2D MXenes,particularly Ti_(3)C_(2)T_(x),have emerged as promising multifu nctional materials for advancing solidstate batteries(SSBs).While SSBs offer superior safety and energy density over liquid-electrolyte systems...2D MXenes,particularly Ti_(3)C_(2)T_(x),have emerged as promising multifu nctional materials for advancing solidstate batteries(SSBs).While SSBs offer superior safety and energy density over liquid-electrolyte systems,critical challenges such as interfacial resistance,limited ion transport,dendrite growth,and mechanical degradation hinder their widespread adoption.This review aims to provide a comprehensive analysis of the roles and fu nctions of Ti_(3)C_(2)T_(x) MXenes in SSBs,emphasizing their application as interlayers,anode/cathode additives,and current collectors,and highlighting their impact on interracial stability,ionic/electro nic transport,electrochemical performance,and cycling durability in SSB architectures.Unlike other 2D materials,Ti_(3)C_(2)T_(x) exhibits outsta nding metallic conductivity,tu nable surface terminations,hydrophilicity,and excellent mechanical flexibility,making it ideal for multifu nctional integration in SSBs,As a component in solid-state electrolytes(SSEs),Ti_(3)C_(2)T_(x) improves ionic conductivity and mecha nical strength.When used in electrodes,it serves as a conductive scaffold that enhances charge transport and structural durability.Additionally,its role as an interfacial interlayer effectively reduces interfacial impedance,accommodates volume changes,and suppresses dendrite formation.Its lightweight and high conductivity enable its use as a current collector.This review highlights recent advances in Ti_(3)C_(2)T_(x)-based components for SSBs like Li-,Na-,Zn,Li-S,etc.,emphasizing enha ncements in ion/electron transport,interfacial stability,and structural robustness.Finally,the review outlines challenges and opportunities along with a future outlook focused on improving the MXene oxidation,tailoring surface terminations,improving long-term stability,and exploring scalable fabrication strategies for MXene-based SSB components.展开更多
Solid-state sodium batteries(SSSBs)have been highly prized as a promising alternative to conventional battery systems using organic liquid electrolytes due to their improved safety,higher energy density,and substantia...Solid-state sodium batteries(SSSBs)have been highly prized as a promising alternative to conventional battery systems using organic liquid electrolytes due to their improved safety,higher energy density,and substantial resources and low cost of sodium.Na_(3)Zr_(2)Si_(2)PO_(12)(NZSP)solid electrolyte is attracting considerable interest owing to its excellent thermal and chemical stability and favorable compatibility with Na metal anode and high-voltage cathode.However,two main challenges of poor roomtemperature ionic conductivity and high interfacial resistance limit the application of NZSP electrolyte in SSSBs.So far,intensive efforts have been devoted to developing modification strategies to improve the room-temperature ionic conductivity of NZSP.This review aims to provide a comprehensive summary and discussion of some optimization strategies for enhancing the room-temperature ionic conductivity of the NZSP solid electrolyte.These optimization strategies are categorized into foreignion doping or substitution,sintering behavior modulation,and regulation of chemical composition based on precursors,and their optimization mechanisms are also elaborated.Finally,the prospects of NZSP-based solid electrolytes are presented.This review is expected to offer better guidance for designing and developing high-performance NZSP-based solid electrolytes for accelerating the practical application of SSSBs.展开更多
We proposed a strategy to address the issue by synthesizing MnO with half-filled 3 d electron orbitals.That is,MnO nanocubes with an edge length of 61.82 nm were successfully prepared through electros-pinning and one-...We proposed a strategy to address the issue by synthesizing MnO with half-filled 3 d electron orbitals.That is,MnO nanocubes with an edge length of 61.82 nm were successfully prepared through electros-pinning and one-step pyrolysis as the cathode electrode for Li-O_(2)batteries.It is observed that the intermediate LiMnO_(4)rather than Li_(2)O_(2)is formed when LiO_(2)interactes with MnO(111)during the discharge process.It is precisely because of LiMnO_(4)that reduces its charge overpotential to 0.29 V.The novel reaction mechanism dominated by LiMnO_(4)further facilitates the lower charge overpotential,thereby enhancing the energy efficiency of the batteries.展开更多
Solid-state lithium batteries are considered one of the most promising next-generation energy storage technologies owing to their safety and high energy density.The key to solid-state lithium battery advancement lies ...Solid-state lithium batteries are considered one of the most promising next-generation energy storage technologies owing to their safety and high energy density.The key to solid-state lithium battery advancement lies in the design and optimization of suitable solid-state electrolytes.Among various solid-state electrolytes,solid-state composite polymer electrolytes offer the combined benefits of solid inorganic electrolytes and solid polymer electrolytes.In particular,Li1_(+x)Al_(x)Ti_(2-x)(PO_(4))_(3)(LATP)/polymer composite polymer electrolytes exhibit high ionic conductivity due to LATP and improved flexibility from the polymer matrix.These systems also demonstrate robust mechanical properties and excellent electrode contact.While recent reviews have primarily focused on the performance of LATP/polymer composite polymer electrolytes and the general effects of composite polymer electrolyte modifications for solid-state lithium battery applications,this review provides a concise overview of the Li^(+)transport mechanisms in LATP/polymer composite polymer electrolytes and strategies to enhance ionic conductivity.It highlights several modification approaches,including the use of fillers,additives,and LATP coatings,which markedly influence the performance of composite polymer electrolytes across different polymer matrices.Finally,the review addresses the challenges of LATP/polymer composite polymer electrolytes and outlines key research directions for developing advanced composite polymer electrolytes for high-performance solid-state lithium batteries.展开更多
Solid-state batteries are attracting considerable attention for their high-energy density and improved safety over conventional lithium-ion batteries.Among solid-state electrolytes,sulfide-based options like Li_(6)PS_...Solid-state batteries are attracting considerable attention for their high-energy density and improved safety over conventional lithium-ion batteries.Among solid-state electrolytes,sulfide-based options like Li_(6)PS_(5)Cl are especially promising due to their superior ionic conductivity.However,interfacial degradation between sulfide electrolytes and high-voltage cathodes,such as LiCoO_(2),limits long-term performance.This study demonstrates that a LiBF_(4)-derived F-rich coating on LiCoO_(2),applied by immersing LiCoO_(2) particles in a LiBF_(4) solution followed by annealing,can significantly enhance performance in Li_(6)PS_(5)Cl-based solid-state batteries.This coating enables stable high-voltage(4.5 V vs Li^(+)/Li)operation,achieving an initial specific capacity of 153.82 mAh g^(−1) and 87.1%capacity retention over 300 cycles at 0.5C.The enhanced performance stems from the F-rich coating,composed of multiple phases including LiF,CoF_(2),Li_(x)BF_(y)O_(z),and Li_(x)BO_(y),which effectively suppresses side reactions at the LiCoO_(2)|Li_(6)PS_(5)Cl interface and improves lithium-ion diffusivity,thereby enabling greater Li capacity utilization.Our findings provide a practical pathway for advancing solid-state batteries with high-voltage LiCoO_(2) cathodes,offering substantial promise for next-generation energy storage systems.展开更多
