Progress in Solid State Chemistry最新文献

{"title":"Synergistic ligand-antisolvent modulation for selective CsPbBr3 perovskite synthesis and functional diversity","authors":"Mengping Wang,&nbsp;Shiyu Wang,&nbsp;Xinxin Liu,&nbsp;Zhenyi Yu,&nbsp;Guangjiu Zhao","doi":"10.1016/j.progsolidstchem.2026.100598","DOIUrl":"10.1016/j.progsolidstchem.2026.100598","url":null,"abstract":"<div><div>In this work, we propose a ligand–antisolvent synergistic regulation strategy to synthesize Cs–Pb–Br materials with dual antibacterial and encryption functions. An amphiphilic ligand derived from 5-bromovaleric acid (5-BVA) and oleamide (OAm) is employed with two green antisolvents (water and ethanol). The use of water as an antisolvent yields high-purity CsPbBr₃ quantum dots (QDs) with water stability exceeding 50 days. These QDs exhibit potent antibacterial activity through electrostatic interactions with bacterial cell membranes achieving up to 99.8% inhibition at a low concentration of 120 μg/ml. In contrast, ethanol as the antisolvent leads to a mixed CsPbBr₃/CsPb₂Br₅ phase. This mixed phase exhibits water-triggered fluorescence activation originating from CsPbBr₃ recrystallization alongside a thermal quenching effect that enables reversible on–off fluorescence switching upon cooling–heating cycles. This water-induced fluorescence activation effect combined with reversible thermal quenching properties enables multi-level encryption. Ultimately this ligand-antisolvent synergistic regulation strategy not only offers theoretical guidance for the rational and tailored design of multifunctional perovskites but also establishes a foundation for their practical applications in complex optoelectronic and biological environments.</div></div>","PeriodicalId":415,"journal":{"name":"Progress in Solid State Chemistry","volume":"84 ","pages":"Article 100598"},"PeriodicalIF":9.7,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148573475","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synergistic boosting of luminescence intensity in Sr3Lu(PO4)3:Cr3+ via B-site substitution and energy transfer toward multifunctional near-infrared applications","authors":"Chao Wei,&nbsp;Jingyu Ran,&nbsp;Jie Zhang","doi":"10.1016/j.progsolidstchem.2026.100609","DOIUrl":"10.1016/j.progsolidstchem.2026.100609","url":null,"abstract":"<div><div>The wideband near-infrared (NIR) phosphors for next-generation intelligent NIR light sources are becoming a research hotspot in the field of luminescent materials due to their potential applications in optical sensing, biological imaging, and smart lighting. This study reports a Cr³⁺-activated A₃B(PO₄)₃-type (Sr₃Lu(PO₄)₃), abbreviated as SLP) near-infrared phosphor. Under 466 nm blue light excitation, SLP:Cr³⁺ phosphor exhibits a broad near-infrared emission from 700 to 1200 nm with a peak wavelength at 860 nm, a full width at half maximum (FWHM) of 141 nm, and an initial quantum yield of 31.48%. Structural and spectroscopic characterization confirms that Cr³⁺ preferentially occupies the octahedral coordination sites of Lu³⁺ in the matrix, forming a weak crystal field environment that favors the spin-allowed ⁴T₂→⁴A₂ transition of Cr³⁺, leading to broad near-infrared emission. Additionally, by substituting Y³⁺ for the B-site (Lu³⁺ site), the luminescent intensity of the material is significantly enhanced, and the quantum yield is increased to 81.53%. Furthermore, the introduction of Yb³⁺ constructs a Cr³⁺→Yb³⁺ energy transfer system, further optimizing the luminescent performance. Although the phosphor exhibits severe thermal quenching, the packaged near-infrared phosphor-converted light-emitting diodes (NIR pc-LEDs) maintain a low surface temperature of 59.5 °C at 500 mA, ensuring reliable operation. The phosphor also exhibits excellent temperature sensitivity (max relative sensitivity: 3.33%·K⁻¹) for fluorescence thermometry. Practical applications including invisible QR code encryption, night vision, biological imaging, and long-distance illumination are demonstrated, showcasing the versatility of the developed NIR pc-LED. This work provides a high-performance NIR phosphor candidate for multi-functional smart light sources.