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application of surfactant for improving leaching process of weathered crust elution-deposited rare earth ores

Journal of Rare Earths 2024年第1期42卷 181-190,I0007页

作者： Fang Zhou Lisen Zhang Zhiwei Wang Yixin Zhang Ru'an Chi Xiaoyan Wu Key Laboratory for Green chemical Process of Ministry of Education Wuhan Institute of TechnologyWuhan430073China

Weathered crust elution-deposited rare earth ores(WREOs)in China are the main source of medium and heavy rare earths in the world.In order to improve the seepage and the mass transfer of traditional ammonium salt leaching process of WREOs,surfactants were added in the ammonium sulfate leaching solution and the ammonium chloride leaching solution.The leaching kinetics,the mass transfer process,and the adhesion work reduction factor calculated from the interfacial properties were studied to reveal the strengthening mechanism of surfactant.In the presence of the tested five surfactants,cetyl trimethyl ammonium bromide(CTAB),dodecyl trimethyl ammonium bromide(DTAB),sodium dodecyl sulfate(SDS),sodium oleate and oleic acid,the permeability of WREOs is improved,the rare earth(RE)leaching efficiency increase and the impurity aluminum(Al)leaching efficiency decrease,indicating its promotional effect on the leaching process of WREOs.Furthermore,CTAB shows a better leaching enhancement,and the optimal addition dosage is 0.4 g/L for the two ammonium salt leaching agent systems.The kinetics analysis shows the internal diffusion controls model of RE and Al leaching process,and the leaching kinetics equations of RE and Al related to CTAB concentration were obtained for the two ammonium salt leaching systems.According to the chromatographic plate theory,the mass transfer efficiency of RE increases with the CTAB concentration increasing until 0.4 g/L,which confirms that the optimal CTAB addition is 0.4 g/L.Smaller adhesion work and adhesion work reduction factor indicate more favorable permeation as well as the leaching process.

关键词： Weathered crust elution-deposited rare earth ores Surfactant Kinetics Mass transfer

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Design method of extractant for liquideliquid extraction based on elements and chemical bonds

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Chinese Journal of chemical Engineering 2024年第4期68卷 193-202页

作者： Yuwen Wei Chunling Zhang Yue Zhang Lili Wang Li Xia Xiaoyan Sun Shuguang Xiang institute of Process System Engineering College of Chemical EngineeringQingdao University of Science and TechnologyQingdao 266042China Yantai Guobang chemical Machinery technology Co. Ltd.Yantai 264002China

In the petrochemical industry process,the relative volatility between the components to be separated is close to one or the azeotrope that systems are difficult to separate.Liquideliquid extraction is a common and effective separation method,and selecting an extraction agent is the key to extraction technology research.In this paper,a design method of extractants based on elements and chemical bonds was proposed.A knowledge-based molecular design method was adopted to pre-select elements and chemical bond groups.The molecules were automatically synthesized according to specific combination rules to avoid the problem of“combination explosion”of molecules.The target properties of the extractant were set,and the extractant meeting the requirements was selected by predicting the correlation physical properties of the generated molecules.Based on the separation performance of the extractant in liquideliquid extraction and the relative importance of each index,the fuzzy comprehensive evaluation membership function was established,the analytic hierarchy process determined the mass ratio of each index,and the consistency test results were passed.The results of case study based on quantum chemical analysis demonstrated that effective determination of extractants for the analysis of benzeneecyclohexane systems.The results unanimously prove that the method has important theoretical significance and application value.