Halide solid-state electrolytes(SSEs)with high ionic conductivity and excellent compatibility with highvoltage oxide cathodes in all-solid-state lithium batteries(ASSLBs)offer improved safety and cycling performance.H...Halide solid-state electrolytes(SSEs)with high ionic conductivity and excellent compatibility with highvoltage oxide cathodes in all-solid-state lithium batteries(ASSLBs)offer improved safety and cycling performance.However,the ionic conductivity of halide SSEs at room temperature(RT)and their stability against lithium(Li)metal anodes still require further enhancement.In this study,Li_(2+x)ZrCl_(6-x)S_(x)(0≤x≤1)SSEs,featuring two highly amorphous phases,are synthesized via an aliovalent sulfursubstitution strategy.Notably,a new phase(C2/m),distinct from Li_(2)ZrCl_(6)(LZC)(p3m1),is induced by modulating the sulfur substitution level for chlorine.Consequently,the crystallinity of the coexisting two-phase SSEs is significantly lower than that of the single-phase material.Owing to their highly amorphous nature,the ionic conductivity of Li_(2.25)ZrCl_(5.75)S_(0.25)(LZCS0.25)increases from 0.33 mS cm^(-1)(LZC)to0.97 mS cm^(-1)at RT.In addition,LZCS0.25 exhibits higher compressibility and lower reduction potential(1.78 V vs.2.34 V for LZC),and the Li/LZCS0.25/Li symmetric cell exhibits improved cycling stability.ASSLBs employing LZCS0.25 and LiCoO_(2) or single-crystal LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2) demonstrate high reversible specific capacity and excellent long-term cycling stability.This strategy for regulating the amorphous structure provides valuable guidance for the development of high-performance SSEs for ASSLBs.展开更多
In sulfide-based all-solid-state lithium batteries(ASLBs),the development of high-capacity anode materials with stable interfaces to sulfide solid-state electrolytes(SSEs)is critical.Here,In_(2)O_(3)is explored as an ...In sulfide-based all-solid-state lithium batteries(ASLBs),the development of high-capacity anode materials with stable interfaces to sulfide solid-state electrolytes(SSEs)is critical.Here,In_(2)O_(3)is explored as an anode material for ASLBs for the first time,demonstrating exceptional interfacial stability and electrochemical performance.The In_(2)O_(3)anode,with a substantial mass loading of 7.64 mg cm^(-2),sustains a charge-specific capacity of528.0 mAh g^(-1)(4.03 mAh cm^(-2))at a current density of0.76 mA cm^(-2)over 500 cycles,with a capacity retention of 81.2%.Additionally,it exhibits remarkable long-term cycling stability(2900 cycles)under a high current density of 3.82 mA cm^(-2),with an exceptionally low decay rate of0.016%per cycle.The charge-discharge mechanism of the In_(2)O_(3)anode is elucidated in detail,revealing that the electrochemical evolution of In_(2)O_(3)in ASLBs involves notonly the alloying/dealloying process of indium(In)but also a conversion reaction between In and Li_(2)O.Notably,as cycling progresses,the conversion reaction of In and Li_(2)O diminishes,with the reversible alloy ing/dealloy ing process becoming predominant.This work offers valuable insights for advancing oxide anode materials in sulfide-based ASLBs.展开更多
The present work proposes a novel strategy to fabricate an integrated architecture of gel polymer electrolyte （GPE）-nanoarray cathode for lithium-O2 batteries （LOBs）. As a proof-of-concept experiment, the photo-in...The present work proposes a novel strategy to fabricate an integrated architecture of gel polymer electrolyte （GPE）-nanoarray cathode for lithium-O2 batteries （LOBs）. As a proof-of-concept experiment, the photo-initiated in situ polymerization of GPE was carried out via incorporating the precursor solution in advance into a self- standing binder-free oxygen electrode of Co3O4 nanosheets array grown on carbon cloth （Co3O4@CC）, forming an integrated GPE-Co3O4@CC architecture. The performance of the solid-state LOBs using the GPE-Co3O4@CC assembly is greatly enhanced compared to the counterparts with a traditional cell structure, in which GPE was sandwiched by a lithium metal and a cathode. The enhanced performance is ascribed to the combination of the in situ polymerization of GPE and the versatile structure of nanoarray electrode, which results in abundant interfacial contacts between GPE and electrode. This work presents an alternative way to develop high-performance solid-state LOBs by combining the advantages of both gel polymer electrolytes and nanoarray electrodes.展开更多
Composite solid electrolytes(CSEs)are promising for solid-state Li metal batteries but suffer from inferior room-temperature ionic conductivity due to sluggish ion transport and high cost due to expensive active ceram...Composite solid electrolytes(CSEs)are promising for solid-state Li metal batteries but suffer from inferior room-temperature ionic conductivity due to sluggish ion transport and high cost due to expensive active ceramic fillers.Here,a host–vip inversion engineering strategy is proposed to develop superionic CSEs using cost-effective SiO_(2) nanoparticles as passive ceramic hosts and poly(vinylidene fluoride-hexafluoropropylene)(PVH)microspheres as polymer vips,forming an unprecedented“polymer vip-in-ceramic host”(i.e.,PVH-in-SiO_(2))architecture differing from the traditional“ceramic vip-in-polymer host”.The PVH-in-SiO_(2) exhibits excellent Li-salt dissociation,achieving high-concentration free Li+.Owing to the low diffusion energy barriers and high diffusion coefficient,the free Li+is thermodynamically and kinetically favorable to migrate to and transport at the SiO_(2)/PVH interfaces.Consequently,the PVH-in-SiO_(2) delivers an exceptional ionic conductivity of 1.32.10−3 S cm−1 at 25℃(vs.typically 10−5–10−4 S cm−1 using high-cost active ceramics),achieved under an ultralow residual solvent content of 2.9 wt%(vs.8–15 wt%in other CSEs).Additionally,PVH-in-SiO_(2) is electrochemically stable with Li anode and various cathodes.Therefore,the PVH-in-SiO_(2) demonstrates excellent high-rate cyclability in LiFePO4|Li full cells(92.9%capacity-retention at 3C after 300 cycles under 25℃)and outstanding stability with high-mass-loading LiFePO4(9.2 mg cm−1)and high-voltage NCM622(147.1 mAh g−1).Furthermore,we verify the versatility of the host–vip inversion engineering strategy by fabricating Na-ion and K-ion-based PVH-in-SiO_(2) CSEs with similarly excellent promotions in ionic conductivity.Our strategy offers a simple,low-cost approach to fabricating superionic CSEs for large-scale application of solid-state Li metal batteries and beyond.展开更多
The replacement of liquid electrolyte with solid electrolyte can significantly improve the safety and power/energy density of lithium batteries.70Li_(2)S–30P_(2)S_(5) is one of the most promising solid electrolytes w...The replacement of liquid electrolyte with solid electrolyte can significantly improve the safety and power/energy density of lithium batteries.70Li_(2)S–30P_(2)S_(5) is one of the most promising solid electrolytes with high conductivity for solid–state batteries.In this work,the ionic conductivity and stability toward moisture and lithium metal of 70Li_(2)S–30P_(2)S_(5) were enhanced by introducing the different amounts of Li_(2)O additives.65Li_(2)S–30P_(2)S_(5)–1%Li_(2)O delivered the highest conductivity,while 65Li_(2)S–30P_(2)S_(5)–5%Li_(2)O showed the best moisture stability and improved lithium compatibility.Solid-state batteries using 65Li_(2)S–30P_(2)S_(5)–5%Li_(2)O electrolyte and high-voltage LiNi_(0.6)Mn_(0.2)Co_(0.2)O_(2) cathode exhibited low initial discharge capacity(100 mAh·g^(-1))and Coulombic efficiency(69%).Li_(3)InCl_(6) electrolytes were introduced both in the cathode mixture to replace sulfide electrolyte and in the interface layer to improve the cathode compatibility for the solid-state batteries,showing enhanced discharge capacity(175 mAh·g^(-1))and improved initial Coulombic efficiency(86%).Moreover,it also exhibited good performance at-20℃.展开更多