</div></div>","PeriodicalId":415,"journal":{"name":"Progress in Solid State Chemistry","volume":"84 ","pages":"Article 100609"},"PeriodicalIF":9.7,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148958552","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Protonation-state engineering enables low-temperature and phase-selective synthesis of lanthanide tellurites and high-entropy derivatives","authors":"Yiyun Wang,&nbsp;Hong-Bo Cui,&nbsp;Guijian Guan,&nbsp;Ming-Yong Han","doi":"10.1016/j.progsolidstchem.2026.100611","DOIUrl":"10.1016/j.progsolidstchem.2026.100611","url":null,"abstract":"<div><div>Phase selection in multicomponent oxides is frequently constrained by sluggish solid-state diffusion and competing reaction pathways. Here, acid–base control of solution-precipitated lanthanide tellurite precursors is used as a kinetic strategy for the low-temperature, phase-selective formation of Ln₂Te₆O₁₅ and Ln₂Te₄O₁₁ (Ln = lanthanide). Varying the LnCl₃:Na₂TeO₃:HCl ratio defines four nominal precursor regimes: non-protonated Ln₂(TeO₃)₃, partially protonated Ln(TeO₃)(HTeO₃), highly protonated Ln(HTeO₃)₃, and an over-protonated H₂TeO₃/TeO₂-rich boundary. Across the productive 2:3:0–1:3:3 window, increasing nominal protonation lowers the crystallization temperature of La₂Te₆O₁₅ from 600 to 420 °C and the minimum temperature for XRD-phase-pure La₂Te₄O₁₁ formation from 840 to 540 °C after 6 h. Excessive protonation disrupts the connected Ln–Te–O precursor network and yields TeO₂-rich products. The approach is applicable to all 14 nonradioactive lanthanides examined and enables equimolar 14-cation high-entropy derivatives with homogeneous elemental distributions. Rietveld refinements support the targeted cubic and monoclinic structures, while Yb³⁺/Er³⁺ codoping links the precursor-controlled phase pathway to structural order and upconversion emission. To our knowledge, the resulting series includes the first single-lanthanide preparations of Ln₂Te₆O₁₅ for Ln = Ce, Er, Tm, Yb, and Lu, as well as the first 14-cation (La–Lu)₂Te₆O₁₅ and (La–Lu)₂Te₄O₁₁ derivatives. These results establish precursor protonation as a practical kinetic handle for phase-selective synthesis of compositionally complex oxides at reduced temperatures.</div></div>","PeriodicalId":415,"journal":{"name":"Progress in Solid State Chemistry","volume":"84 ","pages":"Article 100611"},"PeriodicalIF":9.7,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149159109","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Solid-state chemical evolution and stabilization of high-voltage O3-type Ni-Fe-Mn layered cathodes for sodium-ion batteries","authors":"Yanshan Wu,&nbsp;Xiang Li,&nbsp;Zhongren Zhou,&nbsp;Xiaoyuan Zeng,&nbsp;Yingjie Zhang,&nbsp;Jie Xiao,&nbsp;Yubo Xing,&nbsp;Peng Dong","doi":"10.1016/j.progsolidstchem.2026.100608","DOIUrl":"10.1016/j.progsolidstchem.2026.100608","url":null,"abstract":"<div><div>O3-type nickel-iron-manganese layered oxides are promising cathode materials for sodium-ion batteries because of their high sodium content, tunable transition-metal redox chemistry, and potential for high energy density. However, when operated at high charging voltages, deep sodium extraction strongly perturbs the layered framework and induces coupled structural, chemical, interfacial, and mechanical degradation. This review summarizes the solid-state chemical evolution of O3-type nickel-iron-manganese cathodes under high-voltage conditions. Particular attention is given to sodium-vacancy rearrangement, transition-metal layer gliding, O3–P3-related phase transitions, cation migration, oxygen-framework instability, surface reconstruction, cathode-electrolyte interphase evolution, transition-metal dissolution, and particle cracking. These degradation processes are discussed as an interconnected failure chain rather than isolated phenomena. Recent stabilization strategies, including bulk doping, interlayer regulation, surface modification, electrolyte optimization, high-entropy design, and data-driven screening, are compared in terms of their effects on phase-transition reversibility, metal-oxygen bonding, oxygen stability, interfacial chemistry, and particle integrity. The review further emphasizes that high-voltage capacity should be evaluated together with structural reversibility, interfacial stability, and full cell compatibility. Future development of O3-type nickel-iron-manganese cathodes requires mechanism-matched multiscale design and practical validation in sodium-ion full cells under realistic testing conditions.