Superior Air Stability Research Articles

Controlled growth of asymmetric chiral TeOx for broad-spectrum, high-responsivity and polarization-sensitive photodetection.

Low-dimensional nanostructures, especially one-dimensional materials, exhibit remarkable anisotropic characteristics due to their low symmetry, making them promising candidates for polarization-sensitive photodetection. Here, we present a chemical vapor deposition synthesis method for tellurium suboxide (TeOx), confirming the practicality of photodetectors constructed from TeOx nanowires (NWs) in high-responsivity, broadband, and polarization-sensitive detection. By precisely controlling the thermodynamics and kinetics of TeOx NWs growth, we achieve large-scale growth of TeOx NWs with highly controllable dimensions and propose a method to induce intrinsic built-in strain in TeOx NWs. Photodetectors based on quasi-one-dimensional TeOx NWs with ohmic contact demonstrate broadband spectral response (638-1550nm), high responsivity (13 700 mA·W-1), and superior air stability. Particularly, owing to the inherent structural anisotropy of the photodetectors, they exhibit polarization-sensitive photodetection, with anisotropy ratios of 1.70 and 1.71 at 638 and 808nm, respectively.

Mo6+ bifunctional substitution of P2-type manganese oxide for high performance sodium-ion batteries

Due to its cost-effectiveness and high specific capacity, P2-type manganese (Mn) oxide is considered a highly promising cathode material for sodium ion batteries (SIBs). However, the practical application of this material is hindered by poor cyclic stability caused by the phase transition of P2-P’2 due to the Jahn-Teller effect of Mn3+ at low voltage and significant volume changes at high voltage. In this study, we utilized Mo6+ dual-function P2-Na0.67Mn0.99Mo0.01O1.997(PO4)0.0008 (NMMPO-1) to achieve exceptional magnification performance and cycle stability. Advanced electron microscopy and X-ray diffraction analysis revealed that Mo6+ acts as a pillar in replacing interlayer Na+ sites within the P2 phase, resulting in extended layer spacing and a stable crystal structure. Additionally, Mo6+ substitution for Mn3+ weakens the Jahn-Teller distortion effect of Mn3+. Ex-situ X-ray diffraction experiments demonstrated that NMMPO-1 effectively inhibits the P2-P’2 phase transition at low voltage while minimizing volume changes during charge–discharge cycles. Overall, our modified NMMPO-1 exhibits excellent cycle stability with 144.55 mA h g−1 after 100 cycles at 0.5C, retaining 83 % capacity retention rate, along with impressive rate performance achieving capacity of 100.57 mA h g−1 at 5C. Furthermore, NMMPO-1 demonstrates superior air stability compared to unmodified samples when exposed to air over multiple cycles. Moreover, through detailed analysis using electrochemical impedance spectroscopy (EIS), cyclic voltammetry (CV), and galvanostatic intermittent titration technique (GITT) curves; it is observed that NMMPO-1 possesses enhanced Na+ diffusion capacity and kinetic properties compared to other materials. This research provides novel insights into the role of substituting high valence cations in layered Mn oxide materials which can contribute towards designing improved performance for future sodium ion battery applications.

Nitrogen doped sulfide solid electrolytes with enhanced air stability and lithium metal compatibility

AbstractCompared with oxide, halide, and polymer‐based solid electrolytes, Li‐ion conducting sulfide solid electrolytes exhibit remarkable ionic conductivity, electronic conductivity, and exceptional thermal and mechanical properties. Despite these advantages, the susceptibility of sulfide electrolytes to air and the formation of lithium dendrites on the anode hinder their large‐scale commercial application. In this study, we propose a doping strategy involving the nitrogen (N) element in sulfide electrolyte Li5.5PS4.5Cl1.5 (LPSCl) with inherently high ionic conductivity. We have successfully synthesized Li5.5+xPS4.5−xNxCl1.5(x = .025, .05, .07, .10) solid electrolytes by enhancing their air stability through doping. The modified electrolyte material demonstrates stable cycling performance exhibiting superior air stability compared to Li5.5PS4.5Cl1.5. The results indicate that the doped sulfide solid electrolyte effectively suppresses the growth of lithium dendrites, thereby enhancing the compatibility between the lithium metal anode and sulfide solid electrolyte.

A Functional Air-Stable Li9.8GeP1.7Sb0.3S11.8I0.2 Superionic Conductor for High-Performance All-Solid-State Lithium Batteries.

