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Li-richening strategy in Li_(2)ZrCl_(6) lattice towards enhanced ionic conductivity

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Journal of Energy Chemistry 2023年第4期79卷 348-356页

作者： Haochang Zhang Zhaozhe Yu Hannan Chen Yongjian Zhou Xiao Huang Bingbing Tian Guangxi Key Laboratory of Manufacturing Systems and Advanced Manufacturing Technology Guilin University of Electronic TechnologyGuilin 541004GuangxiChina International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education Institute of Microscale OptoelectronicsShenzhen UniversityShenzhen 518060GuangdongChina

All-solid-state Li batteries(ASSLBs) with solid-state electrolytes(SSEs) are exciting candidates for nextgeneration energy storage and receive considerable attention owing to their reliability. Halide SSEs are promising candidates due to their excellent stability against 4 V-class layered cathodes. Compared with Li3InCl6or Li_(3)ScCl_(6), the low ionic conductivity of Li_(2)ZrCl_(6)(LZC) is a challenge despite its low raw-material cost. Herein, we report a family of Li-Richened chloride, Li_(2+2x)Zr_(1–x)MxCl_(6), which can be used in highperformance ASSLBs owing to its high ionic conductivity(up to 0.62 mS cm^(-1)). The theoretical(ab initio molecular dynamics simulations) and experimental results prove that the strategy of aliovalent substitution with divalent metals to obtain Li-Richened LZC is effective in improving Li^(+)conductivity in SSEs. By combining Li_(2.1)Zr_(0.95)Mg_(0.05)Cl_(6)(Mg5-LZC) with a Li–In anode and a LiCoO_(2)cathode, a room-temperature ASSLBs with excellent long-term cycling stability(88% capacity retention at 0.3C for 100 cycles) and highrate capability(121 m A h g^(-1)at 1C) is reported. This exploratory work sheds light on improving the Li^(+)conductivity of low-cost LZC-family SSEs for constructing high performance ASSLBs.

关键词： Li-richening Li_(2)ZrCl_(6) Halide solid electrolyte All-solid-state battery Solid electrochemistry Li^(+)conductivity

From protonation & Li-rich contamination to grain-boundary segregation: Evaluations of solvent-free vs. wet routes on preparing Li_(7)La_(3)Zr_(2)O_(12) solid electrolyte

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Journal of Energy Chemistry 2022年第10期31卷 223-239,I0005页

作者： Xiao Huang Yang Lu Yajun Niu Jiawen Tang Yongjian Zhou Yan Yang Bingbing Tian SZU-NUS Collaborative Innovation Center for Optoelectronic Science&Technology International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of EducationInstitute of Microscale OptoelectronicsShenzhen UniversityShenzhen 518060GuangdongChina Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Collaborative Innovation Center for Vessel Pollution Monitoring and Control Dalian Maritime UniversityDalian 116026LiaoningChina

Garnet-type Li_(7)La_(3)Zr_(2)O_(12)(LLZO) has been recognized as a candidate solid electrolyte for high-safety Lianode based solid-state batteries because of its electro-chemical stability against Li-metal and high ionic conductivity. Solvent(e.g., isopropanol(IPA)) has been commonly applied for preparing LLZO powders and ceramics. However, the deterioration of the proton-exchange between LLZO and IPA/absorbed moisture during the mixing and tailoring route has aroused less attention. In this study, a solvent-free dry milling route was developed for preparing the LLZO powders and ceramics. For orthogonal four categories of samples prepared using solvent-free and IPA-assisted routes in the mixing and tailoring processes, the critical evaluation was conducted on the crystallinity, surficial morphology, and contamination of ascalcinated and as-tailored particles, the cross-sectional microstructure of green and sintered pellets,the morphology and electro-chemical properties of grain boundaries in ceramics, as well as the interfacial resistance and performance of Li anode based symmetric batteries. The wet route introduced Li-rich contaminations(e.g., Li OH·H)_(2)O and Li)_(2)CO)_(3)) onto the surfaces of LLZO particles and Li-Ta-O segregations at the adjacent and triangular grain boundaries. The LLZO solid electrolytes prepared through dry mixing in combination with the dry tailoring route without the use of any solvent were found to the optimal performance. The fundamental material properties in the whole LLZO preparation process were found, which are of guiding significance to the development of LLZO powder and ceramic production craft.