The rational design of large-area exposure,nonagglomeration,and longrange dispersion of metal nanoparticles(NPs)in the catalysts is critical for the development of energy storage and conversion systems.Little attentio...The rational design of large-area exposure,nonagglomeration,and longrange dispersion of metal nanoparticles(NPs)in the catalysts is critical for the development of energy storage and conversion systems.Little attention has been focused on modulating and developing catalyst interface contact engineering between a carbon substrate and dispersed metal.Here,a highly dispersed ultrafine ruthenium(Ru)NP strategy by double spatial confinement is proposed,that is,incorporating directed growth of metal–organic framework crystals into a bacterial cellulose templating substrate to integrate their respective merits as an excellent electrocatalytic cathode catalyst for a quasi-solid-state Li–O_(2) battery.The porous carbon matrix with highly dispersed ultrafine Ru NPs is well designed and used as cathode catalysts in a Li–O_(2) battery,demonstrating a high discharge areal capacity of 6.82 mAh cm^(–2) at 0.02 mA cm^(–2),a high-rate capability of 4.93 mAh cm^(–2) at 0.2 mA cm^(–2),and stable discharge/charge cycling for up to 500 cycles(2000 h)with low overpotentials of~1.4 V.This fundamental understanding of the structure–performance relationship demonstrates a new and promising approach to optimize highly efficient cathode catalysts for solid-state Li–O_(2) batteries.展开更多
Herein,we first report one-step synthesis of uniform Mo2 C microflowers(MCMFs)from low-cost precursors via industrialized solid-state strategy.With fine optimization in precursor ratio and pyrolysis temperatures,the a...Herein,we first report one-step synthesis of uniform Mo2 C microflowers(MCMFs)from low-cost precursors via industrialized solid-state strategy.With fine optimization in precursor ratio and pyrolysis temperatures,the as-fabricated MCMFs are assembled well with interconnected single-crystalline nanosheet subunits.More encouragingly,the resultant MCMFs are further highlighted as a competitive anode with robust and long-duration lithium-storage behaviors towards high-performance Li-ion batteries.展开更多
A novel transparent and soft quasi-solid-state electrolyte （QSSE） was proposed and fabricated, which consists of ionic liquid （PYR14TFSI） and nano-fumed silica. The QSSE demonstrates high ionic conductivity of 4.6...A novel transparent and soft quasi-solid-state electrolyte （QSSE） was proposed and fabricated, which consists of ionic liquid （PYR14TFSI） and nano-fumed silica. The QSSE demonstrates high ionic conductivity of 4.6× 10-4 S/cm at room temperature and wide electrochemical stability window of over 5 V. The Li-O2 battery using such quasi-solidstate electrolyte exhibits a low charge-discharge overpotential at the first cycle and excellent long-term cyclability over 500 cycles.展开更多
All-solid-state electrolytes are exceedingly attractive because of the outstanding inherent safety and energy density compared to liquid electrolytes.Whereas,it is still formidable to simultaneously design solid elect...All-solid-state electrolytes are exceedingly attractive because of the outstanding inherent safety and energy density compared to liquid electrolytes.Whereas,it is still formidable to simultaneously design solid electrolytes with favorable electrode/electrolyte interface compatibility and high ionic conductivity in a simple and scalable manner.Hence,the oxygen-vacancy-rich Gd-doped SnO_(2) nanotubes(GDS NTs)are innovatively prepared and applied to the electrolyte of all-solid-state lithium metal batteries for the first time.The addition of GDS NTs can validly construct long-range co ntinuous ion transport networks in the poly(ethylene oxide)(PEO)-based system and greatly improve the mechanical properties of the electrolyte.Compared to the PEO-based electrolyte,the composite electrolyte displays a higher lithium ion conductivity of 2.41×10^(-4) S cm^(-1) at 30℃,a higher lithium ion transference number up to 0.62 and a wider electrochemical window of 5 V at 50℃.In addition,the composite electrolyte manifests outstanding compatibility with high-voltage LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811)cathode,LiFePO4 cathode and lithium metal anode.The assembled Li/Li symmetric battery exhibits stable Li plating/stripping cycling performance,which can cycle steadily for 1500 h at a capacity of 0.3 mA h cm^(-2).And Li/LiFePO4 battery still maintains a high capacity of 131.54 mA h g^(-1) at 0.5C after 800 cycles,which has a superior capacity retention rate of 93.2%.The obtained novel composite electrolyte has promising application prospects in the field of all-solid-state lithium metal cells.展开更多
Solid polymer composite electrolytes possess the benefits of superior compatibility with electrodes and good thermal characteristics for more secure energy storage equipment.Herein,a new gel polymer electrolyte(GPE)co...Solid polymer composite electrolytes possess the benefits of superior compatibility with electrodes and good thermal characteristics for more secure energy storage equipment.Herein,a new gel polymer electrolyte(GPE)containing NH_(2)-MIL-53(Al),[PP_(13)][TFSI],LiTFSI,and PVDF-HFP was prepared using a simple method of solution casting.The effects of encapsulating different ratios of ionic liquid([PP_(13)][TFSI])into the micropores of functionalized metal-organic frameworks(NH_(2)-MIL-53(Al))on the electrochemical properties were compared.XRD,SEM,nitrogen adsorption-desorption isotherms,and electrochemical measurements were conducted.This GPE demonstrates a superior ionic conductivity of 8.08×10^(-4)S·cm^(-1)at 60℃and can sustain a discharge specific capacity of 156.6 mA·h·g^(-1)at 0.2 C for over 100 cycles.This work might offer a potential approach to alleviate the solid-solid contact with the solid-state electrolyte and electrodes and broaden a new window for the creation of all-solid-state batteries.展开更多
The recovery and utilization of carbon dioxide(CO_(2))is the key to achieve the targets of peak carbon dioxide emissions and carbon neutrality.The Na-CO_(2)battery made with cheap alkali metal sodium and greenhouse ga...The recovery and utilization of carbon dioxide(CO_(2))is the key to achieve the targets of peak carbon dioxide emissions and carbon neutrality.The Na-CO_(2)battery made with cheap alkali metal sodium and greenhouse gas CO_(2)is an effective strategy to consume CO_(2)and store clean renewable energy.However,the liquid electrolyte volatilization in the open battery system and inevitable dendrite growth restrict the application of Na-CO_(2)batteries.In this work,magnesium-doped Na_(3)Zr_(2)Si_(2)PO_(12)(NZSP)was studied as a solid electrolyte for solid-state Na-CO_(2)batteries.The ionic conductivity of Na_(3.2)Zr_(1.9)Mg_(0.1)Si_(2)PO_(12)reaches 1.16 mS cm^(−1)at room temperature by replacing Zr ions in Na_(3.2)Zr_(1.9)Mg_(0.1)Si_(2)PO_(12)with Mg ions,and the structural changes are analyzed by neutron powder diffraction.The composite electrolyte consisting of highly conductive Na_(3.2)Zr_(1.9)Mg_(0.1)Si_(2)PO_(12)and high processability poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP)is utilized for the first time to assemble a solid-state Na-CO_(2)battery.The cell shows a full discharge capacity of 7720 mAh g^(−1)at 200 mA g^(−1).The middle gap voltage is lower than 2 V after 120 cycles at 200 mA g^(−1)and at a cut-off capacity of 500 mAh g^(−1).This work demonstrates a promising strategy to design high-performance solid-state Na-CO_(2)batteries.展开更多