Solid-state electrolytes (SSEs) based on sulfides have become a subject of great interest due to their superior Li-ion conductivity, low grain boundary resistance, and adequate mechanical strength. However, they grapple with chemical instability toward moisture hypersensitivity, which decreases their ionic conductivity, leading to more processing requirements. Herein, a Li9.8GeP1.7Sb0.3S11.8I0.2 (LGPSSI) superionic conductor is designed with a Li+ conductivity of 6.6 mS cm-1 and superior air stability based on hard and soft acids and bases (HSAB) theory. The introduction of optimal antimony (Sb) and iodine (I) into the Li10GeP2S12 (LGPS) structure facilitates fast Li-ion migration with low activation energy (Ea) of 20.33 kJ mol-1. The higher air stability of LGPSSI is credited to the strategic substitution of soft acid Sb into (Ge/P)S4 tetrahedral sites, examined by Raman and X-ray photoelectron spectroscopy techniques. Relatively lower acidity of Sb compared to phosphorus (P) realizes a stronger Sb-S bond, minimizing the evolution of toxic H2S (0.1728 cm3 g-1), which is ∼3 times lower than pristine LGPS when LGPSSI is exposed to moist air for 120 min. The NCA//Li-In full cell with a LGPSSI superionic conductor delivered the first discharge capacity of 209.1 mAh g-1 with 86.94% Coulombic efficiency at 0.1 mA cm-2. Furthermore, operating at a current density of 0.3 mA cm-2, LiNbO3@NCA/LGPSSI/Li-In cell demonstrated an exceptional reversible capacity of 117.70 mAh g-1, retaining 92.64% of its original capacity over 100 cycles.

Thickness‐Dependent Crystal Structure, Synthesis, and Magnetism of Thin Film Chromium Chalcogenides: A Review

AbstractIn the search for two‐dimensional (2D) magnets operating under ambient conditions, quasi‐2D non‐van der Waals (vdW) materials have attracted considerable research interest over the last five years. In addition to their high Curie temperature (TC), their superior air stability to that of vdW 2D magnets has made them potential candidates for future room‐temperature spintronics applications. Furthermore, recent progress in the thickness‐dependent crystal lattice and magnetic properties of non‐vdW Cr2X3 (X = S, Se, or Te) has brought them to areas that are once set aside for 2D vdW magnets in fundamental research and applications. Despite covalent bonding between magnetic layers, various bottom‐up synthesis methods produced thickness‐controlled flakes of Cr2X3. Moreover, layer‐dependent structural and magnetic properties are among the novel research directions in these materials. This review systematically summarizes recent studies on Cr2X3 crystal structure, their controllable synthesis, and their respective magnetic properties. A summary of some significant results on thickness‐controlled synthesis in Cr2X3 and thickness‐dependent magnetism in Cr2Te3 is presented. Additionally, experimental and theoretical reports are presented to explain interlayer magnetic interaction. The work reveals the interaction between synthesis, structure, and magnetism. Finally, future research directions of new Cr2X3‐based materials, rich magnetism in Cr2X3, and their potential application are discussed.

Lattice Engineering on Li2CO3-Based Sacrificial Cathode Prelithiation Agent for Improving the Energy Density of Li-Ion Battery Full-Cell.

Developing sacrificial cathode prelithiation technology to compensate for active lithium loss is vital for improving the energy density of lithium-ion battery full-cells. Li2CO3 owns high theoretical specific capacity, superior air stability, but poor conductivity as an insulator, acting as a promising but challenging prelithiation agent candidate. Herein, extracting a trace amount of Co from LiCoO2 (LCO), a lattice engineering is developed through substituting Li sites with Co and inducing Li defects to obtain a composite structure consisting of (Li0.906Co0.043▫0.051)2CO2.934 and ball milled LiCoO2 (Co-Li2CO3@LCO). Notably,both the bandgap and Li─O bond strength have essentially declined in this structure. Benefiting from the synergistic effect of Li defects and bulk phase catalytic regulation of Co, the potential of Li2CO3 deep decomposition significantly decreases from typical >4.7 to ≈4.25V versus Li/Li+, presenting >600 mAh g-1 compensation capacity. Impressively, coupling 5 wt% Co-Li2CO3@LCO within NCM-811 cathode, 235Wh kg-1 pouch-type full-cell is achieved, performing 88% capacity retention after 1000 cycles.