关键词： Molecular design Element and chemical bonds Molecular simulation Thermodynamics Solvent extraction

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A review of solid-state lithium metal batteries through in-situ solidification

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Science China Chemistry 2024年第1期67卷 67-86页

作者： Pan Xu Zong-Yao Shuang Chen-Zi Zhao Xue Li Li-Zhen Fan Aibing Chen Haoting Chen Elena Kuzmina Elena Karaseva Vladimir Kolosnitsyn Xiaoyuan Zeng Peng Dong Yingjie Zhang Mingpei Wang Qiang Zhang Beijing Key Laboratory of Green chemical Reaction Engineering and technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China National and Local Joint Engineering Laboratory for Lithium-ion Batteries and Materials Preparation technology Key Laboratory of Advanced Battery Materials of Yunnan ProvinceFaculty of Metallurgical and Energy EngineeringKunming University of Science and TechnologyKunming 650093China institute of Advanced Materials and technology University of Science and Technology BeijingBeijing 100083China College of chemical and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuang 050018China Ordos Carbon Neutral Research and application Co. Ltd.Ordos City 017010China Ufa institute of Chemistry UFRC RAS Ufa 450054Russia institute for Carbon Neutrality Tsinghua UniversityBeijing 100084China Shanxi Research institute for Clean Energy Tsinghua UniversityTaiyuan 030032China

High-energy-density lithium metal batteries are the next-generation battery systems of choice,and replacing the flammable liquid electrolyte with a polymer solid-state electrolyte is a prominent conduct towards realizing the goal of high-safety and high-specific-energy devices.Unfortunately,the inherent intractable problems of poor solid-solid contacts between the electrode/electrolyte and the growth of Li dendrites hinder their practical applications.The in-situ solidification has demonstrated a variety of advantages in the application of polymer electrolytes and artificial interphase,including the design of integrated polymer electrolytes and asymmetric polymer electrolytes to enhance the compatibility of solid–solid contact and compatibility between various electrolytes,and the construction of artificial interphase between the Li anode and cathode to suppress the formation of Li dendrites and to enhance the high-voltage stability of polymer electrolytes.This review firstly elaborates the history of in-situ solidification for solid-state batteries,and then focuses on the synthetic methods of solidified electrolytes.Furthermore,the recent progress of in-situ solidification technology from both the design of polymer electrolytes and the construction of artificial interphase is summarized,and the importance of in-situ solidification technology in enhancing safety is emphasized.Finally,prospects,emerging challenges,and practical applications of in-situ solidification are envisioned.

关键词： in-situ solidification polymer electrolyte artificial solid electrolyte interphase rechargeable lithium metal batteries dendrite-free lithium metal anode

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Enhanced cyclic stability of partially disordered spinel cathodes through direct fluorination with gaseous fluorine

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Rare Metals 2024年第4期43卷 1635-1646页

作者： Yong-Nian Ma Ling-Chen Kong Shao-Shan Chen Yong Wang Li-Dong Sun Cong Peng Meng-Meng Qin Yu Li Wei Feng Tianjin Key Laboratory of Composite and Functional Materials School of Materials Science and EngineeringTianjin University institute of Advanced technology and Equipment Beijing University of Chemical Technology

Spinel-type cathodes are considered an optimal substitute for conventional layered oxide cathodes owing to their use of inexpensive and earth-abundant manganese as the redox-active element.Moreover,the introduction of cation disorder can effectively suppress the detrimental two-phase reaction to realize high capacities in a wide voltage range.However,the continuous capacity decay during cycles has hindered the widespread application of these cathode materials.Inorganic fluorides exhibit excellent electrochemical stability at high voltage;therefore,in this study,the direct F2 gas reaction with a partially disordered spinel cathode(Li1.6Mn1.6O3.7F0.3,LMOF1.6) was initially applied to investigate the impacts of fluorination on the surface structure and electrochemical performances.The inorganic fluorinated layer,mainly containing LiF,was distributed uniformly on the surface of LMOF1.6nanoparticles after fluorination for an appropriate time without the turbulence caused by the valency of manganese cation,which improved the capacity retention and rate capability by the suppression of structural damage,parasitic reaction,and cation dissolution.The LMOF1.6cathode fluorinated for 0.5 h exhibited a capacity of283.6 mAh·g-1at 50 mA·g-1and an enhanced capacity retention of 29.6% after 50 cycles in the voltage range of1.5-4.8 V,as compared to the pristine LMOF1.6 with only27.9% capacity retention.