Solid-state batteries(SSBs)have been considered the most promising technology because of their superior energy density and safety.Among all the solid-state electrolytes(SEs),Li_(7) La_(3) Zr_(2) O_(12)(LLZO)with high ...Solid-state batteries(SSBs)have been considered the most promising technology because of their superior energy density and safety.Among all the solid-state electrolytes(SEs),Li_(7) La_(3) Zr_(2) O_(12)(LLZO)with high ionic conductivity(3×10^(−4) S/cm)has been widely investigated.However,its large-scale production in ambient air faces a challenge.After air exposure,the generated Li_(2)CO_(3) layer deteriorates the ionic conductivity and interfacial wettability,thus greatly compromising the electrochemical performance of SSBs.Many works aim to eliminate this layer to recover the pristine LLZO surface.Unfor-tunately,few articles have emphasized the merits of Li_(2)CO_(3).In this review,we focus on the two-sidedness of Li_(2)CO_(3).We discuss the various characteristics of Li_(2)CO_(3) that can be used and recapitulate the strategies that utilize Li_(2)CO_(3).Insulating Li_(2)CO_(3) is no longer an obstacle but an opportunity for realizing intimate interfacial contact,high air stability,and outstand-ing electrochemical performance.This review aims to off er insightful guidelines for treating air-induced Li_(2)CO_(3) and lead to developing the enhanced air stability and electrochemical performance of LLZO.展开更多
Nonaqueous Li-O2 batteries attract attention for their theoretical specific energy density.However,due to the difficulty of decomposition of Li2 O2,Li-O2 batteries have high charge overpotential and poor cycling life....Nonaqueous Li-O2 batteries attract attention for their theoretical specific energy density.However,due to the difficulty of decomposition of Li2 O2,Li-O2 batteries have high charge overpotential and poor cycling life.So all kinds of catalysts have been studied on the cathode.Compared to heterogeneous solid catalysts,soluble catalysts achieve faster and more effective transport of electrons by reversible redox pairs.Here,we first report ruthenocene(Ruc) as a mobile redox mediator in a Li-O2 battery.0.01 mol/L Ruc in the electrolyte effectively reduces the charging voltage by 610 mV.Additionally,Ruc greatly increases the cycling life by four-fold(up to 83 cycles) with a simple ketjen black(KB) cathode.The results of SEM,XPS and XRD confirm that less discharge product residue accumulated after recharge.To verify the reaction mechanisms of the mediato r,free energy profiles of the possible reaction pathways based on DFT are provided.展开更多
Combining nanomaterials with complementary properties in a well-designed structure is an effective tactic to exploit multifunctional, high-performance materials for the energy conversion and storage. Nonprecious metal...Combining nanomaterials with complementary properties in a well-designed structure is an effective tactic to exploit multifunctional, high-performance materials for the energy conversion and storage. Nonprecious metal catalysts, such as cobalt oxide, with superior activity and excellent stability to other catalysts are widely desired. Nevertheless, the performance of CoO nanoparticles as an electrode material were significantly limit for its inferior conductivity, dissolution, and high cohesion. Herein, we grow ultrafine cobalt monoxide to decorate the interlayer and surface of the Ti3C2 Txnanosheets via a hydrothermal method companied by calcination. The layered MXenes act as the underlying conductive substrate,which not only increase the electron transfer rate at the interface but also greatly improve the electrochemical properties of the nanosized Co O particles by restricting the aggregation of CoO. The resulting CoO/Ti3C2 Txnanomaterial is applied as oxygen electrode for lithium-oxygen battery and achieves more than 160 cycles and first cycle capacity of 16,220 mAh g-1 at 100 mA g-1. This work paves a promising avenue for constructing a bi-functional catalyst by coupling the active component of a transition metal oxide(TMO) with the MXene materials in lithium-oxygen battery.展开更多
Two types of spinel cathode powders, LiMn2O4 and LiAl0.1Mn1.9O3.9F0.1, were synthesized by solid-state reaction, X-ray diffraction （XRD） patterns of the prepared samples were identified as the spinel structure with ...Two types of spinel cathode powders, LiMn2O4 and LiAl0.1Mn1.9O3.9F0.1, were synthesized by solid-state reaction, X-ray diffraction （XRD） patterns of the prepared samples were identified as the spinel structure with a space group of Fd 3^- m. The cubic lattice parameter was determined from least-squares fitting of the XRD data. The LiAl0.1Mn1.9O3.9F0.1 sample showed a little lower initial capacity, but better cycling performance than the LiMn2O4 sample at both room temperature and an elevated temperature. The Vanderbilt method was used to test the electrochemical conductivity of the LiMn2O4 samples. The electrochemical impedance spectroscopy （EIS） method was employed to investigate the electrochemical properties of these spinel LiMn2O4 samples.展开更多
基金supported by a National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(NRF-2020R1A6A1A03043435 and 2020R1A2C1099862)supported by the Korea Institute for Advancement of Technology(KIAT)grant funded by the Korean Government(MOTIE)(P0012451,The Competency Development Program for Industry Specialist)。
文摘2D MXenes,particularly Ti_(3)C_(2)T_(x),have emerged as promising multifu nctional materials for advancing solidstate batteries(SSBs).While SSBs offer superior safety and energy density over liquid-electrolyte systems,critical challenges such as interfacial resistance,limited ion transport,dendrite growth,and mechanical degradation hinder their widespread adoption.This review aims to provide a comprehensive analysis of the roles and fu nctions of Ti_(3)C_(2)T_(x) MXenes in SSBs,emphasizing their application as interlayers,anode/cathode additives,and current collectors,and highlighting their impact on interracial stability,ionic/electro nic transport,electrochemical performance,and cycling durability in SSB architectures.Unlike other 2D materials,Ti_(3)C_(2)T_(x) exhibits outsta nding metallic conductivity,tu nable surface terminations,hydrophilicity,and excellent mechanical flexibility,making it ideal for multifu nctional integration in SSBs,As a component in solid-state electrolytes(SSEs),Ti_(3)C_(2)T_(x) improves ionic conductivity and mecha nical strength.When used in electrodes,it serves as a conductive scaffold that enhances charge transport and structural durability.Additionally,its role as an interfacial interlayer effectively reduces interfacial impedance,accommodates volume changes,and suppresses dendrite formation.Its lightweight and high conductivity enable its use as a current collector.This review highlights recent advances in Ti_(3)C_(2)T_(x)-based components for SSBs like Li-,Na-,Zn,Li-S,etc.,emphasizing enha ncements in ion/electron transport,interfacial stability,and structural robustness.Finally,the review outlines challenges and opportunities along with a future outlook focused on improving the MXene oxidation,tailoring surface terminations,improving long-term stability,and exploring scalable fabrication strategies for MXene-based SSB components.
