with performance comparable to commercial materials. When implemented in 56 Ah prismatic cells, the cells deliver stable cycling properties with a capacity retention of ~90% after 1200 cycles. Compared with the other strategies, this technical approach shows superior economic benefits and practical promise. It is anticipated that this method may redefine the recycling paradigm for retired LIBs and drive the sustainable development of industries.

关键词： Retired lithium-ion batteries Lithium recycling Chemical leaching Active lithium Lithium iron phosphate

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Reconfiguring confined magnetic colloids with tunable fluid transport behavior

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National Science Review 2021年第5期8卷 147-157页

作者： Zhizhi Sheng mengchuang Zhang Jing liu Paolo Malgaretti Jianyu Li Shuli Wang Wei Lv Rongrong Zhang Yi Fan Yunmao Zhang Xinyu Chen Xu Hou State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen University Collaborative Innovation Center of Chemistry for Energy Materials Xiamen University Department of Physics Research Institute for Biomimetics and Soft MatterFujian Provincial Key Laboratory for Soft Functional Materials ResearchJiujiang Research InstituteCollege of Physical Science and TechnologyXiamen University Max Planck Institute for Intelligent Systems IV Institute for Theoretical Physics University of Stuttgart Department of Mechanical Engineering McGill University Department of Biomedical Engineering McGill University Tan Kah Kee Innovation Laboratory

Collective dynamics of confined colloids are crucial in diverse scenarios such as self-assembly and phase behavior in materials science, microrobot swarms for drug delivery and microfluidic control. Yet,fine-tuning the dynamics of colloids in microscale confined spaces is still a formidable task due to the complexity of the dynamics of colloidal suspension and to the lack of methodology to probe colloids in confinement. Here, we show that the collective dynamics of confined magnetic colloids can be finely tuned by external magnetic fields. In particular, the mechanical properties of the confined colloidal suspension can be probed in real time and this strategy can be also used to tune microscale fluid transport. Our experimental and theoretical investigations reveal that the collective configuration characterized by the colloidal entropy is controlled by the colloidal concentration, confining ratio and external field strength and direction. Indeed, our results show that mechanical properties of the colloidal suspension as well as the transport of the solvent in microfluidic devices can be controlled upon tuning the entropy of the colloidal suspension. Our approach opens new avenues for the design and application of drug delivery, microfluidic logic, dynamic fluid control, chemical reaction and beyond.

关键词： confined magnetic colloids entropy pressure threshold fluid transport liquid gating technology

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Performance prediction of magnetorheological fluid‐based liquid gating membrane by kriging machine learning method

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Interdisciplinary Materials 2022年第1期1卷 157-169页

作者： mengchuang Zhang Yuan Jing Jian Zhang Zhizhi Sheng Yaqi Hou Jiadai Xu Baiyi Chen Jing liu Miao Wang Xu Hou Department of Physics Research Institute for Biomimetics and Soft MatterFujian Provincial Key Laboratory for Soft Functional Materials ResearchJiujiang Research InstituteCollege of Physical Science and TechnologyXiamen UniversityXiamenChina Institute of Artificial Intelligence Xiamen UniversityXiamenChina School of Civil Aviation Northwestern Polytechnical UniversityXi'anChina Yangtze River Delta Research Institute of Northwestern Polytechnical University Taicang CityJiangsu ProvinceChina State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamenChina Suzhou Institute of Nano-Tech and Nano-Bionics Chinese Academy of SciencesSuzhouChina Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) XiamenChina

Smart liquid gating membrane is a responsive structural material as a pressure-driven system that consists of solid membrane and dynamic liquid,responding to the external *** accurate prediction of rheological and mechanical properties is important for the designs of liquid gating membranes for various ***,high predicted accuracy by the traditional sequential method requires a large amount of experimental data,which is not practical in some *** conquer these problems,artificial intelligence has promoted the rapid development of material science in recent years,bringing hope to solve these *** we propose a Kriging machine learning model with an active candidate region,which can be smartly updated by an expected improvement probability method to increase the local accuracy near the most sensitive search region,to predict the mechanical and rheolo-gical performance of liquid gating system with an active minimal size of ex-perimental *** this,this new machine learning model can instruct our experiments with optimal *** methods are then verified by liquid gating membrane with magnetorheological fluids,which would be of wide interest for the design of potential liquid gating applications in drug release,microfluidic logic,dynamic fluid control,and beyond.

关键词： active candidate region techniques artificial intelligence Kriging machine learning method magnetorheological fluid-based liquid gating membrane rheological and mechanical model

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基于运动学分析的行星滚柱丝杠副应力循环规律

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华南理工大学学报（自然科学版） 2021年第9期49卷 135-144页

作者：姚琴刘永寿马尚君张猛创苏州科技大学机械工程学院江苏苏州215009 西北工业大学力学与土木建筑学院陕西西安710129 西北工业大学陕西省机电传动与控制工程实验室陕西西安710072 西北工业大学民航学院陕西西安710072 西北工业大学长三角研究院江苏太仓215400

行星滚柱丝杠副运动和力的传递是通过多个滚柱在丝杠和螺母之间的行星运动以及螺旋曲面的相互啮合来实现的。文中基于丝杠、螺母和滚柱的空间螺旋曲面特征,采用相应的参数方程建立了行星滚柱丝杠副的运动学分析模型;根据连续相切原理得... 详细信息

