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Electrolyte Design for low‑temperature Li‑Metal Batteries:Challenges and Prospects

Nano-Micro Letters 2024年第2期16卷 365-382页

作者： Siyu Sun Kehan Wang Zhanglian Hong Mingjia Zhi Kai Zhang Jijian Xu Department of Chemistry City University of Hong KongHong Kong 999077People’s Republic of China State Key Laboratory of Silicon Materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China State Key Laboratory of Advanced Chemical Power Sources Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)Haihe Laboratory of Sustainable Chemical TransformationsCollaborative Innovation Center of Chemical Science and Engineering(Tianjin)College of ChemistryNankai UniversityTianjin 300071People’s Republic of China Department of Chemical and Biomolecular Engineering University of Maryland College ParkCollege ParkMD 20742USA

Electrolyte design holds the greatest opportunity for the development of batteries that are capable of sub-zero temperature operation.To get the most energy storage out of the battery at low temperatures,improvements in electrolyte chemistry need to be coupled with optimized electrode materials and tailored electrolyte/electrode interphases.Herein,this review critically outlines electrolytes’limiting factors,including reduced ionic conductivity,large de-solvation energy,sluggish charge transfer,and slow Li-ion transportation across the electrolyte/electrode interphases,which affect the low-temperature performance of Li-metal batteries.Detailed theoretical derivations that explain the explicit influence of temperature on battery performance are presented to deepen understanding.Emerging improvement strategies from the aspects of electrolyte design and electrolyte/electrode interphase engineering are summarized and rigorously compared.Perspectives on future research are proposed to guide the ongoing exploration for better low-temperature Li-metal batteries.

关键词： Solid electrolyte interphase Li metal low temperature Electrolyte design Batteries

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Alkyl dimethyl betaine activates the low-temperature collection capacity of sodium oleate for scheelite

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International Journal of Minerals,Metallurgy and Materials 2024年第1期31卷 71-80页

作者： Xu Wang Zhengquan Zhang Yanfang Cui Wei Li Congren Yang Hao Song Wenqing Qin Fen Jiao School of Minerals Processing and Bioengineering Central South UniversityChangsha 410083China Key Laboratory of Hunan Province for Clean and Efficient Utilization of Strategic Calcium-containing Mineral Resources Central South UniversityChangsha 410083China College of Engineering Drexel UniversityPhiladelphiaPA 19102USA Luoyang Zhenbei Industry and Trade Co. Ltd.Luoyang 47100China

The impact of alkyl dimethyl betaine (ADB) on the collection capacity of sodium oleate (NaOl) at low temperatures was evaluated using flotation tests at various scales. The low-temperature synergistic mechanism of ADB and NaOl was explored by infrared spectroscopy, X-ray photoelectron spectroscopy, surface tension measurement, foam performance test, and flotation reagent size measurement.The flotation tests revealed that the collector mixed with octadecyl dimethyl betaine (ODB) and NaOl in a mass ratio of 4:96 exhibited the highest collection capacity. The combined collector could increase the scheelite recovery by 3.48% at low temperatures of 8–12℃. This is particularly relevant in the Luanchuan area, which has the largest scheelite concentrate output in China. The results confirmed that ODB enhanced the collection capability of NaOl by improving the dispersion and foaming performance. Betaine can be introduced as an additive to NaOl to improve the recovery of scheelite at low temperatures.

关键词： scheelite betaine low temperature synergistic effect dispersion foamability

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Introducing cerium into TiO_(2)@MnO_(x) hollow-sphere structure for highly active photothermocatalysis degradation of ethyl acetate and NO under H_(2)O at low temperature

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Journal of Rare Earths 2024年第5期42卷 889-898,I0003页

作者： Yinming Fan Yanhong Wang Morui Li Yinian Zhu Zongqiang Zhu Shengpeng Mo Lihao Zhang Shen Tang Xiaobin Zhou Yanping Zhang Collaborative Innovation Center for Water Pollution Control and Water Safety in Karst Area Guilin University of TechnologyGuilin541004China The Guangxi Key Laboratory of Theory and Technology for Environmental Pollution Control.Guilin University of Technology.Guilin 541004China Technical Innovation Center of Mine Geological Environmental Restoration Engineering in Southern Karst Area Nanning530022China