基金National Natural Science Foundation of China,Grant/Award Number:52272225。
文摘Solid-state sodium batteries(SSSBs)have been highly prized as a promising alternative to conventional battery systems using organic liquid electrolytes due to their improved safety,higher energy density,and substantial resources and low cost of sodium.Na_(3)Zr_(2)Si_(2)PO_(12)(NZSP)solid electrolyte is attracting considerable interest owing to its excellent thermal and chemical stability and favorable compatibility with Na metal anode and high-voltage cathode.However,two main challenges of poor roomtemperature ionic conductivity and high interfacial resistance limit the application of NZSP electrolyte in SSSBs.So far,intensive efforts have been devoted to developing modification strategies to improve the room-temperature ionic conductivity of NZSP.This review aims to provide a comprehensive summary and discussion of some optimization strategies for enhancing the room-temperature ionic conductivity of the NZSP solid electrolyte.These optimization strategies are categorized into foreignion doping or substitution,sintering behavior modulation,and regulation of chemical composition based on precursors,and their optimization mechanisms are also elaborated.Finally,the prospects of NZSP-based solid electrolytes are presented.This review is expected to offer better guidance for designing and developing high-performance NZSP-based solid electrolytes for accelerating the practical application of SSSBs.
基金Funded by the National Natural Science Foundation of China(No.22075035)the Technology Planning Project of Liaoning Province(No.2020JH2/10700008)the Dalian Science and Technology Innovation Fund Project(No.2022JJ11CG005)。
文摘We proposed a strategy to address the issue by synthesizing MnO with half-filled 3 d electron orbitals.That is,MnO nanocubes with an edge length of 61.82 nm were successfully prepared through electros-pinning and one-step pyrolysis as the cathode electrode for Li-O_(2)batteries.It is observed that the intermediate LiMnO_(4)rather than Li_(2)O_(2)is formed when LiO_(2)interactes with MnO(111)during the discharge process.It is precisely because of LiMnO_(4)that reduces its charge overpotential to 0.29 V.The novel reaction mechanism dominated by LiMnO_(4)further facilitates the lower charge overpotential,thereby enhancing the energy efficiency of the batteries.
基金supported by grants from the National Natural Science Foundation of China(Grant Nos.52302303,52472247,52172229,52272201,52072136,51972257)the Natural Science Foundation of Hubei Province(JCZRYB202500537).
文摘Solid-state lithium batteries are considered one of the most promising next-generation energy storage technologies owing to their safety and high energy density.The key to solid-state lithium battery advancement lies in the design and optimization of suitable solid-state electrolytes.Among various solid-state electrolytes,solid-state composite polymer electrolytes offer the combined benefits of solid inorganic electrolytes and solid polymer electrolytes.In particular,Li1_(+x)Al_(x)Ti_(2-x)(PO_(4))_(3)(LATP)/polymer composite polymer electrolytes exhibit high ionic conductivity due to LATP and improved flexibility from the polymer matrix.These systems also demonstrate robust mechanical properties and excellent electrode contact.While recent reviews have primarily focused on the performance of LATP/polymer composite polymer electrolytes and the general effects of composite polymer electrolyte modifications for solid-state lithium battery applications,this review provides a concise overview of the Li^(+)transport mechanisms in LATP/polymer composite polymer electrolytes and strategies to enhance ionic conductivity.It highlights several modification approaches,including the use of fillers,additives,and LATP coatings,which markedly influence the performance of composite polymer electrolytes across different polymer matrices.Finally,the review addresses the challenges of LATP/polymer composite polymer electrolytes and outlines key research directions for developing advanced composite polymer electrolytes for high-performance solid-state lithium batteries.
基金financial support under the scope of the COMET program within the K2 Center“Integrated Computational Material,Process and Product Engineering(IC-MPPE)”(Project ASSESS P1.10)financial support by the Austrian Federal Ministry for Digital and Economic Affairs,the National Foundation for Research,Technology and Development and the Christian Doppler Research Association(Christian Doppler Laboratory for Solid-State Batteries).
文摘Solid-state batteries are attracting considerable attention for their high-energy density and improved safety over conventional lithium-ion batteries.Among solid-state electrolytes,sulfide-based options like Li_(6)PS_(5)Cl are especially promising due to their superior ionic conductivity.However,interfacial degradation between sulfide electrolytes and high-voltage cathodes,such as LiCoO_(2),limits long-term performance.This study demonstrates that a LiBF_(4)-derived F-rich coating on LiCoO_(2),applied by immersing LiCoO_(2) particles in a LiBF_(4) solution followed by annealing,can significantly enhance performance in Li_(6)PS_(5)Cl-based solid-state batteries.This coating enables stable high-voltage(4.5 V vs Li^(+)/Li)operation,achieving an initial specific capacity of 153.82 mAh g^(−1) and 87.1%capacity retention over 300 cycles at 0.5C.The enhanced performance stems from the F-rich coating,composed of multiple phases including LiF,CoF_(2),Li_(x)BF_(y)O_(z),and Li_(x)BO_(y),which effectively suppresses side reactions at the LiCoO_(2)|Li_(6)PS_(5)Cl interface and improves lithium-ion diffusivity,thereby enabling greater Li capacity utilization.Our findings provide a practical pathway for advancing solid-state batteries with high-voltage LiCoO_(2) cathodes,offering substantial promise for next-generation energy storage systems.
