A review of Al-based material dopants for high-performance solid state lithium metal batteries

As the world transitions to green energy, there is a growing focus among many researchers on the requirement for high-efficient and safe batteries. Solid-state lithium metal batteries(SSLMBs) have emerged as a promising alternative to traditional liquid lithium-ion batteries(LIBs), offering higher energy density, enhanced safety, and longer lifespan. The rise of SSLMBs has brought about a transformation in energy storage, with aluminum(Al)-based material dopants playing a crucial role in advancing the next generation of batteries. The review highlights the significance of Al-based material dopants in SSLMBs applications, particularly its contributions to solid-state electrolytes(SSEs), cathodes, anodes,and other components of SSLMBs. Some studies have also shown that Al-based material dopants effectively enhance SSE ion conductivity, stabilize electrode and SSE interfaces, and suppress lithium dendrite growth, thereby enhancing the electrochemical performance of SSLMBs. Despite the above mentioned progresses, there are still problems and challenges need to be addressed. The review offers a comprehensive insight into the important role of Al in SSLMBs and addresses some of the issues related to its applications, endowing valuable support for the practical implementation of SSLMBs.

Incorporating multifunctional LiAlSiO_(4) into polyethylene oxide for high-performance solid-state lithium batteries

High ionic conductivity,good electrochemical stability,and satisfactory mechanical property are the crucial factors for polymer solid state electrolytes.Herein,fast ion conductor LiAlSiO_4(LASO) is incorporated into polyethylene oxide(PEO)-based solid-state electrolytes(SSEs).The SSEs containing LASO exhibit enhanced mechanical properties performance compared to pristine PEO-LiTFSI electrolyte.A reduced melting transition temperature of 40.57℃ is enabled by introducing LASO in to PEO-based SSE,which is beneficial to the motion of PEO chain and makes it possible for working at a moderate environment.Coupling with the enhanced motion of PEO,dissociation of the lithium salt,and conducting channel of LASO,the optimized composite polymer SSE exhibits a high ionic conductivity of 4.68×10^(-4),3.16×10^(-4) and 1.62×10^(-4) S cm^(-1) at 60,50 and 40℃,respectively.The corresponding LiFePO_4//Li solid-state battery exhibits high specific capacities of 166,160 and 139 mAh g^(-1) at 0.2 C under 60,40 and 25℃.In addition,it remains 130 mAh g^(-1) at 4.0 C,and maintains 91.74% after 500 cycles at 1.0 C under 60℃.This study provides a simple approach for developing ionic conductor-filled polymer electrolytes in solid-state lithium battery application.

Incombustible solid polymer electrolytes:A critical review and perspective

Since the advent of the solid-state batteries,employing solid polymer electrolytes(SPEs)to replace routine flammable liquid electrolytes is regarded to be one of the most promising solutions in pursing highenergy-density battery systems.SPEs with superior thermal stability,good processability,and high mechanical modulus obtain increasing attentions.However,SPE-based batteries are not impenetrable due to their decomposition and combustibility under extreme conditions.Researchers believe incorporating appropriate flame-retardant additives/solvents/fragments into SPEs can intrinsically reduce their flammability to solve the battery safety issues.In this review,the recent research progress of incombustible SPEs,with special emphasis on flame-retardant structural design,is summarized.Specifically,a brief introduction of flame-retardant mechanism,evaluation index for safety of SPEs,and a detailed overview of the latest advances on diverse-types SPEs in various battery systems are highlighted.The deep insight into thermal ru naway process,the free-standing incombustible GPEs,and the ratio nal design of pouch cell structures may be the main directions to motivate revolutionary next-generation for safety batteries.

