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A closed-loop process for recycling LiNi_xCo_yMn_((1-x-y))O_2 from mixed cathode materials of lithium-ion batteries

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Green Energy & Environment 2017年第1期2卷 42-50页

作者： Rujuan Zheng Wenhui Wang Yunkun dai Quanxin Ma Yuanlong Liu Deying Mu Ruhong Li Jie Rena changsong dai MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of Technology College of Chemistry and Chemical Engineering Qiqihar University College of Animal Science and Veterinary Medicine Jilin University State Key Laboratory of Advanced Chemical Power Sources

With the rapid development of consumer electronics and electric vehicles(EV), a large number of spent lithium-ion batteries(LIBs) have been generated worldwide. Thus, effective recycling technologies to recapture a significant amount of valuable metals contained in spent LIBs are highly desirable to prevent the environmental pollution and resource depletion. In this work, a novel recycling technology to regenerate a LiNi_(1/3)Co_(1/3)Mn_(1/3)O_2 cathode material from spent LIBs with different cathode chemistries has been developed. By dismantling, crushing,leaching and impurity removing, the LiNi_(1/3)Co_(1/3)Mn_(1/3)O_2(selected as an example of LiNi_xCo_yMn_(1-x-y)O_2) powder can be directly prepared from the purified leaching solution via co-precipitation followed by solid-state synthesis. For comparison purposes, a fresh-synthesized sample with the same composition has also been prepared using the commercial raw materials via the same method. X-ray diffraction(XRD), scanning electron microscopy(SEM) and electrochemical measurements have been carried out to characterize these samples. The electrochemical test result suggests that the re-synthesized sample delivers cycle performance and low rate capability which are comparable to those of the freshsynthesized sample. This novel recycling technique can be of great value to the regeneration of a pure and marketable LiNi_xCo_yMn_(1-x-y)O_2 cathode material with low secondary pollution.

关键词： Spent lithium-ion battery Cathode material recycling Acid leaching Purification Co-precipitation

The origins of kinetics hysteresis and irreversibility of monoclinic Li_(3)V_(2)(PO_(4))_(3)

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Journal of Energy Chemistry 2022年第4期31卷 593-603页

作者： Hua Huo Zeyu Lin Guiming Zhong Shuaifeng Lou Jiajun Wang Yulin Ma changsong dai Yueping Xiong Geping Yin Yong Yang Key Laboratory of Materials for New Energy Conversion and Storage(Ministry of Industry and Information Technology) School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001HeilongjiangChina State Key Laboratory for Physical Chemistry of Solid Surface and Department of Chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina Xiamen Institute of Rare Earth Materials Haixi InstitutesChinese Academy of SciencesXiamen 361021FujianChina

Monoclinic Li_(2)V_(2)(PO_(4))_(3);is a promising cathode material with complex charge–discharge *** structural investigation of this compound mainly focuses on local environments;while the reaction kinetics and the driving force of irreversibility of this material remain *** fully understand the above issues,both the equilibrium and the non-equilibrium reaction routes have been systematically investigated in this *** characterization techniques including X-ray diffraction,variable temperature(spinning rate)and ex/in situ ^(7)Li,^(31)P solid state NMR have been employed to provide comprehensive insights into kinetics,dynamics,framework structure evolution and charge ordering,which is essential to better design and application of lithium transition metal phosphate *** results suggest that the kinetics process between the non-equilibrium and the quasi-equilibrium delithiation pathways from Li_(2)V_(2)(PO_(4))_(3);to V_(2)(PO_(4))_(3);is related with a slow relaxation from two-site to one-site *** importantly,it has been demonstrated that the irreversibility in this system is not solely affected by cation and/or charge ordering/disordering,but mainly driven by framework structure distortion.