</div></div>","PeriodicalId":415,"journal":{"name":"Progress in Solid State Chemistry","volume":"84 ","pages":"Article 100608"},"PeriodicalIF":9.7,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148958558","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A-site cation engineering of Mn5+-activated ABaPO4 (A=Li, Na, K) phosphors for high-performance NIR-II luminescence and optical thermometry","authors":"Yutong Wang,&nbsp;Hang Zhao,&nbsp;Jiayin Niu,&nbsp;Anurak Weahayee,&nbsp;Wanwisa Limphirat,&nbsp;Theeranun Siritanon,&nbsp;Jingyi Ren,&nbsp;Peng Jiang,&nbsp;Yanfei Sun,&nbsp;Tingting Lu","doi":"10.1016/j.progsolidstchem.2026.100603","DOIUrl":"10.1016/j.progsolidstchem.2026.100603","url":null,"abstract":"<div><div>The development of high-performance narrowband near-infrared second window (NIR-II) phosphors remains a critical challenge in the fields of advanced bioimaging and optical thermometry. Herein, a series of Mn⁵⁺-doped ABaPO₄ (A = Li, Na, K) phosphors are synthesized via conventional solid-state method, and the effect of A-site alkali metal cations on their crystal structure and luminescence properties is comparatively investigated. Mn <em>K</em>-edge X-ray absorption near-edge structure (XANES) spectroscopy unambiguously confirms that Mn ions are predominantly stabilized in the +5 oxidation state and exclusively occupy tetrahedral [PO₄] sites in all three hosts. All samples exhibit characteristic narrowband NIR-II emission in the 1160-1200 nm range originating from the ¹E → ³A₂ spin-forbidden transition of Mn⁵⁺. The lattice distortion induced by different A-site cations significantly modulates the doping limit, crystal field strength, thermal stability and temperature sensing performance of Mn⁵⁺ ions. All three Mn⁵⁺-doped hosts exhibit good thermal stability. The fluorescence decay lifetime of LiBaPO₄: Mn⁵⁺ reaches 772.436 μs＀ NaBaPO₄: Mn⁵⁺ shows unique energy level splitting and achieves a maximum relative temperature sensitivity of 2.43% K⁻¹ based on the fluorescence intensity ratio technique. KBaPO₄: Mn⁵⁺ possesses a highly symmetric crystal lattice and a higher doping limit, with a thermal quenching activation energy (<em>ΔE</em>) of 0.414 eV. This work not only provides three promising NIR-II phosphors for bioimaging and optical thermometry, but also offers new insights into the research of Mn⁵⁺-activated phosphate systems.</div></div>","PeriodicalId":415,"journal":{"name":"Progress in Solid State Chemistry","volume":"84 ","pages":"Article 100603"},"PeriodicalIF":9.7,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148573477","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Mechanically reinforced NASICON electrolytes co-doped with Sc3+ and Mg2+ for dendrite-resistant sodium metal batteries","authors":"Yuhan Yi,&nbsp;Qiao Wang,&nbsp;Chuang Yu,&nbsp;Liping Li,&nbsp;Xin Zhang,&nbsp;Guangshe Li","doi":"10.1016/j.progsolidstchem.2026.100606","DOIUrl":"10.1016/j.progsolidstchem.2026.100606","url":null,"abstract":"<div><div>Both the electrochemical and mechanical properties of solid-state electrolytes are crucial for achieving stable battery performance, while the widely studied NASICON-type electrolytes such as Na₃Zr₂Si₂PO₁₂ (NZSP) still suffer from poor conductivity and a tendency to Na metal penetration. To address these problems simultaneously, we propose an integrated chemistry-structure-mechanics design principle, in which aliovalent Sc/Mg co-doping (chemistry) regulates lattice framework and grain-boundary evolution (structure), thereby enhancing mechanical robustness (mechanics) without compromising ionic transport. The optimized sample (Na_3.4Zr_1.7Sc_0.2Mg_0.1Si₂PO₁₂) achieves a high room-temperature conductivity of 1.26 × 10⁻³ S cm⁻¹ and a 25% increase in hardness compared with the Mg-free analogue. The solid-state cell assembled with this electrolyte (Na/Na_3.4Zr_1.7Sc_0.2Mg_0.1Si₂PO₁₂/Na₃V₂(PO₄)₃) shows excellent cycling stability in a wide temperature range of 0-80 °C, and retains 90% of its initial capacity after 440 cycles at 30 °C and 1C. These results demonstrate that aliovalent co-doping to concurrently optimize lattice chemistry and ceramic microstructure is an effective route to high-performance NASICON electrolytes.</div></div>","PeriodicalId":415,"journal":{"name":"Progress in Solid State Chemistry","volume":"84 ","pages":"Article 100606"},"PeriodicalIF":9.7,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148844051","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Localized lone pair structural representation (LPSR): A transferable framework for ns2 lone-pair stereochemistry from electronic localization to crystal architecture","authors":"Jean Galy,&nbsp;Alicia Castro,&nbsp;Samir F. Matar","doi":"10.1016/j.progsolidstchem.2026.100610","DOIUrl":"10.1016/j.progsolidstchem.2026.100610","url":null,"abstract":"<div><div>Stereo chemically active ns² lone pairs play a major role in determining the local geometry and, in many cases, the extended architecture of crystal structures. Their structural consequences are well established, while electronic-structure