The CeO_(2)-TiO_(2)@MnO_(x) catalyst was prepared by the co-precipitation method and applied to the photothermocatalysis system of ethyl acetate and NO simultaneous degradation under H_(2)O at low temperature,which introduced Ce into TiO_(2)@MnO_(x) hollow sptrera structure.The optimum TiO_(2)/MnO_(x) ratio and Ce introducing amount were obtained in the process.Among of them,the NO and ethyl acetate conversion percentage of TiO_(2)@MnO_(x)(n_(Mn):n_(Ti)=40:40)is 74%and 62%at 240℃,respectively.CeO_(2)-TiO_(2)@MnO_(x)(n_(Mn):n_(Ce)=1:1)exhibits the best catalytic performance,its efficiency for NO conversion is 83%and the conversion of ethyl acetate reaches 72%at 240℃.In addition,it is confirmed that the Cedoped nanocomposites have more uniform dispersion through various characterization and analysis methods.Meanwhile,these catalysts have a large specific surface area as well as a large number of surface-active oxygen and oxygen vacancies.It can further improve the catalytic performance based on the adjusted ratio of active components.Moreover,this work investigated the relationship between multi-metal interactions and catalytic performance in the presence of H_(2)O.Finally,the possible reaction pathways for the simultaneous removal of NO and ethyl acetate were explored in our system.

关键词： Photothermocatalysis Ethyl acetate NO low temperature H_(2)O Rare earths

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An effective'salt in dimethyl sulfoxide/water'electrolyte enables high-voltage supercapacitor operated at-50℃

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Journal of Energy Chemistry 2024年第6期93卷 361-367,I0009页

作者： Yingbin Liu Chang Yu Xuedan Song Siyi Hou Shuqin Lan Jinhe Yu Yuanyang Xie Jieshan Qiu State Key Lab of Fine Chemicals Frontier Science Center for Smart MaterialsSchool of Chemical EngineeringLiaoning Key Lab for Energy Materials and Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina School of Chemistry Frontier Science Center for Smart MaterialsLiaoning Key Lab for Energy Materials and Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina College of Chemical Engineering State Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Compared with organic electrolytes,aqueous electrolytes exhibit significantly higher ionic conductivity and possess inherent safety features,showcasing unique advantages in supercapacitors.However,challenges remain for low-salt aqueous electrolytes operating at high voltage and low temperature.Herein,we report a low-salt(0.87 m,m means mol kg^(-1))'salt in dimethyl sulfoxide/water'hybrid electrolyte with non-flammability via hybridizing aqueous electrolyte with an organic co-solvent of dimethyl sulfoxide(hydrogen bond acceptor).As a result,the 0.87 m hybrid electrolyte exhibits enhanced electrochemical stability,a freezing temperature below-50℃,and an outstanding ionic conductivity of 0.52mS cm~(-1)at-50℃.Dimethyl sulfoxide can anchor water molecules through intermolecular hydrogen bond interaction,effectively reinforcing the stability of water in the hybrid electrolyte.Furthermore,the interaction between dimethyl sulfoxide and water molecules diminishes the involvement of water in the generation of ordered ice crystals,finally facilitating the low-temperature performance of the hybrid electrolyte.When paired with the 0.87 m'salt in dimethyl sulfoxide/water'hybrid electrolyte,the symmetric supercapacitor presents a 2.0 V high operating voltage at 25℃,and can operate stably at-50℃.Importantly,the suppressed electrochemical reaction of water at-50℃further leads to the symmetric supercapacitor operated at a higher voltage of 2.6 V.This modification strategy opens an effective avenue to develop low-salt electrolytes for high-voltage and low-temperature aqueous supercapacitors.