关键词： NMR spectroscopy Electrochemistry Solid-state structures Kinetics

Performance simulation method and state of health estimation for lithium-ion batteries based on aging-effect coupling model

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Green Energy and Intelligent Transportation 2023年第3期2卷 16-29页

作者： Deyu Fang Wentao Wu Junfu Li Weizhe Yuan Tao Liu changsong dai Zhenbo Wang Ming Zhao School of Automotive Engineering Harbin Institute of TechnologyWeihai 264209ShandongChina School of New Energy Harbin Institute of TechnologyWeihai 264209ShandongChina Guangdong Guanghua Sci-Tech Co. Ltd.Shantou 515000GuangdongChina School of Chemical Engineering and Chemistry Harbin Institute of TechnologyHarbin 150001HeilongjiangChina School of Energy Science and Engineering Harbin Institute of TechnologyHarbin 150001HeilongjiangChina Zhuhai Zhongli New Energy Sci-Tech Co. Ltd.Zhuhai 519000GuangdongChina

Accurate simulation of characteristics performance and state of health(SOH)estimation for lithium-ion batteries are critical for battery management systems(BMS)in electric *** simplified electrochemical model(SEM)can achieve accurate estimation of battery terminal voltage with less computing *** ensure the applica-bility of life-cycle usage,degradation physics need to be involved in SEM *** work conducts deep analysis on battery degradation physics and develops an aging-effect coupling model based on an existing improved single particle(ISP)***,three mechanisms of solid electrolyte interface(SEI)film growth throughout life cycle are analyzed,and an SEI film growth model of lithium-ion battery is built coupled with the ISP ***,a series of identification conditions for individual cells are designed to non-destructively determine model ***,battery aging experiment is designed to validate the battery performance simulation method and SOH estimation *** validation results under different aging rates indicate that this method can accurately es-timate characteristics performance and SOH for lithium-ion batteries during the whole life cycle.

关键词： Improved single particle model Failure physics Characteristics performance simulation State of health estimation

Structural evolution of layered oxide cathodes for spent Li-ion batteries:Degradation mechanism and repair strategy

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SusMat 2023年第3期3卷 362-378页

作者： Shan Jin Jianquan Liang Deying Mu Tianning Lin Yuyang Tian Jian Zhang YueWang Meng Chen Qingmo Shi changsong dai MIIT Key Laboratory of CriticalMaterials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbinChina State Grid Heilongjiang Electric Power Co. Ltd.Electric Power Research InstituteHarbinChina Dongying Cospower Technology Co. Ltd.DongyingChina

Sustainable development has long been recognized as one of the most critical issues in today’s energy and environment-conscious *** has never been more urgent to recycle and reuse the end-of-life cathode ***,this work systematically investigates the structure-critical degradation mechanism of polycrystalline LiNi_(x)Co_(y)Mn_(1−x−y)O_(2)(NCM),combining experimental characterization and DFT *** the key degradation factors,a synergistic repair strategy based on deep mechanochemical activation and heat treatment was successfully proposed to direct regenerate the *** indicate the induction and promotion of synergistic repair technique on the reconstruction of particlemorphology,the recovery of the chemical composition and crystal structure,and the favorable transformation of the impurities phase in the failed *** particular,the synergistic repair process induces a gradient distribution of LiF and further enables partial fluorine doping into the NCM surface,forming abundant oxygen vacancies and increasing the content of highly reactive Ni2+.Benefiting from the comprehensive treatment for the multi-scale and multi-form degradation behaviors,the repaired material exhibits a capacity of 176.8 mA h g^(-1)at 0.1 C,which is comparable to the corresponding commercial material(172.8 mA h g^(-1)).The satisfactory capacity of the recovered cathode proves that it is an effective direct renovating strategy.