Aqueous tape casting phosphate ceramic electrolyte membrane for high performance all solid-state lithium metal battery

Li1.3Al0.3Ti1.7(PO4)3 (LATP) solid electrolyte has caused great attention because of its low cost, high ionic conductivity, and superior air stability. In this work, high quality LATP ceramic electrolyte membranes are fabricated by an aqueous tape casting technique in the air, in contrast to traditional fabrication methods that are usually inefficient and noncontinuous, this technique provides an environment-friendly, scalable, continuous fabrication route for mass production of ceramic electrolyte membranes. The as-prepared LATP ceramic membrane with a relative density of 95.6 % shows a total Li ionic conductivity of 3.8 × 10−4 S cm−1. Simply coated with a flexible polymer electrolyte film on the surface of the LATP ceramic membrane, the solid-solid interfacial polarization between the LATP ceramic membrane and the electrodes can be well controlled under a reasonable level, leading to excellent battery performance. Discharge capacities of 160.6, 157.6, 151.2, 138.9 and 123.9 mAh g−1 at 0.05, 0.1, 0.2, 0.5 and 1 C rates are achieved, respectively. This study demonstrates a promising strategy for commercializing all-solid-state batteries with a cost-effective and scalable manufacturing technique.

Zero-Dimensional Hybrid Antimony Chloride with Near-Unity Broad-Band Orange-Red Emission toward Solid-State Lighting.

Zero-dimensional (0D) hybrid metal halides are attractive owing to their distinctive structure as well as photoluminescence (PL) characteristics. To discover 0D hybrid metal halides with high photoluminescence quantum yield and good stability is of great significance for white light-emitting diodes (LEDs). Herein, a novel hybrid antimony chloride (CTP)2SbCl5 is synthesized, which shows a bright broad-band orange-red emission peaking at 620 nm under the low energy excitation (365 nm), achieving an excellent photoluminescence quantum yield of 96.8%. In addition, (CTP)2SbCl5 shows an additional emission peaking at 470 nm when excited at high energy (323 nm). PL spectra and density functional theory results demonstrate that the observed dual-band emission originates from the singlet and triplet self-trapped excitons confined in isolated [SbCl5]2- square pyramids. Moreover, (CTP)2SbCl5 presents relatively superior air stability, and the PL intensity still maintains 78% of the initial PL intensity when exposed to the air for above 2 weeks. Benefiting from high-efficiency PL emission and good stability of (CTP)2SbCl5, a stable warm white LED device with a 92.3% color rendering index was prepared by coating blue phosphor BaMgAl10O17:Eu2+, green (Sr,Ba)2SiO4:Eu2+, and orange-red (CTP)2SbCl5 on a 365 nm LED chip. This work provides an efficient luminescent material and also demonstrates the potential application of 0D hybrid antimony chloride in solid-state lighting.

Polarization-Sensitive Photodetector Based on High Crystallinity Quasi-1D BiSeI Nanowires Synthesized via Chemical Vapor Deposition.

Bismuth chalcohalides (BiSeI and BiSI), a class of superior light absorbers, have recently garnered great attention owing to their promise in constructing next-generation optoelectronic devices. However, to date, the photodetection application of bismuth chalcohalides is still limited due to the challenge in controllable preparation. Herein, the synthesis of large-scale quasi-1D BiSeI nanowires via chemical vapor deposition growth is reported. By precisely tuning the growth temperature and the Se supply, it can effectively control the growth thermodynamics and kinetics of BiSeI crystal, and thus achieve high purity quasi-1D BiSeI nanowires with high crystal quality, uniform diameter, and tunable domain length. Theory and optical characterizations of the quasi-1D BiSeI nanowires reveal an indirect bandgap of 1.57eV with prominent optical linear dichroism. As a result, the quasi-1D BiSeI nanowire-based photodetector demonstrates a broadband photoresponse (400-800nm) with high responsivity of 5880mAW-1 , fast response speed of 0.11ms and superior air stability. More importantly, the photodetector displays strong polarization sensitivity (anisotropic ratio = 1.77) under the 532nm light irradiation. This work will provide important guides to the synthesis of other quais-1D metal chalcohalides and shed light on their potential in constructing novel multifunctional optoelectronic devices.

Quantum Dot-Siloxane Anchoring on Colloidal Quantum Dot Film for Flexible Photovoltaic Cell.

