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progress in Natural Science:Materials International 2024年第2期34卷 338-344页

作者： Yuan li pengfei Huang Chunyu Cui Xiaoyuan Ma li Chen Zekun li linhai li Yuhong Tian School of Biological and Chemical Engineering Guangxi University of Science and Technology School of College of Chemistry and Chemical Engineering Hunan University Isky Future Energy Institute

li metal batteries（LMBs） have attracted much attention due to the ultra-high theoretical capacity of the li metal anode（LMA）.However,the uncontrollable dendrites growth and low coulombic efficiency hinder their practical ***,we explore 3,5-difluoropyridine（2F-BD） as a novel electrolyte additive to enable highperformance *** 2F-BD additive participates in and modifies the solvation structure of li ions by reducing the coordinated number of pF6-at the electrode surface,leading to the formation of a liF and li3N-rich solid electrolyte interphase（SEI）.The liF component increases the robustness of SEI and suppresses the formation of li dendrites,while the li3N component facilitates the transportation and reaction kinetics of li *** a result,the li‖li symmetric cell presents a stable cycling performance of up to 500 h at a current density of 1 mA *** coupling with liFepO4cathode,the obtained full cell achieves high specific capacities of 106.06 mA h g-1and 84.98 mA h g-1at 2.55 mA cm-2and 5.10 mA cm-2,respectively,and maintains a high capacity retention of84.0% after 1000 cycles at 0.13 mA cm-2,with an average cycling CE of 99.58%.

关键词： li metal batteries li dendrites Electrolyte additive

Leaching kinetics of fluorine during the aluminum removal from spent li-ion battery cathode materials

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Journal of Environmental Sciences 2024年第4期138卷 312-325页

作者： Shengjie li Jianxin Zhu Research Center for Eco-Environmental Sciences Chinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China

The high content of aluminum(Al)impurity in the recycled cathode powder seriously affects the extraction efficiency of Nickel,Cobalt,Manganese,and lithium resources and the actual commercial value of recycled materials,so Al removal is crucially important to conform to the industrial standard of spent li-ion battery cathode *** this work,we systematically investigated the leaching process and optimum conditions associated with Al removal from the cathode powder materials collected in a wet cathode-powder peeling and recycling production line of spent li-ion batteries(liBs).Moreover,we specifically studied the leaching of fluorine(F)synergistically happened along with the removal process of Al,which was not concerned about in other studies,but one of the key factors affecting pollution prevention in the recovery *** mechanism of the whole process including the leaching of Al and F from the cathode powder was indicated by using NMR,FTIR,and XpS,and a defluoridation process was preliminarily investigated in this *** leaching kinetics of Al could be successfully described by the shrinking core model,controlled by the diffusion process and the activation energy was 11.14 kJ/***,the leaching of F was attributed to the dissolution of lipF6and decomposition of pVDF,and the kinetics associated was described by Avrami *** interaction of Al and F is advantageous to realize the defluoridation to some *** is expected that our investigation will provide theoretical support for the large-scale recycling of spent liBs.

关键词： Al removal F leaching Cathode powder Heating alkali leaching Leaching kinetics

Orbital pacing and secular evolution of lake-level changes reconstructed by sedimentary noise modeling during the Early Jurassic icehouses-(super)greenhouses

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Science China Earth Sciences 2024年第1期67卷 252-267页

作者： Meng li Xin li Stephen p.HESSELBO Mingjie li Wenjin liU Wei WU Jienan pAN Ruizhen GAO School of Resources and Environment Henan Polytechnic UniversityJiaozuo 454000China Camborne School of Mines and Environment and Sustainability Institute University of ExeterPenryn TR109FEUnited Kingdom Qinghai No.105 Coal Geological Exploration Team Xining 810000China