Carbon‐based materials for all‐solid‐state zinc–air batteries

Solid‐state Zn–air batteries(ZABs)hold great potential for application in wearable and flexible electronics.However,further commercialization of current ZABs is still limited by the poor stability and low energy efficiency.It is,thus,crucial to develop efficient catalysts as well as optimize the solid electrolyte system to unveil potential of the ZAB technology.Due to the low cost and versatility in tailoring the structures and properties,carbon materials have been extensively used as the conductive substrates,catalytic air electrodes,and important components in the electrolytes for the solid‐state ZABs.Within this context,we discuss the challenges facing current solid‐state ZABs and summarize the strategies developed to modify properties of carbon‐based electrodes and electrolytes.We highlight the metal−organic framework/covalent organic framework‐based electrodes,heteroatom‐doped carbon,and the composites formed of carbon with metal oxides/sulfides/phosphides.We also briefly discuss the progress of graphene oxide‐based solid electrolyte.

A flexible PEO-based polymer electrolyte with cross-linked network for high-voltage all solid-state lithium-ion battery

Solid state lithium-ion batteries(SLIBs)have been considered as one of the most promising sustainable next-generation technologies for energy storage.However,the poor interfacial compatibility and low ion conductivity of solid electrolytes still remain a major challenge for SLIBs.Herein,a free-standing flexible solid polymer LA-PAM-PEO electrolyte is constructed through the electrospinning technology featuring with high Li+conductivity(6.1×10^(−4)S cm^(−1)),strong mechanical strength and high Li+migration num-ber(0.32),which breaks the restriction between ionic conductivity and mechanical strength in polymer solid electrolyte.The cross-linking between LA,PAM and PEO is verified to decrease the crystalline of PEO,thus increasing the Li+conductivity.Moreover,benefiting from the 3D network composed of in-terconnected nanofibers and the covalent bonds between LA,PAM and PEO,the mechanical strength of LA-PAM-PEO SPE was also effectively im proved.The LA-PAM-PEO SPE also delivers a high electrochemi-cal window(4.95 V),and low interface resistance(243.8).As a result,the Li/Li symmetrical cell with the LA-PAM-PEO displayed outstanding stability after 1000 h with the uniform Li deposition on the in-terface of Li electrode,in sharp contrast to the PEO SPE.In addition,the Li/LA-PAM-PEO SPE/LFP displays a discharge capacity of 135 mA h g^(−1)after 1000 cycles at the rate of 1 C,with a capacity retention of 93.5%.The proposed LA-PAM-PEO SPE thus opens new possibilities for the fabrication and engineering of solid-state Li-ion batteries.

Forming solid electrolyte interphase in situ in an ionic conducting Li_(1.5)Al_(0.5)Ge_(1.5)(PO_4)_3-polypropylene(PP) based separator for Li-ion batteries

A new concept of forming solid electrolyte interphases（SEI） in situ in an ionic conducting Li（1.5）Al（0.5）Ge（1.5）（PO4）3-polypropylene（LAGP-PP） based separator during charging and discharging is proposed and demonstrated. This unique structure shows a high ionic conductivity, low interface resistance with electrode, and can suppress the growth of lithium dendrite. The features of forming the SEI in situ are investigated by scanning electron microscopy（SEM） and x-ray photoelectron spectroscopy（XPS）. The results confirm that SEI films mainly consist of lithium fluoride and carbonates with various alkyl contents. The cell assembled by using the LAGP-coated separator demonstrates a good cycling performance even at high charging rates, and the lithium dendrites were not observed on the lithium metal electrode. Therefore, the SEI-LAGP-PP separator can be used as a promising flexible solid electrolyte for solid state lithium batteries.

Porous garnet as filler of solid polymer electrolytes to enhance the performance of solid-state lithium batteries

In order to enhance the ionic conductivity of solid polymer electrolytes(SPEs)and their structural rigidity against lithium dendrite during lithium-ion battery(LIB)cycling,we propose porous garnet Li6.4La3Zr2Al0.2O12(LLZO),as the filler to SPEs.The porous LLZO with interlinked grains was synthesized via a resol-assisted cationic coordinative co-assembly approach.The porous structure of LLZO with high specific surface area facilitates the interaction between polymer and filler and provides sufficient entrance for Li^(+)migration into the LLZO phase.Furthermore,the interconnection of LLZO grains forms continuous inorganic pathways for fast Li^(+)migration,which avoid the multiple diffusion for Li^(+)in interface.As a result,the SPEs with porous LLZO(SPE-PL)show a high ionic conductive of 0.73 mS·cm^(-1) at 30℃ and lithium-ion transference number of 0.40.The porous LLZO with uniformly dispersed pores also acts as an ion distributor to regulate ionic flux.The lithium-symmetrical batteries assembled with SPE-PL show a highly stable Li plating/stripping cycling for nearly 3000 h at 0.1 mA·cm^(-2).The corresponding Li/LiFePO_(4) batteries also exhibit excellent cyclic performance with capacity retention of 75%after nearly 500 cycles.This work brings new insights into the design of conductive fillers and the optimization of SPEs.