Lead sulfide (PbS) colloidal quantum dots (CQDs) are promising materials for next-generation flexible solar cells because of near-infrared absorption, facile bandgap tunability, and superior air stability. However, CQD devices still lack enough flexibility to be applied to wearable devices owing to the poor mechanical properties of CQD films. In this study, a facile approach is proposed to improve the mechanical stability of CQDs solar cells without compromising the high power conversion efficiency (PCE) of the devices. (3-aminopropyl)triethoxysilane (APTS) is introduced on CQD films to strengthen the dot-to-dot bonding via QD-siloxane anchoring, and as a result, crack pattern analysis reveals that the treated devices become robust to mechanical stress. The device maintains 88% of the initial PCE under 12000 cycles at a bending radius of 8.3mm. In addition, APTS forms a dipole layer on CQD films, which improves the open circuit voltage (VOC ) of the device, achieving a PCE of 11.04%, one of the highest PCEs in flexible PbS CQD solar cells.

Air-Stable Violet Phosphorus/MoS2 van der Waals Heterostructure for High-Responsivity and Gate-Tunable Photodetection.

Violet phosphorus (VP), a newly emerging elemental 2D semiconductor, with attractive properties such as tunable bandgap, high carrier mobility, and unusual structural anisotropy, offers significant opportunities for designing high-performance electronic and optoelectronic devices. However, the study on fundamental property and device application of 2D VP is seriously hindered by its inherent instability in ambient air. Here, a VP/MoS2 van der Waals heterostructure is constructed by vertically staking few-layer VP and MoS2 , aiming to utilize the synergistic effect of the two materials to achieve a high-performance 2D photodetector. The strong optical absorption of VP combining with the type-II band alignment of VP/MoS2 heterostructure make VP play a prominent photogating effect. As a result, the VP/MoS2 heterostructure photodetector achieves an excellent photoresponse performances with ultrahigh responsivity of 3.82 × 105 AW-1 , high specific detectivity of 9.17 × 1013 Jones, large external quantum efficiency of 8.91 × 107 %, and gate tunability, which are much superior to that of individual MoS2 device or VP device. Moreover, the VP/MoS2 heterostructure photodetector indicates superior air stability due to the effective protection of VP by MoS2 encapsulation. This work sheds light on the future study of the fundamental property and optoelectronic device application of VP.

In-situ constructed SnO2 gradient buffer layer as a tight and robust interphase toward Li metal anodes in LATP solid state batteries

Li1.3Al0.3Ti1.7(PO4)3 (LATP), of much interest owing to its high ionic conductivity, superior air stability, and low cost, has been regarded as one of the most promising solid-state electrolytes for next-generation solid-state lithium batteries (SSLBs). Unfortunately, the commercialization of SSLBs is still impeded by severe interfacial issues, such as high interfacial impedance and poor chemical stability. Herein, we proposed a simple and convenient in-situ approach to constructing a tight and robust interface between the Li anode and LATP electrolyte via a SnO2 gradient buffer layer. It is firmly attached to the surface of LATP pellets due to the volume expansion of SnO2 when in-situ reacting with Li metal, and thus effectively alleviates the physical contact loosening during cycling, as confirmed by the mitigated impedance rising. Meanwhile, the as-formed SnO2/Sn/LixSn gradient buffer layer with low electronic conductivity successfully protects the LATP electrolyte surface from erosion by the Li metal anode. Additionally, the LixSn alloy formed at the Li surface can effectively regulate uniform lithium deposition and suppress Li dendrite growth. Therefore, this work paves a new way to simultaneously address the chemical instability and poor physical contact of LATP with Li metal in developing low-cost and highly stable SSLBs.

Benzothiadiazole versus Thiazolobenzotriazole: A Structural Study of Electron Acceptors in Solution-Processable Organic Semiconductors.

Despite the rapid progress of organic electronics, developing high-performance n-type organic semiconductors is still challenging. Donor-acceptor (D-A) type conjugated structures have been an effective molecular design strategy to achieve chemically-stable semiconductors and the appropriate choice of the acceptor units determines the electronic properties and device performances. We have now synthesized two types of A1 -D-A2 -D-A1 type conjugated molecules, namely, NDI-BTT-NDI and NDI-TBZT-NDI, with different central acceptor units. In order to investigate the effects of the central acceptor units on the charge-transporting properties, organic field-effect transistors (OFETs) were fabricated. NDI-TBZT-NDI had shallower HOMO and deeper LUMO levels than NDI-BTT-NDI. Hence, the facilitated charge injection resulted in ambipolar transistor performances with the optimized hole and electron mobilities of 0.00134 and 0.151 cm2 V-1 s-1 , respectively. In contrast, NDI-BTT-NDI displayed only an n-channel OFET performance with the electron mobility of 0.0288 cm2 V-1 s-1 . In addition, the device based on NDI-TBZT-NDI showed a superior air stability to that based on NDI-BTT-NDI. The difference in these OFET performances was reasonably explained by the contact resistance and film morphology. Overall, this study demonstrated that the TBZ acceptor is a promising building block to create n-type organic semiconductors.