关键词： Dimethyl sulfoxide Co-solvent High voltage low temperature Supercapacitors

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Structure and defect dual-engineering of cobalt oxides for lowtemperature Zn-air batteries

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Nano Research 2024年第5期17卷 4108-4117页

作者： Hang Lei Zhuowen Huangfu Liangjun Chen Xuelin Yang Zilong Wang Wenjie Mai Hubei Provincial Collaborative Innovation Center for New Energy Microgrid College of Electrical Engineering&New EnergyChina Three Gorges UniversityYichang 443002China Siyuan Laboratory Guangdong Provincial Engineering Technology Research Center of Vacuum Coating Technologies and New Energy MaterialsDepartment of PhysicsJinan UniversityGuangzhou 510632China

The exploration of bifunctional electrocatalysts with high catalytic activity and long-term durability for low-temperature Zn-air batteries(ZABs)is an ongoing challenge.Here,quintet-shelled hollow spheres,P-doped multi-layer Co_(3)O_(4)(PM-Co_(3)O_(4)),with enriched oxygen vacancies are prepared by thermally induced mass relocation and a simple phosphating process.Various advanced characterizations reveal P anion-induced effects on internal electronic structure and local coordination environment.The finite element method elucidates that the complex multi-layer spherical nanostructure is conducive to the transport and diffusion of OH-and O_(2).Benefiting from its unique structural features and abundant oxygen vacancies,the well-designed PM-Co_(3)O_(4) presents small reversible oxygen overpotential for catalyzing oxygen reduction/evolution reactions.Accordingly,the fabricated low-temperature ZABs based on PM-Co_(3)O_(4) as air-cathode exhibit high power density(20.8 mW·cm^(-2))and long-term stability(over 600 cycles)at the ultra-low temperature of-40℃,outperforming state-of-art Pt/C+IrO_(2)-based ZABs.Furthermore,the dynamic evolution mechanism of cobalt oxide catalysts during ZAB operation is elucidated.This work provides a guideline to design efficient electrocatalysts with regulated electronic configurations and exquisite nano-/microstructures for ZABs under extreme working conditions.

关键词： Zn-air batteries electrocatalysts low temperature hollow spheres oxygen vacancies

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Simultaneous removal of sulfur dioxide and nitrogen oxide from flue gas by phosphorus sludge:The performance and absorption mechanism

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Chinese Journal of Chemical Engineering 2024年第1期65卷 212-221页

作者： Yuanyuan Yin Xujun Wang Lei Xu Binbin He Yunxiang Nie Yi Mei Faculty of Chemical Engineering Kunming University of Science and TechnologyKunming 650500China Yunnan Provincial Key Laboratory of Energy Saving in Phosphorus Chemical Engineering and New Phosphorus Materials Kunming 650500China The Higher Educational Key Laboratory for Phosphorus Chemical Engineering of Yunnan Province Kunming 650500China

Developing low-cost and green simultaneous desulfurization and denitrification technologies is of great significance for sulfur dioxide(SO_(2))and nitrogen oxide(NO_(x))emission control at low temperatures,especially for small and medium-sized coal-fired boilers and furnaces.Herein,phosphorus sludge,an industrial waste from the production process of yellow phosphorus,has been developed to simultaneously eliminate SO_(2)and NO_(x)from coal-fired flue gas.The key factors affecting the experimental results indicate that desulfurization and denitrification efficiency of over 95%can be achieved at a low temperature of 55℃.Further,the absorption mechanism was investigated by characterizing the solid and liquid phases of the phosphorus sludge during the absorption process.The efficient removal of SO_(2)is attributed to the abundance of iron(Fe^(3+))and manganese(Mn^(2+))in the absorbent.SO_(2)can be rapidly catalyzed and converted to SO_(4)^(2-)by them.The key to NOx removal is the oxidation of NO toward watersoluble high-valent nitrogen oxides by oxidizing reactive substances induced via yellow phosphorus,which are then absorbed by water and converted to NO_(3)^(-).Meanwhile,yellow phosphorus is oxidized to phosphoric acid(H_(3)PO_(4)).The spent absorption slurry can be reused through wet process phosphoric acid production,as it contains sulfuric acid(H_(2)SO_(4)),nitric acid(HNO_(3)),and H_(3)PO_(4).Accordingly,this is a technology with broad application prospects.