文摘Halide solid-state electrolytes(SSEs)with high ionic conductivity and excellent compatibility with highvoltage oxide cathodes in all-solid-state lithium batteries(ASSLBs)offer improved safety and cycling performance.However,the ionic conductivity of halide SSEs at room temperature(RT)and their stability against lithium(Li)metal anodes still require further enhancement.In this study,Li_(2+x)ZrCl_(6-x)S_(x)(0≤x≤1)SSEs,featuring two highly amorphous phases,are synthesized via an aliovalent sulfursubstitution strategy.Notably,a new phase(C2/m),distinct from Li_(2)ZrCl_(6)(LZC)(p3m1),is induced by modulating the sulfur substitution level for chlorine.Consequently,the crystallinity of the coexisting two-phase SSEs is significantly lower than that of the single-phase material.Owing to their highly amorphous nature,the ionic conductivity of Li_(2.25)ZrCl_(5.75)S_(0.25)(LZCS0.25)increases from 0.33 mS cm^(-1)(LZC)to0.97 mS cm^(-1)at RT.In addition,LZCS0.25 exhibits higher compressibility and lower reduction potential(1.78 V vs.2.34 V for LZC),and the Li/LZCS0.25/Li symmetric cell exhibits improved cycling stability.ASSLBs employing LZCS0.25 and LiCoO_(2) or single-crystal LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2) demonstrate high reversible specific capacity and excellent long-term cycling stability.This strategy for regulating the amorphous structure provides valuable guidance for the development of high-performance SSEs for ASSLBs.
基金financially supported by the National Natural Science Foundation of China(No.22301151)the Natural Science Foundation of Inner Mongolia Autonomous Region of China(No.2022QN05024)+1 种基金the Science and Technology Projects of Inner Mongolia Autonomous Region(No.2024SKYPT0011)the Science and Technology Planning Project of Hohhot,China(No.2024-JieBangGuaShuai-Gao-4)
文摘In sulfide-based all-solid-state lithium batteries(ASLBs),the development of high-capacity anode materials with stable interfaces to sulfide solid-state electrolytes(SSEs)is critical.Here,In_(2)O_(3)is explored as an anode material for ASLBs for the first time,demonstrating exceptional interfacial stability and electrochemical performance.The In_(2)O_(3)anode,with a substantial mass loading of 7.64 mg cm^(-2),sustains a charge-specific capacity of528.0 mAh g^(-1)(4.03 mAh cm^(-2))at a current density of0.76 mA cm^(-2)over 500 cycles,with a capacity retention of 81.2%.Additionally,it exhibits remarkable long-term cycling stability(2900 cycles)under a high current density of 3.82 mA cm^(-2),with an exceptionally low decay rate of0.016%per cycle.The charge-discharge mechanism of the In_(2)O_(3)anode is elucidated in detail,revealing that the electrochemical evolution of In_(2)O_(3)in ASLBs involves notonly the alloying/dealloying process of indium(In)but also a conversion reaction between In and Li_(2)O.Notably,as cycling progresses,the conversion reaction of In and Li_(2)O diminishes,with the reversible alloy ing/dealloy ing process becoming predominant.This work offers valuable insights for advancing oxide anode materials in sulfide-based ASLBs.
基金financially supported by the National Natural Science Foundation of China(Nos.21673169 and 51672205)the National Key Research and Development Program of China(No.2016YFA0202602)+1 种基金the Research Start-Up Fund from Wuhan University of Technologythe Fundamental Research Funds for the Central Universities(Nos.2016IVA083 and 2017IB005)
文摘The present work proposes a novel strategy to fabricate an integrated architecture of gel polymer electrolyte （GPE）-nanoarray cathode for lithium-O2 batteries （LOBs）. As a proof-of-concept experiment, the photo-initiated in situ polymerization of GPE was carried out via incorporating the precursor solution in advance into a self- standing binder-free oxygen electrode of Co3O4 nanosheets array grown on carbon cloth （Co3O4@CC）, forming an integrated GPE-Co3O4@CC architecture. The performance of the solid-state LOBs using the GPE-Co3O4@CC assembly is greatly enhanced compared to the counterparts with a traditional cell structure, in which GPE was sandwiched by a lithium metal and a cathode. The enhanced performance is ascribed to the combination of the in situ polymerization of GPE and the versatile structure of nanoarray electrode, which results in abundant interfacial contacts between GPE and electrode. This work presents an alternative way to develop high-performance solid-state LOBs by combining the advantages of both gel polymer electrolytes and nanoarray electrodes.
基金financial support from the National Natural Science Foundation of China(Nos.52250010 and 52201242)the 261 Project of MIIT,Natural Science Foundation of Jiangsu Province(No.BK20240179)the Young Elite Scientists Sponsorship Program by CAST(No.2021QNRC001).
文摘Composite solid electrolytes(CSEs)are promising for solid-state Li metal batteries but suffer from inferior room-temperature ionic conductivity due to sluggish ion transport and high cost due to expensive active ceramic fillers.Here,a host–vip inversion engineering strategy is proposed to develop superionic CSEs using cost-effective SiO_(2) nanoparticles as passive ceramic hosts and poly(vinylidene fluoride-hexafluoropropylene)(PVH)microspheres as polymer vips,forming an unprecedented“polymer vip-in-ceramic host”(i.e.,PVH-in-SiO_(2))architecture differing from the traditional“ceramic vip-in-polymer host”.The PVH-in-SiO_(2) exhibits excellent Li-salt dissociation,achieving high-concentration free Li+.Owing to the low diffusion energy barriers and high diffusion coefficient,the free Li+is thermodynamically and kinetically favorable to migrate to and transport at the SiO_(2)/PVH interfaces.Consequently,the PVH-in-SiO_(2) delivers an exceptional ionic conductivity of 1.32.10−3 S cm−1 at 25℃(vs.typically 10−5–10−4 S cm−1 using high-cost active ceramics),achieved under an ultralow residual solvent content of 2.9 wt%(vs.8–15 wt%in other CSEs).Additionally,PVH-in-SiO_(2) is electrochemically stable with Li anode and various cathodes.Therefore,the PVH-in-SiO_(2) demonstrates excellent high-rate cyclability in LiFePO4|Li full cells(92.9%capacity-retention at 3C after 300 cycles under 25℃)and outstanding stability with high-mass-loading LiFePO4(9.2 mg cm−1)and high-voltage NCM622(147.1 mAh g−1).Furthermore,we verify the versatility of the host–vip inversion engineering strategy by fabricating Na-ion and K-ion-based PVH-in-SiO_(2) CSEs with similarly excellent promotions in ionic conductivity.Our strategy offers a simple,low-cost approach to fabricating superionic CSEs for large-scale application of solid-state Li metal batteries and beyond.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.51821005,21975087,U1966214 and 51902116)the Certificate of China Postdoctoral Science Foundation Grant(No.2019M652634)We gratefully acknowledge the Analytical and Testing Center of HUST for allowing us to use its facilities.