行星滚柱丝杠副运动和力的传递是通过多个滚柱在丝杠和螺母之间的行星运动以及螺旋曲面的相互啮合来实现的。文中基于丝杠、螺母和滚柱的空间螺旋曲面特征,采用相应的参数方程建立了行星滚柱丝杠副的运动学分析模型;根据连续相切原理得到了接触点位置,再由接触点的运动特性推导了行星滚柱丝杠副的结构参数关系。在此基础上,模拟了丝杠、螺母和滚柱的空间运动轨迹,进一步得到了零件螺纹牙上的应力循环规律,并对行星滚柱丝杠副的工作寿命进行预测。结果表明:丝杠与滚柱在接触点处具有相对速度,螺母与滚柱的接触点为速度瞬心;滚柱与螺母上每个具体接触点承受着稳定的脉动循环接触应力的作用,而丝杠上每个具体接触点承受着周期性变幅循环接触应力的作用。

关键词：行星滚柱丝杠副空间螺旋曲面运动学分析应力循环

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氮改性ZnO-ZrO_(2)/SBA-15催化剂的酸碱性与其催化乙醇合成1,3-丁二烯反应性能的关系

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化学学报 2024年第5期82卷 493-502页

作者：薛冰关伟鑫王鹏侯少文陈欣辉王奕星苟焕其郭锋浩王梦闯王天姿刘金德郑洲柴寿根陈家锐张建林棘云飞倪珺绿色化学合成技术国家重点实验室培育基地浙江工业大学杭州310014 浙江普康化工有限公司开化324302 嘉兴南洋万事兴化工有限公司嘉兴314201

1,3-丁二烯(以下简称丁二烯)作为化工的重要有机中间体,在石油以及橡胶工业有着广泛的用途.以乙醇为原料生产丁二烯能够解决生产原料不可再生的问题,所以受到越来越多的关注.本工作采用SBA-15为载体,硝酸盐为氧化物前驱体,含氮有机物为... 详细信息

1,3-丁二烯(以下简称丁二烯)作为化工的重要有机中间体,在石油以及橡胶工业有着广泛的用途.以乙醇为原料生产丁二烯能够解决生产原料不可再生的问题,所以受到越来越多的关注.本工作采用SBA-15为载体,硝酸盐为氧化物前驱体,含氮有机物为助剂,通过水热合成法制备了催化剂,并探究了乙醇合成丁二烯反应过程中,乙醇转化率、丁二烯收率与催化剂酸碱性的关系.具体来说,使用三聚氰胺(M)、三聚氰酸(Ma)、1,10-菲啰啉(Pm)、咪唑(Im)和1,3,5-三嗪(St)为含氮助剂,制备了Zn-Zr/SBA-15+X催化剂.通过对催化剂的活性评价,计算得到乙醇脱氢和脱水、乙醛缩合、Meerwein-Ponndorf-Verley(MPV)反应的活性.根据反应活性和丁二烯收率与催化剂酸碱性(酸碱强度和含量)的变化关系,发现适当数量的弱酸(0.022 mmol·g^(-1))、中酸(0.078 mmol·g^(-1))、中碱(0.055 mmol·g^(-1))和强碱(0.056 mmol·g^(-1))有助于乙醇脱氢反应的发生,过量的弱酸和中酸将导致乙醇的脱水反应.中等数量的中酸(0.078 mmol·g^(-1))和中碱(0.055mmol·g^(-1))有利于乙醛缩合和MPV反应的发生.丁二烯收率与乙醛缩合活性和MPV活性关联较大.三聚氰胺改性的催化剂(Zn-Zr/SBA-15+M)的弱酸、中酸、中碱和强碱含量符合以上的最优数量,因此催化性能最优异:乙醇转化率为99.5%,丁二烯选择性为65.5%,丁二烯产能达到了0.45 gBD·g^(-1)cat·h^(-1).

关键词：氮改性 ZnO-ZrO_(2) 酸碱性乙醇丁二烯

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配体缺陷Pd@UiO-66催化乙醇合成正丁醇

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石油学报（石油加工） 2024年第5期40卷 1254-1263页

作者：王栋何耀辉周丹枫关伟鑫何亚军冯启龙王鹏侯少文陈欣辉王奕星苟焕其郭锋浩王梦闯王天姿刘金德倪珺浙江工业大学化学工程学院绿色化学合成技术国家重点实验室培育基地浙江杭州310014

选择乙酸作为调节剂,采用溶剂热合成法制备含有不同配体缺陷数量的UiO-66-xHAc载体,通过浸渍-反应法将金属Pd封装入UiO-66-xHAc中,得到了一系列Pd@UiO-66-xHAc催化剂,考察了其催化乙醇合成正丁醇的反应性能。通过N2物理吸附-脱附、X射... 详细信息

选择乙酸作为调节剂,采用溶剂热合成法制备含有不同配体缺陷数量的UiO-66-xHAc载体,通过浸渍-反应法将金属Pd封装入UiO-66-xHAc中,得到了一系列Pd@UiO-66-xHAc催化剂,考察了其催化乙醇合成正丁醇的反应性能。通过N2物理吸附-脱附、X射线衍射(XRD)、透射电子显微镜(TEM)、氨气程序升温脱附(NH3-TPD)、热重分析(TG)等表征技术,发现改变乙酸用量时,配体缺陷数量会随着乙酸用量的提高而增加,同时催化剂的Lewis酸的强度和数量也随之线性增加。虽然增加乙酸用量能够提升乙醇的转化效率,但是过量的Lewis酸量反而会促进乙醚等副产品的生成。当使用Pd@UiO-66-50HAc催化剂时,在温度为250℃、压力为2 MPa、LHSV为4 h^(-1)的反应条件下,乙醇转化率可以达到60.1%,同时正丁醇的选择性达到40.5%,正丁醇的收率达到24.2%。

关键词：乙醇正丁醇 UiO-66载体配体缺陷 Lewis酸

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