关键词： Absorption Oxidation Multiphase reaction Phosphorus sludge Yellow phosphorus low temperature

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low-temperature caproate production,microbial diversity,and metabolic pathway in xylose anaerobic fermentation

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Frontiers of Environmental Science & Engineering 2023年第3期17卷 121-130页

作者： Qingting Wang Kun Dai Jie Tang Sidi Hong Sijie Zheng Ting Sun Raymond Jianxiong Zeng Fang Zhang Center of Wastewater Resource Recovery College of Resources and EnvironmentFujian Agriculture and Forestry UniversityFuzhou 350002China

Mixed culture fermentation(MCF)is challenged by the unqualified activity of enriched bacteria and unwanted methane dissolution under low temperatures.In this work,caproate production from xylose was investigated by MCF at a low temperature(20°C).The results showed that a 9 d long hydraulic retention time(HRT)in a continuously stirred tank reactor was necessary for caproate production(~0.3 g/L,equal to 0.6 g COD/L)from xylose(10 g/L).The caproate concentration in the batch mode was further increased to 1.6 g/L.However,changing the substrate to ethanol did not promote caproate production,resulting in~1.0 g/L after 45 d of operation.Four genera,Bifidobacterium,Caproiciproducens,Actinomyces,and Clostridium_sensu_stricto_12,were identified as the enriched caproate-producing bacteria.The enzymes in the fatty acid biosynthesis(FAB)pathway for caproate production were identified via metagenomic analysis.The enzymes for the conversion of(C_(n+2))-2,3-Dehydroxyacyl-CoA to(C_(n+2))-Acyl-CoA(i.e.,EC 1.***.1.8 and EC 1.***.1.38)in the reverseβ-oxidation(RBO)pathway were not identified.These results could extend the understanding of low-temperature caproate production.

关键词： Xylose fermentation Caproate low temperature Bifidobacterium FAB pathway RBO pathway

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low-temperature Li-S batteries enabled by all amorphous con version process of organosulfur cathode

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Journal of Energy Chemistry 2022年第1期31卷 496-502,I0013页

作者： Zhenkang Wang Xiaowei Shen Sijie Li Yuxuan Wu Tingzhou Yang Jie Liu Tao Qian Chenglin Yan College of Energy Key Laboratory of Advanced Carb on Materials and Wearable Energy Technologies of Jiangsu ProvinceSoochow UniversitySuzhou 215006JiangsuChina College of Chemistry and Chemical Engineering.Nantong University Seyuan 9Nantong 226000JiangsuChina

The high degree of crystallinity of discharging in termediates of Li-S batteries(Li_(2)S_(2)/Li_(2)S)causes a severe capacity attenuation at low temperatures.Herein,a sulfur-rich polymer is fabricated,which enables all the discharging in termediates to exist in an amorphous state without long-range order,promoti ng the substantial conversion of discharging intermediates and enhancing Li-S batteries'performance at low temperatures greatly.This cathode material exhibits excellent performance both at room and low temperatures.Even under an extremely low temperature(-40℃),the discharge capacity can remain 67% of that at room temperature.Besides,in-situ UV/Vis spectroscopy and density functional theory calculations reveal that this organosulfur cathode undergoes a new mechanism during discharge.Li_(2)S_(6) and Li_(2)S_(3) are the primary discharging intermediates that are quite different from conventional Li-S batteries.These results provide a new directi on for a broader range of applications of Li-S batteries.