关键词： Li_(7)La_(3)Zr_(2)O_(12) Solid electrolyte Solvent-free procedure Ion-exchange Grain boundary Fundamental material properties

Recent Advances on Porous Materials for Synergetic Adsorption and Photocatalysis

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Energy & Environmental Materials 2022年第3期5卷 711-730页

作者： tianqi Wang Bingbing Tian Bin Han Dingren Ma Mingzhe Sun Aamir Hanif Dehua Xia Jin Shang International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education Institute of Microscale OptoelectronicsShenzhen UniversityShenzhen 518060China School of Energy and Environment City University of Hong KongTat Chee AvenueKowloonHong Kong China Institute of Microscale Optoelectronics Shenzhen UniversityShenzhen 518060China Key Laboratory for City Cluster Environmental Safety and Green Development of the Ministry of Education Institute of Environmental and Ecological EngineeringGuangdong University of TechnologyGuangzhou 510006China School of Environmental Science and Engineering Sun Yat-Sen UniversityGuangzhou 510275China City University of Hong Kong Shenzhen Research Institute Nanshan District8 Yuexing 1st RoadShenzhen Hi−Tech Industrial ParkShenzhen 518060China Department of Chemistry Islamic University of Science and TechnologyAwantipora 192122India

Porous photocatalysts are promising materials capable of simultaneously adsorbing and oxidizing/reducing target species,showing great potentials in environmental remediation and energy generation.This review offered a comprehensive overview of the recent progress in design,fabrication,and applications of porous photocatalysts,including carbon-based semiconductors,metal oxides/sulfides,metal–organic frameworks,and adsorbent–photocatalyst hybrids.The fundamental understanding of the structure–performance relationships of porous materials together with the in-depth insights into the synergetic effects between adsorption and photocatalysis was presented.The strategies to further improve the photocatalytic activity of porous photocatalysts were proposed.This review would provide references and outlooks of constructing efficient porous materials for adsorptive and photocatalytic removal of pollutants and energy production.

关键词： adsorption photocatalysis porous materials synergetic effect

Constructing stable Li-solid electrolyte interphase to achieve dendrites-free solid-state battery:A nano-interlayer/Li prereduction strategy

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Nano Research 2022年第8期15卷 7180-7189页

作者： Yajun Niu Zhaozhe Yu Yongjian Zhou Jiawen Tang Maoxin Li Zechao Zhuang Yan Yang Xiao Huang Bingbing Tian Guangxi Key Laboratory of Manufacturing Systems and Advanced Manufacturing Technology Guilin University of Electronic TechnologyGuilin 541004China International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education Institute of Microscale OptoelectronicsShenzhen UniversityShenzhen 518060China Department of Chemistry Tsinghua UniversityBeijing 100084China Collaborative Innovation Center for Vessel Pollution Monitoring and Control Dalian Maritime UniversityDalian 116026China