Lake-level changes can significantly affect paleoenvironmental evolution,resource occurrence,terrestrial carbon budget,and biodiversity in continental *** is one of the most critical factors controlling lake-level *** of the Early Jurassic has been evidenced by oscillating icehouses to(super)greenhouses with interrupted intermittent extreme climatic events(hyperthermal and cooling),e.g.,the Toarcian oceanic anoxic event(~183 Ma)and the late pliensbachian cooling event(~185 Ma).Lake-level evolution and hydrologic cycling on Earth’s surface during the Early Jurassic icehouses-to-(super)greenhouses are thus far poorly understood due to a lack of continuous high-resolution nonmarine *** we present a super-long nonmarine lake level record for this pivotal interval from the early pliensbachian to Toarcian by sedimentary noise modeling,and construct a 16.7-Myr-long astronomical time scale(174.2 Ma to 190.9 Ma)based on cyclostratigraphy analysis of rock color datasets(CIE b*)of the Qaidam *** results document lake-level oscillations on a 5-to 10-million-year(Myr)scale which shows a pronounced correlation with long-term climate variation and extreme climatic events,and 1-to 2.5-Myr-scale lake-level changes that are prominently paced by the 2.4-Myr long-eccentricity forcing and the 1.2-Myr obliquity *** the pliensbachian Stage,the 1.2-Myr-scale lake-level changes are in phase with the coeval sealevel *** forced growth and decay of the ephemeral or permanent ice sheets in polar regions are interpreted to control the synchronous ups-and-downs of continental lake level and global sea ***,during the Toarcian ice-free greenhouses to(super)greenhouses,the 1.2-Myr-scale lake-level variations show an anti-phase relationship with global sea level,indicating a‘seesaw’interaction between continental reservoirs(lakes and groundwater)and global *** 2.4-Myr longeccentricity cycles mainly regulate variation

关键词： Milankovitch cycles Orbital forcing Sedimentary noise model Lake level Continental basins

SEI/dead li-turning capacity loss for high-performance anode-free solid-state lithium batteries

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Journal of Energy Chemistry 2024年第9期96卷 145-152页

作者： Qianwen Yin Tianyu li Hongzhang Zhang Guiming Zhong Xiaofei Yang Xianfeng li Division of Energy Storage Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China Key Laboratory of Long-Duration and Large-Scale Energy Storage Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Laboratory of Advanced Spectro-Electrochemistry and lithium-Ion Batteries Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina

Anode-free solid-state lithium metal batteries(AF-SSLBs)have the potential to deliver higher energy density and improved safety beyond lithium-metal ***,the unclear mechanism for the fast capacity decay in AF-SSLBs,either determined by dead li or solid electrolyte interface(SEI),limits the proposal of effective strategies to prolong cycling *** clarify the underlying mechanism,herein,the evolution of SEI and dead li is quantitatively analyzed by a solid-state nuclear magnetic resonance(ss-NMR)technology in a typical lipF6-based polymer *** results show that the initial capacity loss is attributed to the formation of SEI,while the dead li dominates the following capacity loss and the growth rate is 0.141 mA h cm^(−2)cycle−*** reduce the active li loss,the combination of inorganic-rich SEI and self-healing electrostatic shield effect is proposed to improve the reversibility of li deposition/dissolution behavior,which reduces the capacity loss rate for the initial SEI and following dead li generation by 2.3 and 20.1 folds,*** a result,the initial Coulombic efficiency(ICE)and stable CE increase by 15.1%and 15.3%in li-Cu cells,which guides the rational design of high-performance AF-SSLBs.

关键词： Solid-state lithium batteries Solid-state NMR Anode-free SEI Dead li

performances of fissured red sandstone after thermal treatment with constant-amplitude and low-cycle impacts

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Journal of Rock Mechanics and Geotechnical Engineering 2024年第2期16卷 561-587页

作者： Yongjun Chen Tubing Yin p.G.Ranjith Xibing li Qiang li Dengdeng Zhuang School of Resources and Safety Engineering Central South UniversityChangsha410083China Department of Civil Engineering Monash UniversityMelbourne3800Australia Oulu Mining School University of OuluOuluFI-90014Finland

In the engineering practices,it is increasingly common to encounter fractured rocks perturbed by temperatures and frequent dynamic *** this paper,the dynamic behaviors and fracture characteristics of red sandstone considering temperatures(25℃,200℃,400℃,600℃,and 800℃)and fissure angles(0°,30°,60°,and 90°)were evaluated under constant-amplitude and low-cycle(CALC)impacts actuated by a modified split Hopkinson pressure bar(SHpB)***,fracture morphology and second-order statistics within the grey-level co-occurrence matrix(GLCM)were examined using scanning electron microscopy(SEM).Meanwhile,the deep analysis and discussion of the mechanical response were conducted through the synchronous thermal analyzer(STA)test,numerical simulations,one-dimensional stress wave theory,and material *** multiple regression models between response variables and interactive effects of independent variables were established using the response surface method(RSM).The results demonstrate the fatigue strength and life diminish as temperatures rise and increase with increasing fissure angles,while the strain rate exhibits an inverse ***,the peak stress intensification and strain rate softening observed during CALC impact exhibit greater prominence at increased fissure *** failure is dominated by tensile damage with concise evolution paths and intergranular cracks as well as the compressor-crushed zone which may affect the failure mode after 400℃.The second-order statistics of GLCM in SEM images exhibit a considerable dependence on the ***,thermal damage dominated by thermal properties controls the material structure and wave impedance and eventually affects the incident wave *** tensile wave reflected from the fissure surface is the inherent mechanism responsible for the angle effect exhibited by the fatigue strength and ***,the peak stress intensification and strain rate softening during impact are determ