关键词： low temperature Organosulfur polymers Li-S battery Crystallinity

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low-temperature and high-voltage planar micro-supercapacitors based on anti-freezing hybrid gel electrolyte

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Journal of Energy Chemistry 2022年第9期31卷 195-202,I0006页

作者： Manning Chen Xiaoyu Shi Xiaolei Wang Hanqing Liu Sen Wang Caixia Meng Yu Liu Liangzhu Zhang Yuanyuan Zhu Zhong-Shuai Wu College of Chemistry and Environment Shenyang University of TechnologyShenyang 110870LiaoningChina State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China Dalian National Laboratory for Clean Energy Chinese Academy of SciencesDalian 116023LiaoningChina

Micro-supercapacitors(MSCs)are considered as highly competitive power sources for miniaturized electronics.However,narrow voltage window and poor anti-freezing properties of MSCs in conventional aqueous electrolytes lead to low energy density and limited environmental adaption.Herein,we report the construction of low-temperature and high-energy-density MSCs based on anti-freezing hybrid gel electrolytes(HGE)through introducing ethylene glycol(EG)additives into aqueous LiCl electrolyte.Since EG partially destroys hydrogen bond network among water molecules,the HGE exhibits maximum electrochemical stability window of 2.7 V and superior anti-freezing features with a glass transition temperature of-62.8℃.Further,the optimized MSCs using activated carbon microelectrodes possess impressive volumetric capacitance of 28.9 F cm^(-3)and energy density of 10.3 mWh cm^(-3)in the voltage of 1.6 V,2.6 times higher than MSCs tested in 1.2 V.Importantly,the MSCs display 68.3%capacitance retention even at-30℃ compared to the value at 25℃,and ultra-long cyclability with 85.7%of initial capacitance after 15,000 times,indicating extraordinary low-temperature performance.Besides,our devices offer favorable flexibility and modular integration.Therefore,this work provides a general strategy of realizing flexible,safe and anti-freezing microscale power sources,holding great potential towards subzero-temperature microelectronic applications.

关键词： Hybrid gel electrolyte Micro-supercapacitors low temperature High voltage Graphene

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Mobile ARGONAUTE 1d binds 22-nt miRNAs to generate phasiRNAs important for low-temperature male fertility in rice

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Science China(Life Sciences) 2023年第2期66卷 197-208页

作者： Fuyan Si Haofei Luo Chao Yang Jie Gong Bin Yan Chunyan Liu Xianwei Song Xiaofeng Cao State Key Laboratory of Plant Genomics and National Center for Plant Gene Research Institute of Genetics and Developmental BiologyChinese Academy of SciencesBeijing 100101China The Municipal Key Laboratory of the Molecular Genetics of Hybrid Wheat Institute of Hybrid WheatBeijing Academy of Agriculture and Forestry SciencesBeijing 100097China Innovative Academy of Seed Design(INASEED) Institute of Genetics and Developmental BiologyChinese Academy of SciencesBeijing 100101China College of Life Sciences University of the Chinese Academy of SciencesBeijing 100039China CAS Center for Excellence in Molecular Plant Sciences Chinese Academy of SciencesBeijing 100101China

Phased small interfering RNAs(phasiRNAs) are abundantly expressed in anthers and linked to environment-related male fertility in grasses, yet how they function under different environmental conditions remains unclear. Here, we identified a rice(Oryza sativa) low temperature-induced Argonaute(AGO) protein, OsAGO1d, that is responsible for generating phasiRNAs and preserving male fertility at low temperature. Loss of OsAGO1d function causes low-temperature male sterility associated with delayed programmed cell death of tapetal cells during anther development. OsAGO1d binds miR2118 and miR2275 family members and triggers phasiRNA biogenesis;it also binds 21-nt phasiRNAs with a 5′ terminal U. In total, phasiRNAs from 972loci are OsAGO1d-dependent. OsAGO1d protein moves from anther wall cells into meiocytes, where it loads miR2275 to produce 24-nt phasiRNAs. Together, our results show that OsAGO1d acts as a mobile signal to fine-tune phasiRNA production and this function is important for male fertility at low temperature.

关键词： mobile signal ARGONAUTE 22-nt miRNA phasiRNA low temperature male sterility rice

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