Solid-state batteries based on Li and nonflammable solid-state electrolytes(SSEs)have aroused the attention of numerous researchers because of their absolute safety and potentially high energy density.Most SSEs after coming into contact with Li are reduced,which leads to high interfacial charge-transfer impedance and dendrites formation.In this study,an“interlayer-Li pre-reduction strategy”was proposed to solve the above problem of reduction.An intermediate layer was introduced between solid electrolyte and Li,and it reacted with Li to produce a stable and ion-conductive interphase.Cubic garnet-type Nb-doped Li_(7)La_(3)Zr_(2)O_(12)(Nb-LLZO)was selected as an example solid electrolyte since it is characterized by high ionic conductivity,feasible preparation under ambient conditions,as well as low cost.The high impedance arising from the reduction at the Nb-LLZO|Li interface has limited its application.In this paper,a nano-scale Li phosphorus oxynitride(LiPON)layer was deposited on the Nb-LLZO pellets through radio frequency(RF)magnetron sputtering,which pre-reacted with Li in-situ to produce a lithiophilic,electronically insulating,and ionic conductive interphase.The produced interphase significantly inhibited the reduction of Nb5+against Li and the formation and propagation of Li dendrites.It is noteworthy that Li|LiPON|Nb-LLZO|LiPON|Li cells stably cycled for over 2,000 h without any short circuit.This study emphasizes and demonstrates the significance of the pre-conversion of modification layer between unstable SSE and Li metal to improve interfacial stability.

关键词： Nb-doped Li_(7)La_(3)Zr_(2)O_(12)(Nb-LLZO) conversion reaction Li phosphorus oxynitride(LiPON) interfacial reduction solid-state battery

Aqueous Zn^(2+)/Na^(+) dual-salt batteries with stable discharge voltage and high Coulombic efficiency by systematic electrolyte regulation

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Science China Chemistry 2022年第2期65卷 399-407页

作者： Chunli Wang Lianshan Sun Maoxin Li Lin Zhou Yong Cheng Xin Ao Xiuyun Zhang Limin Wang Bingbing Tian Hong Jin Fan SZU-NUS Collaborative Innovation Center for Optoelectronic Science&Technology International Collaborative Laboratory of 2D Materials for Optoelectronic Science and Technology of Ministry of EducationInstitute of Microscale OptoelectronicsShenzhen UniversityShenzhen 518060China School of Physical and Mathematical Science Nanyang Technological UniversitySingapore 637371Singapore China-Singapore International Joint Research Institute Guangzhou 510663China College of Physics Science and Technology Yangzhou UniversityYangzhou 225002China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryCASChangchun 130022China Institute for Energy Research Jiangsu UniversityZhenjiang 212013China

While aqueous Zn-Na hybrid batteries have garnered widespread attention because of their low cost and high safety,it is still challenging to achieve long cycle-life and stable discharge-voltage due to sluggish reaction kinetics,zinc dendrite formation,and side reactions.Herein,we design a Zn^(2+)/Na^(+) dual-salt battery,in which sodiation of the NVP cathode favors zinc intercalation under an energy threshold,leading to decoupled redox reactions on the cathode and anode.Systematic investigations of the electrolyte effects show that the ion intercalation mechanism and the kinetics in the mixture of triflate-and acetate-based electrolytes are superior to those in the common acetate-only electrolytes.As a result,we have achieved fast discharging capability,suppressed zinc dendrites,a stable discharge voltage at 1.45 V with small polarization,and nearly 100%Coulombic efficiency in the dual-salt mixture electrolyte with optimized concentration of 1 M Zn(OAc)_(2)+1 M NaCF_(3)SO_(3).This work demonstrates the importance of electrolyte regulation in aqueous dual-salt hybrid batteries for the energy storage.

关键词： dual-salt battery high voltage acetate electrolyte zinc dendrite Na_(3)V_(2)(PO_(4))_(3)

A multiphase sodium vanadium phosphate cathode material for high-rate sodium-ion batteries

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Journal of Materials Science & Technology 2021年第7期66卷 121-127页