关键词： cathode material degradation mechanism impurity phase transformation spent lithium-ion batteries synergistic repair strategy

Mg、F复合掺杂尖晶石LiMg_(0．1)Mn_(1．9)O_(3．95)F_(0．05)的合成和电化学行为研究(英文)

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稀有金属材料与工程 2007年第A03期36卷 182-187页

作者：苏荣军戴长松哈尔滨商业大学黑龙江哈尔滨150076 哈尔滨工业大学黑龙江哈尔滨150001

以己二酸为配位体采用溶胶-凝胶法合成了LiMn_2O_4,Mg掺杂或Mg和F复合掺杂的尖晶石锂镁氧化物正极材料。对合成出的样品采用X-射线衍射仪、X-光电子能谱、扫描显微电子镜、循环伏安测试和充放电测试仪进行了详细的研究。X-射线衍射结果... 详细信息

以己二酸为配位体采用溶胶-凝胶法合成了LiMn_2O_4,Mg掺杂或Mg和F复合掺杂的尖晶石锂镁氧化物正极材料。对合成出的样品采用X-射线衍射仪、X-光电子能谱、扫描显微电子镜、循环伏安测试和充放电测试仪进行了详细的研究。X-射线衍射结果表明,所有的样品都具有相同的纯尖晶石相,LiMg_(0.1)Mn_(1.9)O_4和LiMg_(0.1)Mn_(1.9)O_(3.95)F_(0.05)与LiMn_2O_4的样品相比,具有较小的晶格参数和晶胞体积。X-光电子能谱试验结果表明,在LiMn_2O_4中,Mn^(3+)和Mn^(4+)的相对量分别为50.2%和49.8%,而LiMg_(0.1)Mn_(1.9)O_(3.95)F_(0.05)中Mn^(3+)和Mn^(4+)的相对量分别为48.4%和51.6%。扫描电镜结果显示,LiMg_(0.1)Mn_(1.9)O_(3.95)F_(0.05)颗粒尺寸略小、尺寸分布窄,形态结构更为规整。循环伏安实验显示,Mg和F复合掺杂的尖晶石具有更好的可逆性。LiMn_2O_4,LiMg_(0.1)Mn_(1.9)O_4,LiMg_(0.1)Mn_(1.9)O_(3.95)F_(0.05)样品的首次放电能量和能量保持率分别为123、111、114 mAh·g^(-1)和86.5%、92.3%、90.9%,且LiMg_(0.1)Mn_(1.9)O_4和LiMg_(0.1)Mn_(1.9)O_(3.95)F_(0.05)具有比LiMn_2O_4更高的库仑效率。

关键词：锂离子电池阴极材料 LiMg0.1Mn1.9O3.95F0.05 电化学性能

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泡沫材料的最新研究进展

稀有金属材料与工程 2005年第3期34卷 337-340页

作者：戴长松张亮王殿龙胡信国哈尔滨工业大学黑龙江哈尔滨150001

综述了泡沫铝、泡沫钛、泡沫硅和泡沫铅等材料的制备方法,以及如何控制材料的组成和孔隙率来制备不同性能的材料,重点介绍了这些泡沫材料在汽车工业、人体植入材料、光学材料、微电子、计算机和铅酸电池等方面表现出来的优异性能,并展... 详细信息

综述了泡沫铝、泡沫钛、泡沫硅和泡沫铅等材料的制备方法,以及如何控制材料的组成和孔隙率来制备不同性能的材料,重点介绍了这些泡沫材料在汽车工业、人体植入材料、光学材料、微电子、计算机和铅酸电池等方面表现出来的优异性能,并展望其广阔的市场前景。

关键词：泡沫铝泡沫钛泡沫硅泡沫铅泡沫材料

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光亮剂对化学镀镍层性能及结构的影响

稀有金属材料与工程 2006年第4期35卷 651-654页

作者：戴长松王殿龙袁国辉胡信国哈尔滨工业大学黑龙江哈尔滨150001

研究了酸性化学镀镍溶液的贵金属离子、重金属离子光亮剂对镀层硬度、结合力、孔隙率以及耐蚀性的影响,并通过AFM,XRD和XPS,分析光亮剂对镀层组织结构的影响。结果表明:贵金属离子光亮剂能明显提高EN镀层的耐蚀性,而重金属离子光亮剂降... 详细信息