文摘The replacement of liquid electrolyte with solid electrolyte can significantly improve the safety and power/energy density of lithium batteries.70Li_(2)S–30P_(2)S_(5) is one of the most promising solid electrolytes with high conductivity for solid–state batteries.In this work,the ionic conductivity and stability toward moisture and lithium metal of 70Li_(2)S–30P_(2)S_(5) were enhanced by introducing the different amounts of Li_(2)O additives.65Li_(2)S–30P_(2)S_(5)–1%Li_(2)O delivered the highest conductivity,while 65Li_(2)S–30P_(2)S_(5)–5%Li_(2)O showed the best moisture stability and improved lithium compatibility.Solid-state batteries using 65Li_(2)S–30P_(2)S_(5)–5%Li_(2)O electrolyte and high-voltage LiNi_(0.6)Mn_(0.2)Co_(0.2)O_(2) cathode exhibited low initial discharge capacity(100 mAh·g^(-1))and Coulombic efficiency(69%).Li_(3)InCl_(6) electrolytes were introduced both in the cathode mixture to replace sulfide electrolyte and in the interface layer to improve the cathode compatibility for the solid-state batteries,showing enhanced discharge capacity(175 mAh·g^(-1))and improved initial Coulombic efficiency(86%).Moreover,it also exhibited good performance at-20℃.
基金National Natural Science Foundation of China,Grant/Award Number:22179005National Key Research and Development Program of China,Grant/Award Number:2018YFC1900102。
文摘The rational design of large-area exposure,nonagglomeration,and longrange dispersion of metal nanoparticles(NPs)in the catalysts is critical for the development of energy storage and conversion systems.Little attention has been focused on modulating and developing catalyst interface contact engineering between a carbon substrate and dispersed metal.Here,a highly dispersed ultrafine ruthenium(Ru)NP strategy by double spatial confinement is proposed,that is,incorporating directed growth of metal–organic framework crystals into a bacterial cellulose templating substrate to integrate their respective merits as an excellent electrocatalytic cathode catalyst for a quasi-solid-state Li–O_(2) battery.The porous carbon matrix with highly dispersed ultrafine Ru NPs is well designed and used as cathode catalysts in a Li–O_(2) battery,demonstrating a high discharge areal capacity of 6.82 mAh cm^(–2) at 0.02 mA cm^(–2),a high-rate capability of 4.93 mAh cm^(–2) at 0.2 mA cm^(–2),and stable discharge/charge cycling for up to 500 cycles(2000 h)with low overpotentials of~1.4 V.This fundamental understanding of the structure–performance relationship demonstrates a new and promising approach to optimize highly efficient cathode catalysts for solid-state Li–O_(2) batteries.
基金financial support from National Natural Science Foundation of China(Nos.51772127,51772131,51802119)Taishan Scholars(No.ts201712050)Major Program of Shandong Province Natural Science Foundation(No.ZR2018ZB0317)。
文摘Herein,we first report one-step synthesis of uniform Mo2 C microflowers(MCMFs)from low-cost precursors via industrialized solid-state strategy.With fine optimization in precursor ratio and pyrolysis temperatures,the as-fabricated MCMFs are assembled well with interconnected single-crystalline nanosheet subunits.More encouragingly,the resultant MCMFs are further highlighted as a competitive anode with robust and long-duration lithium-storage behaviors towards high-performance Li-ion batteries.
基金Project supported by the National Key R&D Program of China(Grant Nos.2016YFB0100300 and 2016YFB0100100)the National Basic Research Program of China(Grant No.2014CB932300)+2 种基金the Beijing Municipal Science&Technology Commission,China(Grant No.D171100005517001)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDA09010000)the National Natural Science Foundation of China(Grant No.51502334)
文摘A novel transparent and soft quasi-solid-state electrolyte （QSSE） was proposed and fabricated, which consists of ionic liquid （PYR14TFSI） and nano-fumed silica. The QSSE demonstrates high ionic conductivity of 4.6× 10-4 S/cm at room temperature and wide electrochemical stability window of over 5 V. The Li-O2 battery using such quasi-solidstate electrolyte exhibits a low charge-discharge overpotential at the first cycle and excellent long-term cyclability over 500 cycles.
基金supported by the National Natural Science Foundation of China(52203066,51973157,61904123,51873152)the Tianjin Natural Science Foundation(18JCQNJC02900)+3 种基金the Science and Technology Plans of Tianjin(19PTSYJC00010)the Tianjin Research Innovation Project for Postgraduate Students(2021YJSB234)the Science&Technology Development Fund of Tianjin Education Commission for Higher Education(2018KJ196)State Key Laboratory of Membrane and Membrane Separation,Tiangong University。
文摘All-solid-state electrolytes are exceedingly attractive because of the outstanding inherent safety and energy density compared to liquid electrolytes.Whereas,it is still formidable to simultaneously design solid electrolytes with favorable electrode/electrolyte interface compatibility and high ionic conductivity in a simple and scalable manner.Hence,the oxygen-vacancy-rich Gd-doped SnO_(2) nanotubes(GDS NTs)are innovatively prepared and applied to the electrolyte of all-solid-state lithium metal batteries for the first time.The addition of GDS NTs can validly construct long-range co ntinuous ion transport networks in the poly(ethylene oxide)(PEO)-based system and greatly improve the mechanical properties of the electrolyte.Compared to the PEO-based electrolyte,the composite electrolyte displays a higher lithium ion conductivity of 2.41×10^(-4) S cm^(-1) at 30℃,a higher lithium ion transference number up to 0.62 and a wider electrochemical window of 5 V at 50℃.In addition,the composite electrolyte manifests outstanding compatibility with high-voltage LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811)cathode,LiFePO4 cathode and lithium metal anode.The assembled Li/Li symmetric battery exhibits stable Li plating/stripping cycling performance,which can cycle steadily for 1500 h at a capacity of 0.3 mA h cm^(-2).And Li/LiFePO4 battery still maintains a high capacity of 131.54 mA h g^(-1) at 0.5C after 800 cycles,which has a superior capacity retention rate of 93.2%.The obtained novel composite electrolyte has promising application prospects in the field of all-solid-state lithium metal cells.
基金financially supported by National Natural Science Foundation of China(21701083)Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX20_3137)。
文摘Solid polymer composite electrolytes possess the benefits of superior compatibility with electrodes and good thermal characteristics for more secure energy storage equipment.Herein,a new gel polymer electrolyte(GPE)containing NH_(2)-MIL-53(Al),[PP_(13)][TFSI],LiTFSI,and PVDF-HFP was prepared using a simple method of solution casting.The effects of encapsulating different ratios of ionic liquid([PP_(13)][TFSI])into the micropores of functionalized metal-organic frameworks(NH_(2)-MIL-53(Al))on the electrochemical properties were compared.XRD,SEM,nitrogen adsorption-desorption isotherms,and electrochemical measurements were conducted.This GPE demonstrates a superior ionic conductivity of 8.08×10^(-4)S·cm^(-1)at 60℃and can sustain a discharge specific capacity of 156.6 mA·h·g^(-1)at 0.2 C for over 100 cycles.This work might offer a potential approach to alleviate the solid-solid contact with the solid-state electrolyte and electrodes and broaden a new window for the creation of all-solid-state batteries.