Tailored architecture of composite electrolyte for all-solid-state sodium batteries with superior rate performance and cycle life

Seeking for composite electrolytes reinforced all-solid-state sodium ion batteries with superior long lifespan and rate performance remains a great challenge.Here,a unique strategy to tailor the architecture of composite electrolyte via inserting polymer chains into a small quantity of sulfate sodium grafted C_(48)0H_(28)O_(32)Zr_(6)(UIOSNa)is proposed.The intimate contact between polymer segments and UIOSNa with limited pore size facilitates the anion immobilization of sodium salts and reduction of polymer crystallinity,thereby providing rapid ion conduction and reducing the adverse effect caused by the immigration of anions.The tNa+grafting of-SO_(3)Na groups on fillers allows the free movement of more sodium ions to further improve and ionic conductivity.Consequently,even with the low content of UIOSNa fillers,a high ionic conductivity of 6.62×10^(-4) S·cm^(-1) at 60℃ and a transference number of 0.67 for the special designed composite electrolyte are achieved.The assembled all-solid-state sodium cell exhibits a remarkable rate performance for 500 cycles with 95.96%capacity retention at a high current rate of 4 C.The corresponding pouch cell can stably work for 1000 cycles with 97.03%capacity retention at 1 C,which is superior to most of the reported composite electrolytes in the literature.

New electrochemical energy storage systems based on metallic lithium anode the research status,problems and challenges of lithium-sulfur,lithium-oxygen and all solid state batteries

Li-ion batteries have played a key role in the portable electronics and electrification of transport in modern society. Nevertheless,the limited highest energy density of Li-ion batteries is not sufficient for the long-term needs of society. Since lithium is the lightest metal among all metallic elements and possesses the lowest redox potential of.3.04 V vs. standard hydrogen electrode, it delivers the highest theoretical specific capacity of 3860 mA h g^(-1) and a high working voltage of full batteries which causes a great interest in electrochemical energy storage systems. Lithium-sulfur, lithium-oxygen and corresponding all solid state batteries based on metal lithium anode have received widely attention owing to their high energy densities. However, the problems in the cathode,electrolyte and anode of these three systems restrict their practical application. In this review, the research status and problems of these three energy storage systems are summarized and the challenges and future perspectives are also outlined.

A highly ionic transference number eutectogel hybrid electrolytes based on spontaneous coupling inhibitor for solid-state lithium metal batteries

Polymer-based solid electrolytes have been extensively studied for solid-state lithium metal batteries to achieve high energy density and reliable security.But,its practical application is severely limited by low ionic conductivity and slow Li+transference.Herein,based on the“binary electrolytes”of poly(vinylidene fluoride-chlorotrifluoroethylene)(P(VDF-CTFE))and lithium salt(LiTFSI),a kind of eutectogel hybrid electrolytes(EHEs)with high Li+transference number was developed via tuning the spontaneous coupling of charge and vacated space generated by Li-cation diffusion utilizing the Li6.4La3Zr1.4Ta0.6O12(LLZTO)dopant.LLZTO doping promotes the dissociation of lithium salt,increases Li+carrier density,and boosts ion jumping and the coordination/decoupling reactions of Li+.As a result,the optimized EHEs-10%possess a high Li-transference number of 0.86 and a high Li+conductivity of 3.2×10–4 S·cm–1 at room temperature.Moreover,the prepared EHEs-10%composite solid electrolyte presents excellent lithiumphilic and compatibility,and can be tested stably for 1,200 h at 0.3 mA·cm–2 with assembled lithium symmetric batteries.Likewise,the EHEs-10%films match well with high-loading LiFePO4 and LiCoO2 cathodes(>10 mg·cm–2)and exhibit remarkable interface stability.Particularly,the LiFePO4//EHEs-10%//Li and LiCoO2//EHEs-10%//Li cells deliver high rate performance of 118 mAh·g–1 at 1 C and 93.7 mAh·g–1 at 2 C with coulombic efficiency of 99.3%and 98.1%,respectively.This work provides an in-depth understanding and new insights into our design for polymer electrolytes with fast Li+diffusion.