Red@Black phosphorus core–shell heterostructure with superior air stability for high-rate and durable sodium-ion battery

Heterostructured electrodes have gained increasing attentions owing to the synergistic effects from individual building components and the unique interfaces. However, rational design and controllable fabrication of high areal capacity and durable phosphorus-based heterostructure anode for industry remains a critical challenge. Herein, a new red@black phosphorus core–shell heterostructure anchored on three-dimensional N-doped graphene (RP@BP/3DNG) has been prepared via a facile one-step solvothermal strategy. As demonstrated by experimental data and theoretical calculations, RP@BP/3DNG shows a superior high electronic conductivity and an extremely low Na+ diffusion barrier due to the build-in filed at the RP@BP heterointerface, thus RP@BP/3DNG delivers an ultra-high areal capacity of 3.46 mAh cm−2 (1440.2 mAh/g at 0.05 A/g), impressive rate performance (521.3 mAh/g at 10.0 A/g) as well as unprecedented capacity retention rate of 89.3% after 1200 cycles at 10.0 A/g when evaluated as an anode for sodium ion batteries (SIBs). Furthermore, the internal electric field at the interfaces of RP@BP leads to the shift of electron cloud from BP to RP, which greatly suppresses the reaction activity of lone-pair electrons of BP atoms, and therefore RP@BP/3DNG shows much enhanced air stability. This work heralds a new insight for designing high-performance and stable P-based anodes for rechargeable batteries.

Anomalous displacement reaction for synthesizing above-room-temperature and air-stable vdW ferromagnet PtTe2Ge1/3.

Emerging van der Waals (vdW) magnets provide a paradise for the exploration of magnetism in the ultimate two-dimensional (2D) limit, and the construction of integrated spintronic devices, and have become a research frontier in the field of low-dimensional materials. To date, prototypical vdW magnets based on metals of the first transition series (e.g. V, Cr, Mn and Fe) and chalcogen elements suffer from rapid oxidation restricted by the Hard-Soft-Acid-Base principle, as well as low Curie temperatures (T C), which has become a generally admitted challenge in 2D spintronics. Here, starting from air-unstable Cr2Ge2Te6 vdW thin flakes, we synthesize Ge-embedded PtTe2 (namely PtTe2Ge1/3) with superior air stability, through the displacement reaction in the Cr2Ge2Te6/Pt bilayer. In this process, the anomalous substitution of Cr with Pt in the thermal diffusion is inverse to the metal activity order, which can be attributed to the compatibility between soft-acid (Pt) and soft-base (Te) elements. Meanwhile, the layered uniform insertion of Ge unbalances Pt-Te bonds and introduces long-range ordered ferromagnetism with perpendicular magnetic anisotropy and a Curie temperature above room temperature. Our work demonstrates the anti-metal-activity-order reaction tendency unique in 2D transition-metal magnets and boosts progress towards practical 2D spintronics.

In Situ Synthesis and Dual Functionalization of Nano Silicon Enabled by a Semisolid Lithium Rechargeable Flow Battery.

Nanosized silicon has attracted considerable attentions as a new-generation anode material for lithium-ion batteries (LIBs) due to its exceptional theoretical capacity and reasonable cyclic stability. However, serious side reactions often take place at the nanosized silicon/electrolyte interface in LIBs, where critical electrochemical properties such as initial Coulombic efficiency (ICE) are compromised. On the basis of this feature, a new method is developed to synthesize nanosilicon-based particles in a facile, scalable way, which are endowed with the function of prelithiation and storage stability in air. A semisolid lithium rechargeable flow battery (SSFB) technology is used for the first time to convert the micrometer-sized silicon raw material into an amorphous-nanosilicon-based material (ANSBM), as a result of the pulverization process induced by the repeated lithiation/delithiation cycles. The particle size is successfully reduced from 1-4 μm to around 30 nm after cycles in the flow battery. Bulk functionalization of the nano silicon is introduced by the unbalanced lithiation/delithiation cyclic process, which endows ANSBM with a unique prelithiation capability universally applicable to different anode systems such as nanosized Si, SiOx, and graphite, as evidenced by the significantly improved ICEs. Superior air stability (10% relative humidity) is exhibited by ANSBM due to surface functionalization by the stable interfacial layer encapsulated by electron-conductive carbon. The outcome of this work provides a promising way to synthesize dual-functionalized nano silicon with good electrochemical performance in terms of improved capacity and increased initial Coulombic efficiency when it is composited with other typical anode materials.