关键词： Spinel-type cathodes Direct fluorination Capacity retention ability High rate capability

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Additives strategies to improving cycling stability of Li metal batteries by modifying electrode electrolyte interphases

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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 application.Here,we explore 3,5-difluoropyridine（2F-BD） as a novel electrolyte additive to enable highperformance LMBs.The 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 ions.As a result,the Li‖Li symmetric cell presents a stable cycling performance of up to 500 h at a current density of 1 mA cm-2.After 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： Electrolyte additive Li dendrites Li metal batteries LiF and Li3N-Rich electrode-electrolyte interphase LiFePO4 cathode

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Modulated noble metal/2D MOF heterostructures for improved hydrogen storage of MgH2

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Rare Metals 2024年第4期43卷 1672-1685页

作者： Zeng-Yi Li Li-Xian Sun Fen Xu Yu-Mei Luo Yong-Peng Xia Sheng Wei Chen-Chen Zhang Ri-Guang Cheng Chao-Feng Ye Meng-Yuan Liu Ju-Lan Zeng Zhong Cao Hong-Ge Pan School of Material Science and Engineering Guilin University of Electronic Technology School of Chemistry and chemical Engineering Changsha University of Science and Technology institute of Science and technology for New Energy Xi'an Technological University

The conjugation of external species with twodimensional（2D） materials has broad application prospects.In this study,we have explored the potential of noble metal/2D MOF heterostructures in hydrogen storage.Specifically,the MgH2-Ni-MOF@Pd system has shown remarkable hydrogen desorption/sorption performances,starting to liberate hydrogen at 181 0C,which is 230 0C lower than that of pristine MgH2.Under the catalytic effect of Ni-MOF@Pd,the dehydrogenation apparent activation energy of MgH2 is noticeably decreased from（133.5 ± 17.5） to（34.58 ± 1.87） kJ·mol-1,and the hydrogenation apparent activation energy is reduced from（70.41 ± 7.43） to（25.78 ± 4.64） kJ·mol-1,which is lowered by 63.4%.The fully-dehydrogenated MgH2-NiMOF@Pd composite rapidly uptakes hydrogen,with 2.62wt% at 100℃ and 6.06 wt% at 150℃ within 300 s,respectively.The mechanism analysis of MgH2 catalyzed by Ni-MOF@Pd has revealed that the transformation of Mg2Ni and Mg2NiH4could act as a "hydrogen pump",providing numerous channels for fast diffusion and transport of hydrogen atoms.Moreover,in the dehydrogenation process,the element Pd reacts with MgH2to form the MgPd alloy phase,which makes MgH2take precedence to decompose through the Mg-Pd alloy rather than self-decomposition,further reducing thermal stability and improving de/hydrogenation kinetics.The synergistic effect of Mg-Pd,Mg2Ni,and the special ultra-thin 2D sheet structure of the additive is the main reason for the good hydrogen storage property of MgH2-Ni-MOF@Pd.Our findings provide inspiration for designing efficient multifunctional additives with unique morphologies to optimize the hydrogen desorption/sorption behaviors of hydrogen storage materials.

关键词： Hydrogen storage Magnesium hydride 2D metal-organic framework nanosheets Ni/Pd Synergistic catalysis

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Machine-learned wearable sensors for real-time hand-motion recognition: toward practical applications

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National Science Review 2024年第2期11卷 231-263页

作者： Kyung Rok Pyun Kangkyu Kwon Myung Jin Yoo Kyun Kyu Kim Dohyeon Gong Woon-Hong Yeo Seungyong Han Seung Hwan Ko Department of Mechanical Engineering Seoul National University IEN Center for Human-Centric Interfaces and Engineering Institute for Electronics and NanotechnologyGeorgia Institute of Technology School of Electrical and Computer Engineering Georgia Institute of Technology Department of chemical Engineering Stanford University Department of Mechanical Engineering Ajou University George W.Woodruff School of Mechanical Engineering Georgia Institute of Technology institute of Advanced Machinery and Design(SNU-IAMD) Seoul National University