作者： Chuan Wang Hai Long Lijiao Zhou Chao Shen Wei Tang Xiaodong Wang Bingbing Tian Le Shao Zhanyuan tian Haijun Su Keyu Xie Research&Development Institute of Northwestern Polytechnical University in Shenzhen Northwestern Polytechnical UniversityShenzhen 518057China State Key Laboratory of Solidification Processing Center for Nano Energy MaterialsSchool of Materials Science and EngineeringNorthwestern Polytechnical University and Shaanxi Joint Laboratory of Graphene(NPU)Xi'an 710072China School of Chemical Engineering and Technology Xi'an Jiaotong UniversityXi'an 710049China Central Analytical Research Facility Queensland University of Technology.Australia International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education Institute of Microscale OptoelectronicsShenzhen UniversityShenzhen 518060China Shaanxi Coal and Chemical Technology Institute Co. Ltd.Jinye RoadXi'an 710070China

The unsatisfactory rate capability and poor cycling stability at high rate of sodium-ion batteries(SIBs) have impeded their practical applications. Herein, a Na_(3)V_(2)(PO_(4))_(3)/Na_(3)V_(3)(PO_(4))_(4) multiphase cathode materials for high-rate and long cycling SIBs was successfully synthesized by regulation the stoichiometric ratio of raw materials. The combined experiment and simulation results show that the multiphase materials consisted of NASICON structural phase Na3V2(PO4)3 and layered structure phase Na_(3)V_(3)(PO_(4))_(4), possess abundant phase boundaries. Electrochemical experiments demonstrate that the multiphase materials maintain a remarkable reversible capacity of 69.0 mA h g^(-1) even at an ultrahigh current density of 100 C with a high capacity retention of 81.25 % even after 10,000 cycles. Na_(3)V_(2)(PO_(4))_(3)/Na_(3)V_(3)(PO_(4))_(4) electrode exhibits a higher working voltage, superior rate capability and better cycling stability than Na_(3)V_(2)(PO_(4))_(3) electrode, which indicates that the introduction of second phase can be an effective strategy for the development of novel cathode materials for SIBs.

关键词： Sodium-ion batteries High-rate capability Multiphase Na_(3)V_(2)(PO_(4))_(3) Na_(3)V_(3)(PO_(4))_(4)

Spatial Variation and Risk Assessment of Arsenic and Heavy Metals in Surface Water and Suspended Particulate Matter in Tail Reaches of the Yellow River, China

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Chinese Geographical Science 2021年第1期31卷 181-196页

作者： SUN Zhigao LI Jing tian Liping CEHN bingbing HU Xingyun Key Laboratory of Humid Subtropical Eco-geographical Process(Fujian Normal University) Ministry of EducationFuzhou 350007China Institute of Geography Fujian Normal UniversityFuzhou 350007China Fujian Provincial Key Laboratory for Subtropical Resources and Environment Fujian Normal UniversityFuzhou 350007China

To determine the pollution levels and potential toxic risks of arsenic(As) and heavy metals(Cr, Ni, Cu, Zn, Pb and Cd) in water and suspended particulate matter(SPM) in tail reaches(including freshwater reach and low-salinity reach) of the Yellow River as the Flow-Sediment Regulation Project(FSRP) has been carried out for approximately 15 yr, the surface water and SPM were sampled at pre-flood(April) and post-flood seasons(October). Results showed that similar changes of As and metal levels in water and SPM were observed along the tail reaches at pre-flood or post-flood season. Compared to pre-flood season, the levels of As, Cu, Cr and Ni in freshwater reach and the concentrations of Cr and Ni in low-salinity reach rose greatly at post-flood season. The levels of As and metals in SPM of freshwater reach or low-salinity reach at pre-flood season were significantly higher than those at post-flood season(P < 0.01).The pollutions of As and metals in surface water of tail reaches at pre-flood or post-flood season were not serious. The SPM in freshwater reach at pre-flood season were polluted by Cd, As, Cr, Cu and Ni while those in low-salinity reach were polluted by Cd and Cr. The SPM in freshwater reach at post-flood season were polluted by Cd and Pb while those in low-salinity reach were polluted by Cd and Cr.Cd was identified as heavy metal of primary concern at both pre-flood and post-flood seasons. Combined with the existed data reported in present research, this study found that the toxic risk of As and metals in SPM of tail reaches at pre-flood season was higher than that at post-flood season, implying that the implementation of FSRP during flooding season, to a great extent, reduced the toxic risk of these elements. With the long-term implementation of FSRP, the pollution levels of As and metals(particularly for Cd) in SPM of tail reaches might be elevated and the potential toxic risk primarily produced by Cr, Ni and As might be increased if effective measures were not taken in future.