关键词： Red sandstone Temperature Fissure Constant-amplitude and low-cycle(CALC) impact Fatigue failure Response surface method(RSM)

Theoretical Design of Defects as a Driving Force for Ion Transport in li_(3)OBr Solid Electrolyte

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Energy & Environmental Materials 2024年第3期7卷 143-153页

作者： Xingyun Luo Yanlu li Xian Zhao State Key Lab of Crystal Materials and Institute of Crystal Materials Shandong UniversityJinan 250100China Center for Optics Research and Engineering Shandong UniversityQingdao 266237China

Due to ever-increasing concerns about safety issues in using li ionic batteries,solid electrolytes have extensively *** li-rich antiperovskite li_(3)OBr has been considered as a promising solid electrolyte candidate,but it still suffers challenges to achieve a high ionic conductivity owing to the high intrinsic symmetry of the crystal ***,we presented a design strategy that introduces various point defects and grain boundaries to break the high lattice symmetry of li_(3)OBr crystal,and their effect and microscopic mechanism of promoting the migration of li-ion were explored *** has been found that li_(i)are the dominant defects responsible for the fast li-ion diffusion in bulk li_(3)OBr and its surface,but they are easily trapped by the grain boundaries,leading to the annihilating of the Frenkel defect pair V'_(li)+li_(i),and thus limits the V'_(li)diffusion at the grain *** V_(Br)defect near the grain boundaries can effectively drive V'_(li)across the grain boundary,thereby converting the carrier of li^(+)migration from li,in the bulk and surface to V'_(li)at the grain boundary,and thus improving the ionic conductivity in the whole li_(3)OBr *** work provides a comprehensive insight into the li^(+)transport and conduction mechanism in the li_(3)OBr *** opens a new way of improving the conductivity for all-solid-state li electrolyte material through the defect design.

关键词： defects density functional theory ionic migration solid electrolyte

Highly polar Cop/Co_(2)p heterojunction composite as efficient cathode electrocatalyst for li-air battery

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Chinese Chemical Letters 2024年第9期35卷 486-490页

作者： Miaomiao li Mengwei Yuan Xingzi Zheng Kunyu Han Genban Sun Fujun li Huifeng li Beijing Key Laboratory of Energy Conversion and Storage Materials College of ChemistryBeijing Normal UniversityBeijing 100875China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjin 300071China Center for Advanced Materials Research Beijing Normal UniversityZhuhai 519087China

In order to advance the commercialization of rechargeable li-air batteries,it is of importance to explore cathode catalyst with efficient catalytic *** metal oxides have poor electrical conductivity,while cobalt phosphide has excellent electrical conductivity and large specific surface ***,its application in organic li-air batteries has been much less studied,and the electrocatalytic activity desires to be further ***,Cop/Co_(2)p heterojunction composite with higher polarity was *** discharge product of high-polarity Cop/Co_(2)p had a new porous box-like morphology,which was easy to be decomposed and exposed more active *** highly polar Cop/Co_(2)p heterostructure composite had homogeneous pores,the synergistic effect existed between Cop and Co_(2)p,and the discharge product was porous box mixed with li_(2)O_(2)and liOH,which made Cop/Co_(2)p achieve high specific capacity of14632 m Ah/g and cycle stably 161 times when used as air electrode cathode *** work furnished a thought for the construction of cathode catalysts with efficient catalytic activity for li-air batteries.

关键词： li-air battery Cathode catalyst Cop/Co_(2)p Heterojunction structure High polarity

Synergy effect of regulated li-plating and functional solid electrolyte interphase on graphite anodes

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Nano Research 2024年第9期17卷 8077-8085页

作者： panpan Wang Baojia Xia Jianling li State Key Laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing 100083China Shanghai Institute of Microsystem and Information Technology Chinese Academy of SciencesShanghai 201800China