methods such as Density Functional Theory (DFT) and the Electron Localization Function (ELF) provide increasingly detailed descriptions of their spatial localization. However, a transferable structural representation connecting localized lone-pair electron density with crystallographic geometry and extended crystal architecture remains lacking. Here we propose the Localized Lone Pair Structural Representation (LPSR) as a stereochemical descriptor framework for spatially localized ns² lone pairs. LPSR distinguishes E, the structural representation of the stereochemical region associated with the localized lone pair, from Ec, the electronically determined center of that region, and incorporates its spatial extent and directionality through a stereochemical volume. The framework is supported by a systematic analysis of chemically diverse ns² systems, including molecular and extended structures. In SF₄E, the close correspondence between E and ELF-derived Ec provides a direct link between the structural representation and electronic localization. Across a broad family of M*X₃E systems, the recurrence of the same spatial relationship among the central cation, coordinating atoms and the stereochemical region demonstrates the transferability of the proposed stereochemical motif. Representative structures of SeO₂, SnO and BiF₃ further show how local stereochemical motifs can be followed into chains, channels, layers and extended frameworks. The resulting hierarchy (electronic localization → Ec → stereochemical volume → stereochemical motif → motif organization → crystal architecture) provides a common structural language for relating electronic localization to crystallographic structure across chemically diverse systems. LPSR is intended as a representational framework rather than a replacement for crystallography, electronic-structure methods or established bonding models. Its principal contribution is to make the stereochemical organization of localized lone pairs explicit and transferable across structural scales.</div></div>","PeriodicalId":415,"journal":{"name":"Progress in Solid State Chemistry","volume":"84 ","pages":"Article 100610"},"PeriodicalIF":9.7,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149050998","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Structural engineering in carbon allotropes (SECA): A model for the solid-state chemist","authors":"Samir F. Matar","doi":"10.1016/j.progsolidstchem.2026.100605","DOIUrl":"10.1016/j.progsolidstchem.2026.100605","url":null,"abstract":"<div><div>Besides machine learned programs of structure prediction and AI driven ones, another direction for the search of novel carbon allotropes is proposed herein with the ‘structural engineering in carbon allotropes’ (SECA) operating model. SECA embeds the control of dimensionality, bonding topology, architecture, … and involves tools and rationales in solid-state chemistry helped with crystallography and support from quantum mechanics calculations of the ground state structures and the energy dependent physical properties. After a contextual introduction, methods and physical properties analysis tools, SECA offers an illustrative case study where, besides devising high symmetry 3D tetragonal C₃₂ allotropes with original (not documented) topologies, a step ahead is made with the proposition of a pressure induced phase transition from the mixed trigonal-tetrahedral Csp²/Csp³ hybridization allotrope (α-C₃₂) to insulating β-C₃₂ made of only Csp³ tetrahedral hybridization, leading to significant densification. Such findings were based on establishing the respective energy-volume equations of states (EOS) leading to a transition pressure close to 40 GPa. Both allotropes present stable mechanical, dynamic and thermal properties with the sp³ β-C₃₂ presenting specific heat C_V = f(T) calculated curve in good agreement with diamond experimental data. Electronic band structures show a transition from a low band gap semiconductor α-C₃₂ to insulating β-C₃₂ like diamond. In so far that “material = matter + properties”, such rationalized research in solid state chemistry can be considered at the forefront of Materials Science, which holds much promise for the near future.