Soft electromechanical sensors have led to a new paradigm of electronic devices for novel motion-based wearable applications in our daily lives. However, the vast amount of random and unidentified signals generated by complex body motions has hindered the precise recognition and practical application of this technology. Recent advancements in artificial-intelligence technology have enabled significant strides in extracting features from massive and intricate data sets, thereby presenting a breakthrough in utilizing wearable sensors for practical applications. Beyond traditional machine-learning techniques for classifying simple gestures, advanced machine-learning algorithms have been developed to handle more complex and nuanced motion-based tasks with restricted training data sets. Machine-learning techniques have improved the ability to perceive, and thus machine-learned wearable soft sensors have enabled accurate and rapid human-gesture recognition, providing real-time feedback to users. This forms a crucial component of future wearable electronics, contributing to a robust human–machine interface. In this review, we provide a comprehensive summary covering materials, structures and machine-learning algorithms for hand-gesture recognition and possible practical applications through machine-learned wearable electromechanical sensors.

关键词： wearable sensor soft electronics artificial intelligence machine learning human–machine interfaces gesture recognition

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A three-way electrolyte with ternary solvents for high-energy-density and long-cycling lithium-sulfur pouch cells

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SusMat 2024年第2期4卷 1-12页

作者： Zheng Li Legeng Yu Chen-Xi Bi Xi-Yao Li JinMa Xiang Chen Xue-Qiang Zhang Aibing Chen Haoting Chen Zuoru Zhang Li-Zhen Fan Bo-Quan Li Cheng Tang Qiang Zhang Tsinghua Center for Green chemical Engineering Electrification Beijing Key Laboratory of Green Chemical Reaction Engineering and TechnologyDepartment of Chemical EngineeringTsinghua UniversityBeijingChina School of Materials Science and Engineering Beijing Institute of TechnologyBeijingChina institute of Advanced Materials and technology University of Science and TechnologyBeijingChina Shanxi Research institute for Clean Energy Tsinghua UniversityTaiyuanChina Center for Next-Generation Energy Materials and School of chemical Engineering Sungkyunkwan UniversityJangan-GuSuwon-SiGyeonggi-DoRepublic of Korea College of chemical and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuangChina Ordos Carbon Neutral Research and application Co. Ltd.Kangbashi DistrictOrdos CityInner MongoliaChina institute for Carbon Neutrality Tsinghua UniversityBeijingChina

Lithium–sulfur(Li–S)batteries promise high-energy-density potential to exceed the commercialized lithiumion batteries but suffer from limited cycling lifespan due to the side reactions between lithium polysulfides(LiPSs)and Li metal anodes.Herein,a three-way electrolyte with ternary solvents is proposed to enable high-energy-density and long-cycling Li–S pouch cells.Concretely,ternary solvents composed of 1,2-dimethoxyethane,di-isopropyl sulfide,and 1,3,5-trioxane are employed to guarantee smooth cathode kinetics,inhibit the parasitic reactions,and construct a robust solid electrolyte interphase,respectively.The cycling lifespan of Li–S coin cells with 50μm Li anodes and 4.0 mg cm^(−2) sulfur cathodes is prolonged from88 to 222 cycles using the three-way electrolyte.Nano-heterogeneous solvation structure of LiPSs and organic-rich solid electrolyte interphase are identified to improve the cycling stability of Li metal anodes.Consequently,a 3.0 Ah-level Li–S pouch cell with the three-way electrolyte realizes a high energy density of 405 Wh kg^(−1) and undergoes 27 cycles.Thiswork affords a three-way electrolyte recipe for suppressing the side reactions of LiPSs and inspires rational electrolyte design for practical high-energy-density and long-cycling Li–S batteries.