The growth of li dendrites poses potential safety hazard to lithium-ion batteries(liBs),and eliminating li dendrites thoroughly stills face tough difficulties ***,regulating li-plating is a critical optimization-direction to address the ***,a“graphite-li hybrid”anode with high reversibility is realized under the constant-capacity lithiation(CCL).Within CCL,the uniform distribution of li-plating on the graphite surface is successfully *** evolution in different states of solid electrolyte interphase(SEI)is investigated in detail to study the interaction between the potentials and impedance during the process of liintercalation and *** the potential below 0 V and the state of charge(SOC)of 110%relative to the theoretical capacity,the F-rich SEI with high stability is constructed to hinder the emergency of li dendrites and maintain the intact structure of graphite anode under long *** cell presents more than 100%Coulombic efficiency(CE)with the 900 cycles,demonstrating the reversible li-plating and the utilization of *** the CCL half-cell provides a good cycling performance and specific capacity of 900 cycles at 0.5 C,it is attributed to the synergy effect of stable inorganic-rich SEI and regulated active li-plating.

关键词： "graphite-li hybrid"anode li-plating reversibility solid electrolyte interphase(SEI)

Robust chemo-mechanical stability of additives-free SiO_(2)anode realized by honeycomb nanolattice for high performance li-ion batteries

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Chinese Chemical Letters 2024年第10期35卷 442-446页

作者： Xinpin pan Yongjian Cui Zhe Wang Bowen li Hailong Wang Jian Hao Feng li Jing li Advanced Energy Storage Materials Lab School of Materials and New EnergyNingxia UniversityYinchuan 750021China School of Chemistry and Chemical Engineering Ningxia UniversityYinchuan 750021China

Silicon-based anodes including Si,Si Oxand SiO_(2)could deliver ultra-large capacities,but degrade fast owing to huge volume change and low ***,large amounts of elastic binder and conductive additives were composited with nanosized silicon-based materials to yield reasonable cycling stability,which nevertheless not only decrease specific capacity but also induce inhomogeneous lithiation/delithiation as well as uneven stress *** nanolattice has exhibited superior mechanical properties which could be ideal structure for silicon-based anodes,but yet faces challenges in integration of chemical reactivity,conductivity and mechanical ***,we fabricate artificial SiO_(2)honeycomb nanolattice consisting of numerous nanoscale SiO_(2)cells interconnected by through-holes,and conformal coating of highly graphitic carbon on the nanolattice is achieved through in situ catalytic ***,the nanolattice is firmly bonded on Cu substrate through atomic interdiffusion irrespective of surface *** unique structure allows fast charge transportation and homogeneous lithiation/delithiation throughout the micron-meter nanolattice,which results in excellent stability and large reversible capacity over 500 cycles at 1 A/*** results highlight design and constructing artificial nanolattice can be an effective way to prevent chemo-mechanical degradation of silicon-based anode materials.

关键词： li-ion batteries Nanolattice SiO_(2)anode Stability Conductivity

Combining cisplatin and a STING agonist into one molecule for metalloimmunotherapy of cancer

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National Science Review 2024年第1期11卷 107-119页

作者： Shuren Zhang Dongfan Song Wenhao Yu Ji li Xiaoyu Wang Yachao li Zihan Zhao Qi Xue Jing Zhao Jie p.li Zijian Guo State Key Laboratory of Coordination Chemistry School of Chemistry and Chemical EngineeringChemistry and Biomedicine Innovation Center (ChemBIC) Nanjing University Department of Urology Afflliated Drum Tower HospitalMedical SchoolNanjing University Nanchuang (Jiangsu)Institute of Chemistry and Health

Mounting evidence suggests that strategies combining DNA-damaging agents and stimulator of interferon genes(STING) agonists are promising cancer therapeutic regimens because they can amplify STING activation and remodel the immunosuppressive tumor microenvironment. However, a single molecular entity comprising both agents has not yet been developed. Herein, we designed two ptIV-MSA-2 conjugates(Ⅰand Ⅱ) containing the DNA-damaging chemotherapeutic drug cisplatin and the innate immuneactivating STING agonist MSA-2; these conjugates showed great potential as multispecific small-molecule drugs against pancreatic cancer. Mechanistic studies revealed that conjugate Ⅰ upregulated the expression of transcripts associated with innate immunity and metabolism in cancer cells, significantly differing from cisplatin and MSA-2. An analysis of the tumor microenvironment demonstrated that conjugate I could enhance the infiltration of natural killer(NK) cells into tumors and promote the activation of T cells, NK cells and dendritic cells in tumor tissues. These findings indicated that conjugate I, which was created by incorporating a pt chemotherapeutic drug and STING agonist into one molecule, is a promising and potent anticancer drug candidate, opening new avenues for small-molecule-based cancer metalloimmunotherapy.

关键词： platinum drug STING agonist single-molecule multitarget metalloimmunology