</div></div>","PeriodicalId":415,"journal":{"name":"Progress in Solid State Chemistry","volume":"84 ","pages":"Article 100605"},"PeriodicalIF":9.7,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148658283","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Metal–organic framework-derived selenium-doped manganese oxide@carbon composite for durable aqueous zinc-ion batteries","authors":"Ashok Kumar Kakarla,&nbsp;Hari Bandi,&nbsp;R. Shanthappa,&nbsp;Wasim Akram Syed,&nbsp;Jae Su Yu","doi":"10.1016/j.progsolidstchem.2026.100604","DOIUrl":"10.1016/j.progsolidstchem.2026.100604","url":null,"abstract":"<div><div>Manganese (Mn)-based materials, owing to their high theoretical capacity, low cost, environmental benignity, and multiple accessible valence states, are attractive cathode candidates for aqueous zinc-ion batteries (AZIBs). However, their practical application is often hindered by intrinsically sluggish electron transport, slow Zn²⁺ diffusion kinetics, and structural instability associated with Jahn–Teller distortion during cycling. Herein, we reported a heterostructured manganese selenide/manganese oxide@carbon (MnSe/MnO@C) composite derived from metal-organic frameworks (MOFs) via a simple thermolysis of Mn MOFs under an inert atmosphere, followed by selenization. The carbonization of Mn MOFs generates a carbonaceous framework favorable for charge transport, while the formation of the heterostructured MnSe/MnO@C introduces abundant heterointerfaces and electrochemically active sites. These structural features are consistent with the reduced charge-transfer resistance and enhanced reaction kinetics observed for the MnSe/MnO@C electrode. Furthermore, when used as the cathode material for AZIBs, the MnSe/MnO@C electrode revealed superior specific capacity and improved cyclability, exhibiting 225 mA h g⁻¹ at 0.5 A g⁻¹ after 500 charge-discharge cycles. Surprisingly, the electrode could achieve a reversible specific capacity of 191 mA h g⁻¹ at 2 A g⁻¹. The ex-situ characterization indicates a mixed Zn²⁺/H⁺ co-storage mechanism accompanied by reversible structural evolution without causing significant morphological damage. This study provides insights into the synthesis of MnSe/MnO@C, electrochemical activation, and remarkable AZIB performances, which leads to a better understanding of its potential applications.</div></div>","PeriodicalId":415,"journal":{"name":"Progress in Solid State Chemistry","volume":"84 ","pages":"Article 100604"},"PeriodicalIF":9.7,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148573480","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Decoupling the physical and chemical interfacial failure mechanisms in sulfide-based ASSBs using zero-strain LTO anodes as a mechanistic probe","authors":"Ziyu Lu,&nbsp;Jiuwei Lei,&nbsp;Lin Li,&nbsp;Siwu Li,&nbsp;Miao Deng,&nbsp;Shiyu Liu,&nbsp;Wen Yin,&nbsp;Wei Xia,&nbsp;Wenqian Tian,&nbsp;Chuang Yu","doi":"10.1016/j.progsolidstchem.2026.100607","DOIUrl":"10.1016/j.progsolidstchem.2026.100607","url":null,"abstract":"<div><div>Zero-strain Li₄Ti₅O₁₂ (LTO) anode is repurposed as a mechanistic probe to decouple interfacial failure modes in sulfide-based all-solid-state batteries. Neutron diffraction reveals multi-site Li⁺ occupancy and Br-induced local structural disorder in the LPSCB (Li_5.5PS_4.5Cl_0.8Br_0.7) electrolyte. Combined DFT calculations, solid-state NMR, in situ EIS, and GITT confirm that the LTO/LPSCB interface is intrinsically chemically inert, with a binding energy of −0.41 eV, a net charge transfer of only ∼0.024 e, and no detectable macroscopic Li⁺ exchange across the interface. Electrochemically, the LTO anode delivers high reversible capacity, excellent long-term stability (79.3% retention after 300 cycles at 1C), and robust rate capability even at elevated temperatures, with a Li⁺ diffusion coefficient (10⁻⁵–10⁻⁹ cm² s⁻¹) substantially surpassing those of graphite and silicon. In full-cell comparisons, the LTO-based cell shows the lowest polarization overpotential and negligible volume change (−0.2%), whereas graphite and silicon anodes suffer from severe interfacial cracking and contact loss. The spinel framework and redox reversibility of LTO remain intact, confirming minimal chemical degradation at the anode/electrolyte interface. When benchmarked against graphite and high-strain silicon anodes, the zero-strain LTO cell exhibits negligible volume change and intact interfacial contact, establishing that mechanical strain is the dominant driver of interfacial degradation. A strain–chemistry coupled design framework is thereby established, providing a quantitative pathway for decoupling failure mechanisms toward durable sulfide-based all-solid-state batteries.</div></div>","PeriodicalId":415,"journal":{"name":"Progress in Solid State Chemistry","volume":"84 ","pages":"Article 100607"},"PeriodicalIF":9.7,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148958553","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}