研究了酸性化学镀镍溶液的贵金属离子、重金属离子光亮剂对镀层硬度、结合力、孔隙率以及耐蚀性的影响,并通过AFM,XRD和XPS,分析光亮剂对镀层组织结构的影响。结果表明:贵金属离子光亮剂能明显提高EN镀层的耐蚀性,而重金属离子光亮剂降低了EN镀层的耐蚀性;两种光亮剂都能降低镀层的表面粗糙度,使构成镀层胞状物变小,并使镀层的非晶结构更加明显,镀态镀层表面Ni以Ni原子和Ni2+离子形式存在,P以负价离子和PO43-离子的形式存在,光亮剂的加入利于镀层表面形成磷酸镍的保护膜。

关键词：化学镀镍光亮剂表面粗糙度原子力显微镜 X光电子能谱

卷绕铅酸电池泡沫铅负极电化学行为的研究(英文)

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稀有金属材料与工程 2007年第A03期36卷 503-509页

作者：戴长松张生王殿龙高丽霞胡信国哈尔滨工业大学应用化学系黑龙江哈尔滨150001

以泡沫铅作为负极集流体制备了卷绕VRLA电池。采用计时电流法、循环伏安曲线、电化学阻抗谱和充放电实验研究了泡沫铅负极的电化学行为,结果表明:泡沫铅负极的真实表面积比铅箔负极的大,因此泡沫铅负极具有较低的过电势,并且不论是在怎... 详细信息

以泡沫铅作为负极集流体制备了卷绕VRLA电池。采用计时电流法、循环伏安曲线、电化学阻抗谱和充放电实验研究了泡沫铅负极的电化学行为,结果表明:泡沫铅负极的真实表面积比铅箔负极的大,因此泡沫铅负极具有较低的过电势,并且不论是在怎样的放电状态下,泡沫铅负极的电化学反应电阻较小;与铅箔负极相比,在10、5和2小时率放电状态下,泡沫铅负极的质量比容量分别增加25.9%,30.0%和48.2%。此外,SEM观察显示,泡沫铅负极表面活性物质为更加细小的晶体颗粒和具有更高的孔率。

关键词：卷绕铅酸电池泡沫铅负极铅箔负极电化学行为

废旧锂离子电池正极材料及电解液的全过程回收及再利用

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化学进展 2020年第7期32卷 950-965页

作者：穆德颖刘铸金珊刘元龙田爽戴长松哈尔滨工业大学化工与化学学院哈尔滨150001 中国科学院宁波材料技术与工程研究所宁波315201 哈尔滨商业大学食品工程学院哈尔滨150076

作为发展势头迅猛的新型储能形式,锂离子电池缓解了能源领域对化石燃料的依赖,同时减轻了日益严峻的环境压力,但是数量巨大的废旧锂离子电池具有危险废弃物和高附加值可用资源的双重属性。因此,通过不同技术手段的创新和组合,实现组成... 详细信息

作为发展势头迅猛的新型储能形式,锂离子电池缓解了能源领域对化石燃料的依赖,同时减轻了日益严峻的环境压力,但是数量巨大的废旧锂离子电池具有危险废弃物和高附加值可用资源的双重属性。因此,通过不同技术手段的创新和组合,实现组成成分日益多样化的废旧锂离子电池的高效回收和再利用具有巨大的挑战和特殊重要的现实意义。本文从预处理工艺出发,详细阐述了放电失活、分类拆解、粉碎筛分、酸浸除杂等一系列过程的技术手段和要求;从原料再生、结构修复以及再制备三个方面探讨了具有代表性的再利用思路,分析了各技术方法的优势和存在的问题。此外,对废旧电解液的无害化处理和回收进行了专题讨论,重点介绍了超临界CO2萃取工艺。最后,针对现阶段存在的问题提出展望,为后续开展废旧锂离子电池回收的相关研究及工业应用提供参考。

关键词：废旧锂离子电池回收再利用预处理材料合成电解液超临界CO2萃取