关键词： arsenic and heavy metals surface water suspended particulate matter tail reaches Yellow River

Formation of NiFe_2O_4/Expanded Graphite Nanocomposites with Superior Lithium Storage Properties

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Nano-Micro Letters 2017年第3期9卷 101-108页

作者： Yinglin Xiao Jiantao Zai Bingbing Tian Xuefeng Qian SZU-NUS Collaborative Innovation Center for Optoelectronic Science and Technology Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong Province College of Optoelectronic Engineering Shenzhen University School of Chemistry and Chemical Engineering State Key Laboratory of Metal Matrix CompositesShanghai Jiao Tong University Department of Chemistry National University of Singapore3 Science Drive 3

A Ni Fe_2O_4/expanded graphite(Ni Fe_2O_4/EG)nanocomposite was prepared via a simple and inexpensive synthesis method. Its lithium storage properties were studied with the goal of applying it as an anode in a lithium-ion battery. The obtained nanocomposite exhibited a good cycle performance, with a capacity of 601 m Ah g^(-1)at a current of 1 A g^(-1)after 800 cycles. This good performance may beattributed to the enhanced electrical conductivity and layered structure of the EG. Its high mechanical strength could postpone the disintegration of the nanocomposite structure,efficiently accommodate volume changes in the Ni Fe_2O_4-based anodes, and alleviate aggregation of Ni Fe_2O_4 nanoparticles.

关键词： NiFe2O4 Expanded graphite Anode materials Lithium-ion batteries

Halide/sulfide composite solid-state electrolyte for Li-anode based all-solid-state batteries

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Chinese Chemical Letters 2023年第11期34卷 326-331页

作者： Haochang Zhang Zhaozhe Yu Jinyin Cheng Hannan Chen Xiao Huang Bingbing Tian International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education Institute of Microscale OptoelectronicsShenzhen UniversityShenzhen 518060China Guangxi Key Laboratory of Manufacturing Systems and Advanced Manufacturing Technology Guilin University of Electronic TechnologyGuilin 541004China

Li_(2)ZrCl_(6)(LZC) solid-state electrolytes(SSEs) have been recognized as a candidate halide SSEs for allsolid-state Li batteries(ASSLBs) with high energy density and safety due to its great compatibility with4V-class cathodes and low bill-of-material(BOM) cost.However,despite the benefits,the poor chemical/electrochemical stability of LZC against Li metal causes the deterioration of Li/LZC interface,which has a detrimental inhibition on Li^(+) transport in ASSLBs.Herein,we report a composite SSE combining by LZC and argyrodite buffer layer(Li_(6)PS_(5)Cl,LPSC) that prevent the unfavorable interaction between LZC and Li metal.The Li/LPSC-LZC-LPSC/Li symmetric cell stably cycles for over 1000 h at 0.3 mA/cm^(2)(0.15mAh/cm^(2)) and has a high critical current density(CCD) value of 2.1 mA/cm^(2)at 25 ℃,Under high temperature(60℃) which promotes the reaction between Li and LZC,symmetric cell fabricated with composite SSE also display stable cycling performance over 1200h at 0.3 mAh/cm^(2).Especially,the Li/NCM ASSLBs fabricated with composite SSE exhibit a high initial coulombic efficiency,as well as superior cycling and rate performance.This simple and efficient strategy will be instrumental in the development of halidebased high-performance ASSLBs.

关键词： Li_(2)ZrCl_(6) Li_(6)PS_(5)Cl Composite solid-state electrolyte Interface stability Li anode