关键词： lithium metal anodes lithium-sulfur batteries pouch cells solid electrolyte interphase three-way electrolyte

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Preparation and properties of high-energy-density aluminum/boroncontaining gelled fuels

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Chinese Journal of chemical Engineering 2024年第1期65卷 230-242页

作者： Yi Chen Kang Xue Yang Liu Lun Pan Xiangwen Zhang Ji-Jun Zou Key Laboratory for Green chemical technology of the Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Collaborative Innovative Center of chemical Science and Engineering(Tianjin) Tianjin 300072China Haihe Laboratory of Sustainable chemical Transformations Tianjin 300192China Zhejiang institute of Tianjin University Ningbo 315201China

Energetic nanofluid fuel has caught the attention of the field of aerospace liquid propellant for its high energy density(HED), but it suffers from the inevitable solid-liquid phase separation problem. To resolve this problem, herein we synthesized the high-Al-/B-containing(up to 30%(mass)) HED gelled fuels, with low-molecular-mass organic gellant Z, which show high net heat of combustion(NHOC), density, storage stability, and thixotropic properties. The characterizations indicate that the application of energetic particles to the gelled fuels obviously destroys their fibrous network structures but can provide the new particle-gellant gelation microstructures, resulting in the comparable stability between 1.0%(mass) Z/JP-10 + 30%(mass) Al or B and pure JP-10 gelled fuel. Moreover, the gelled fuels with high-content Al or B exhibit high shear-thinning property, recovery capability, and mechanical strength, which are favorable for their storage and utilization. Importantly, the prepared 1.0%(mass) Z/JP-10 + 30%(mass) B(or 1.0%(mass) Z/JP-10 + 30%(mass) Al) shows the density and NHOC 1.27 times(1.30) and 1.43 times(1.21)higher than pure JP-10, respectively. This work provides a facile and valid approach to the manufacturing of HED gelled fuels with high content of energetic particles for gel propellants.

关键词： Gelled fuels Energetic aluminum/boron Low-molecular-mass organic gellant Fuel property

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Probing the electric double layer structure at nitrogen-doped graphite electrodes by constant-potential molecular dynamics simulations

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Journal of Energy Chemistry 2024年第6期93卷 299-305,I0008页

作者： Legeng Yu Nan Yao Yu-Chen Gao Zhong-Heng Fu Bo Jiang Ruiping Li Cheng Tang Xiang Chen Tsinghua Center for Green chemical Engineering Electrification(CCEE) Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Beijing Advanced Innovation Center for Materials Genome Engineering Institute for Advanced Materials and TechnologyUniversity of Science and Technology BeijingBeijing 100083China National Materials Corrosion and Protection Data Center University of Science and Technology BeijingBeijing 100083China Ordos Carbon Neutral Research and application Co. Ltd.Ordos 017010Inner Mongoli1China institute for Carbon Neutrality Tsinghua UniversityBeijing 100084China Center for Next-Generation Energy Materials and School of chemical Engineering Sungkyunkwan University2066 Seobu-roJangan-guSuwon-siGyeonggi-do 16419Republic of Korea

Electric double layer(EDL)is a critical topic in electrochemistry and largely determines the working performance of lithium batteries.However,atomic insights into the EDL structures on heteroatom-modified graphite anodes and EDL evolution with electrode potential are very lacking.Herein,a constant-potential molecular dynamics(CPMD)method is proposed to probe the EDL structure under working conditions,taking N-doped graphite electrodes and carbonate electrolytes as an example.An interface model was developed,incorporating the electrode potential and atom electronegativities.As a result,an insightful atomic scenario for the EDL structure under varied electrode potentials has been established,which unveils the important role of doping sites in regulating both the EDL structures and the following electrochemical reactions at the atomic level.Specifically,the negatively charged N atoms repel the anions and adsorb Li~+at high and low potentials,respectively.Such preferential adsorption suggests that Ndoped graphite can promote Li~+desolvation and regulate the location of Li~+deposition.This CPMD method not only unveils the mysterious function of N-doping from the viewpoint of EDL at the atomic level but also applies to probe the interfacial structure on other complicated electrodes.

关键词： Lithium batteries Graphite N-doping Electric double layer Molecular dynamics Constant potential method Electrode potential

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