The interfacial engineering of metal electrodes for high-specific-energy and long-lifespan batteries

High-specific-energy batteries with long-lifespan are the development aspiration for energy storage applications.Metal electrodes with high specific capacity and low reduction potential are potential candidates for next-generation high-specific-energy batteries.Nevertheless,the stability of the metal electrode batteries is constantly suffered from the unstable interface issue during the plat-ing/stripping process,such as dendrite formation,dynamic evolution of solid electrolyte interphase,and other accompanied side reactions.To solve these challenges,numerous researches have been intensively studied based on the interfacial engineering of metal electrodes,including electrode configuration optimization,interfacial chemistry regulation and solid-solid interface construc-tion,and the recent progress is elaborately introduced in this paper.Nevertheless,the dendrite issues cannot be entirely prohibited in solid metal electrodes,which motivate the search for potential alternatives.Liquid-metal electrodes with completely reversible structural changes and high mass transfer rate are rendered as an effective approach to solve the dendrite problem.Therefore,the development of liquid metal electrode batteries is reviewed in this paper,in which the interfacial issues are explicated and some commendable achievements are summarized.In the end,the implementation of interfacial engineering and the development roadmap of the metal electrode batteries are prospected.

Revealing milling durations and sintering temperatures on conductivity and battery performances of Li_(2.25)Zr_(0.75)Fe_(0.25)Cl_(6)electrolyte

Halide electrolytes in solid-state batteries with excellent oxidative stability and high ionic conductivity have been well reported recently.However,the high-cost rare-earth elements and long duration of highrotation milling procure are the major obstacles.Herein,we have successfully synthesized the low cost Li_(2.25)Zr_(0.75)Fe_(0.25)Cl_(6)electrolyte consisting of abundant elements with comparable Li-ion conductivity in a short milling duration of 4 h.Phase transition of the annealed sample was also carefully investigated.Li Ni_(0.6)Co_(0.2)Mn_(0.2)O_(2)/Li_(2.25)Zr_(0.75)Fe_(0.25)Cl_(6)/Li_(5.5)PS_(4.5)Cl_(1.5)/In-Li batteries using different halide electrolytes were constructed and cycled at different voltage windows.Solid-state battery using Li_(2.25)Zr_(0.75)Fe_(0.25)Cl_(6)electrolyte obtained from long milling duration delivers higher discharge capacities and superior capacity retention than shorter milling time between 3.0 and 4.3 V.It delivers much higher discharge capacity when cycled at elevated temperature(60℃)and suffers fast capacity degradation when the upper cut-off voltage increases to 4.5 V at the same current density.This work provides an efficiency synthesis strategy for halide solid electrolyte and studies its applications in all-solid-state batteries in a wide temperature range.

Key Technologies and Prospects for Electric Vehicles Within Emerging Power Systems: Insights from Five Aspects

The energy revolution requires coordination in energy consumption, supply, storage and institutional systems.Renewable energy generation technologies, along with their associated costs, are already fully equipped for large-scale promotion.However, energy storage remains a bottleneck, and solutions areneeded through the use of electric vehicles, which traditionallyplay the role of energy consumption in power systems. Toclarify the key technologies and institutions that support EVsas terminals for energy use, storage, and feedback, the CSEEJPES forum assembled renowned experts and scholars in relevantfields to deliver keynote reports and engage in discussions ontopics such as vehicle–grid integration technology, advancedsolid-state battery technology, high-performance electric motortechnology, and institutional innovation in the industry chain.These experts also provided prospects for energy storage andutilization technologies capable of decarbonizing new powersystems.