Novel Ultrabright and Air‐Stable Photocathodes Discovered from Machine Learning and Density Functional Theory Driven Screening (Adv. Mater. 44/2021)

Photocathode Materials The discovery of high-brightness photocathode materials can considerably expand the capabilities of X-ray free-electron laser facilities. In article number 2104081, Evan R. Antoniuk, Evan J. Reed, and co-workers perform a comprehensive screening of over 74 000 materials to identify novel photocathode candidates. The newly discovered materials are demonstrated to achieve higher brightness and superior air stability than the current state-of-the-art.

Novel Ultrabright and Air-Stable Photocathodes Discovered from Machine Learning and Density Functional Theory Driven Screening.

The high brightness, low emittance electron beams achieved in modern X-ray free-electron lasers (XFELs) have enabled powerful X-ray imaging tools, allowing molecular systems to be imaged at picosecond time scales and sub-nanometer length scales. One of the most promising directions for increasing the brightness of XFELs is through the development of novel photocathode materials. Whereas past efforts aimed at discovering photocathode materials have typically employed trial-and-error-based iterative approaches, this work represents the first data-driven screening for high brightness photocathode materials. Through screening over 74 000 semiconducting materials, a vast photocathode dataset is generated, resulting in statistically meaningful insights into the nature of high brightness photocathode materials. This screening results in a diverse list of photocathode materials that exhibit intrinsic emittances that are up to 4x lower than currently used photocathodes. In a second effort, multiobjective screening is employed to identify the family of M2 O (M = Na, K, Rb) that exhibits photoemission properties that are comparable to the current state-of-the-art photocathode materials, but with superior air stability. This family represents perhaps the first intrinsically bright, visible light photocathode materials that are resistant to reactions with oxygen, allowing for their transport and storage in dry air environments.

Facile Fabrication of Highly Stable and Wavelength-Tunable Tin Based Perovskite Materials with Enhanced Quantum Yield via the Cation Transformation Reaction

Metal halide perovskites have attracted great attention for their superior light energy conversion applications. Herein, we demonstrated a facile synthesis of zero-dimensional Sn2+ perovskite Cs4-xMxSnBr6(M = K+ and Rb+) material through the cation transformation reaction at room temperature. Cs4SnBr6 NCs was mixed with pure metal bromide salts (KBr and RbBr) via the mechanochemical process to successfully synthesize Cs4-xMxSnBr6 perovskite where transformation of Cs to mixed Cs/Rb and mixed Cs/K was achieved. By substituting different cations, the bright fluorescence of the Cs4-xMxSnBr6 was tuned from dim green to greenish-cyan while achieving the photoluminescence (PL) quantum yield of ∼39%. The crystal structure of Sn based perovskite with the substitution of K+ or Rb+ cations was determined by X-ray diffraction (XRD). Moreover, the Cs4-xMxSnBr6 demonstrated superior air stability and exhibited a better photocatalytic activity for CO2 reduction reaction (CO2RR) with high selectivity of CH4 gas with a higher yield rate compared to the pristine Cs4SnBr6 NCs.

Progress and perspective of Li1 + xAlxTi2‐x(PO4)3 ceramic electrolyte in lithium batteries

AbstractThe replacement of liquid organic electrolytes with solid‐state electrolytes (SSEs) is a feasible way to solve the safety issues and improve the energy density of lithium batteries. Developing SSEs materials that can well match with high‐voltage cathodes and lithium metal anode is quite significant to develop high‐energy‐density lithium batteries. Li1 + xAlxTi2 ‐ x(PO4)3 (LATP) SSE with NASICON structure exhibits high ionic conductivity, low cost and superior air stability, which enable it as one of the most hopeful candidates for all‐solid‐state batteries (ASSBs). However, the high interfacial impedance between LATP and electrodes, and the severe interfacial side reactions with the lithium metal greatly limit its applications in ASSBs. This review introduces the crystal structure and ion transport mechanisms of LATP and summarizes the key factors affecting the ionic conductivity. The side reaction mechanisms of LATP with Li metal and the promising strategies for optimizing interfacial compatibility are reviewed. We also summarize the applications of LATP including as surface coatings of cathode particles, ion transport network additives and inorganic fillers of composite polymer electrolytes. At last, this review proposes the challenges and the future development directions of LATP in SSBs.image