基金supported by Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(Grant No.2022-K15)China University of Mining&Technology(Beijing),Beijing National Laboratory for Condensed Matter Physics,and the National Natural Science Foundation of China(No.51672029 and 51372271)the Spanish Ministry of Science,Innovation to the project MAT2017-84496-R.CAL acknowledges ANPCyT,UNSL for financial support(projects PICT2017-1842,PROICO 2-2016),Argentine.
文摘The recovery and utilization of carbon dioxide(CO_(2))is the key to achieve the targets of peak carbon dioxide emissions and carbon neutrality.The Na-CO_(2)battery made with cheap alkali metal sodium and greenhouse gas CO_(2)is an effective strategy to consume CO_(2)and store clean renewable energy.However,the liquid electrolyte volatilization in the open battery system and inevitable dendrite growth restrict the application of Na-CO_(2)batteries.In this work,magnesium-doped Na_(3)Zr_(2)Si_(2)PO_(12)(NZSP)was studied as a solid electrolyte for solid-state Na-CO_(2)batteries.The ionic conductivity of Na_(3.2)Zr_(1.9)Mg_(0.1)Si_(2)PO_(12)reaches 1.16 mS cm^(−1)at room temperature by replacing Zr ions in Na_(3.2)Zr_(1.9)Mg_(0.1)Si_(2)PO_(12)with Mg ions,and the structural changes are analyzed by neutron powder diffraction.The composite electrolyte consisting of highly conductive Na_(3.2)Zr_(1.9)Mg_(0.1)Si_(2)PO_(12)and high processability poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP)is utilized for the first time to assemble a solid-state Na-CO_(2)battery.The cell shows a full discharge capacity of 7720 mAh g^(−1)at 200 mA g^(−1).The middle gap voltage is lower than 2 V after 120 cycles at 200 mA g^(−1)and at a cut-off capacity of 500 mAh g^(−1).This work demonstrates a promising strategy to design high-performance solid-state Na-CO_(2)batteries.
基金the support from the National Natural Science Foundation of China (Nos.U2001220 and 51902223)the Haihe Laboratory of Sustainable Chemical Transformations+2 种基金the Fundamental Research Funds for the Central Universitiesthe National Key Research and Development Program of China (Nos.2021YFF0500600 and 2019YFE0118800)the Natural Science Foundation of Tianjin (No.20JCYBJC00850)
文摘Solid-state batteries(SSBs)have been considered the most promising technology because of their superior energy density and safety.Among all the solid-state electrolytes(SEs),Li_(7) La_(3) Zr_(2) O_(12)(LLZO)with high ionic conductivity(3×10^(−4) S/cm)has been widely investigated.However,its large-scale production in ambient air faces a challenge.After air exposure,the generated Li_(2)CO_(3) layer deteriorates the ionic conductivity and interfacial wettability,thus greatly compromising the electrochemical performance of SSBs.Many works aim to eliminate this layer to recover the pristine LLZO surface.Unfor-tunately,few articles have emphasized the merits of Li_(2)CO_(3).In this review,we focus on the two-sidedness of Li_(2)CO_(3).We discuss the various characteristics of Li_(2)CO_(3) that can be used and recapitulate the strategies that utilize Li_(2)CO_(3).Insulating Li_(2)CO_(3) is no longer an obstacle but an opportunity for realizing intimate interfacial contact,high air stability,and outstand-ing electrochemical performance.This review aims to off er insightful guidelines for treating air-induced Li_(2)CO_(3) and lead to developing the enhanced air stability and electrochemical performance of LLZO.
基金the National Natural Science Foundation of China (Nos.U1732111 and 21676241)“The Recruitment Program of Global Youth Experts” from the Chinese government+2 种基金the “Hundred Talents Program” of Zhejiang UniversityHubei Natural Science Foundation of China (No.2018CFB531)Self-determined Research Funds of CCNU from Colleges’ Basic Research and Operation of MOE (No.CCNU18TS045)。
文摘Nonaqueous Li-O2 batteries attract attention for their theoretical specific energy density.However,due to the difficulty of decomposition of Li2 O2,Li-O2 batteries have high charge overpotential and poor cycling life.So all kinds of catalysts have been studied on the cathode.Compared to heterogeneous solid catalysts,soluble catalysts achieve faster and more effective transport of electrons by reversible redox pairs.Here,we first report ruthenocene(Ruc) as a mobile redox mediator in a Li-O2 battery.0.01 mol/L Ruc in the electrolyte effectively reduces the charging voltage by 610 mV.Additionally,Ruc greatly increases the cycling life by four-fold(up to 83 cycles) with a simple ketjen black(KB) cathode.The results of SEM,XPS and XRD confirm that less discharge product residue accumulated after recharge.To verify the reaction mechanisms of the mediato r,free energy profiles of the possible reaction pathways based on DFT are provided.
基金supported by the National Natural Science Foundations of China (Grants:21871028,21771024)。
文摘Combining nanomaterials with complementary properties in a well-designed structure is an effective tactic to exploit multifunctional, high-performance materials for the energy conversion and storage. Nonprecious metal catalysts, such as cobalt oxide, with superior activity and excellent stability to other catalysts are widely desired. Nevertheless, the performance of CoO nanoparticles as an electrode material were significantly limit for its inferior conductivity, dissolution, and high cohesion. Herein, we grow ultrafine cobalt monoxide to decorate the interlayer and surface of the Ti3C2 Txnanosheets via a hydrothermal method companied by calcination. The layered MXenes act as the underlying conductive substrate,which not only increase the electron transfer rate at the interface but also greatly improve the electrochemical properties of the nanosized Co O particles by restricting the aggregation of CoO. The resulting CoO/Ti3C2 Txnanomaterial is applied as oxygen electrode for lithium-oxygen battery and achieves more than 160 cycles and first cycle capacity of 16,220 mAh g-1 at 100 mA g-1. This work paves a promising avenue for constructing a bi-functional catalyst by coupling the active component of a transition metal oxide(TMO) with the MXene materials in lithium-oxygen battery.
基金This work was financially supported by the National Natural Science Foundation of China (No.50272012).
文摘Two types of spinel cathode powders, LiMn2O4 and LiAl0.1Mn1.9O3.9F0.1, were synthesized by solid-state reaction, X-ray diffraction （XRD） patterns of the prepared samples were identified as the spinel structure with a space group of Fd 3^- m. The cubic lattice parameter was determined from least-squares fitting of the XRD data. The LiAl0.1Mn1.9O3.9F0.1 sample showed a little lower initial capacity, but better cycling performance than the LiMn2O4 sample at both room temperature and an elevated temperature. The Vanderbilt method was used to test the electrochemical conductivity of the LiMn2O4 samples. The electrochemical impedance spectroscopy （EIS） method was employed to investigate the electrochemical properties of these spinel LiMn2O4 samples.
