Mohammad Ali Badragheh , Vanessa Miß , Bernhard Roling , Michael Vogel
{"title":"Effects of disorder on the energy landscape and motional mechanisms involved in lithium ion dynamics and transport in solid electrolytes: Li5.5PS4.5Cl1.5 argyrodite as a case study","authors":"Mohammad Ali Badragheh , Vanessa Miß , Bernhard Roling , Michael Vogel","doi":"10.1016/j.ssi.2025.116903","DOIUrl":"10.1016/j.ssi.2025.116903","url":null,"abstract":"<div><div><sup>7</sup>Li NMR diffusometry and relaxometry are combined with electrochemical impedance spectroscopy to compare the mechanisms for the dynamics and transport of lithium ions in disordered and crystalline electrolytes with argyrodite composition Li<sub>5.5</sub>PS<sub>4.5</sub>Cl<sub>1.5</sub>. The <em>dc</em> conductivity of a disordered sample prepared by ball milling amounts to 0.76 mScm<sup>−1</sup> at room temperature, which is substantially lower than that of two previously studied crystalline argyrodites differing in the order of the anion sublattice due to various heat treatments. However, the activation energy of the <em>dc</em> conductivity is smaller for ball-milled disordered Li<sub>5.5</sub>PS<sub>4.5</sub>Cl<sub>1.5</sub> (<span><math><msub><mi>E</mi><mi>dc</mi></msub><mo>=</mo></math></span> 0.35 eV) than for both crystalline compounds (<span><math><msub><mi>E</mi><mi>dc</mi></msub><mo>=</mo></math></span> 0.38 eV). <sup>7</sup>Li NMR field-gradient measurements of the self-diffusion coefficient <span><math><mi>D</mi></math></span> and its activation energy <span><math><msub><mi>E</mi><mi>D</mi></msub></math></span> confirm these findings and, furthermore, reveal different Haven ratios. <sup>7</sup>Li NMR field-cycling relaxometry shows that the lithium ion jumps in ball-milled Li<sub>5.5</sub>PS<sub>4.5</sub>Cl<sub>1.5</sub> are described by very broad dynamical susceptibilities arising from a temperature-independent Gaussian-like distribution of activation energies <span><math><mi>g</mi><mfenced><msub><mi>E</mi><mi>a</mi></msub></mfenced></math></span> with a mean value of <span><math><msub><mi>E</mi><mi>m</mi></msub><mo>=</mo></math></span> 0.43 eV, while the susceptibilities indicated a high-energy cutoff for the crystalline electrolytes. Based on different relations between the activation energies for the conductivity, diffusivity and jumps, we discuss that the shape and exploration of the energy landscapes of ball-milled and crystalline Li<sub>5.5</sub>PS<sub>4.5</sub>Cl<sub>1.5</sub> samples strongly differ. Moreover, significant differences in the preexponential factor of the <em>dc</em> conductivity, the Haven ratio and the single-particle correlation factor point to distinct types of anion lattice disorder of the ball-milled disordered and heat-treated crystalline samples.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"427 ","pages":"Article 116903"},"PeriodicalIF":3.0,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144124657","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Intrinsic limitation of conductivity in depolymerized sodium-ion glassy networks","authors":"L. Legrand, L.-M. Poitras, N. Sator, M. Micoulaut","doi":"10.1016/j.ssi.2025.116889","DOIUrl":"10.1016/j.ssi.2025.116889","url":null,"abstract":"<div><div>The electric properties of a model fast-ion electrolyte glass (100-<span><math><mi>x</mi></math></span>)SiS<span><math><msub><mrow></mrow><mn>2</mn></msub></math></span> – <span><math><mi>x</mi></math></span>Na<span><math><msub><mrow></mrow><mn>2</mn></msub></math></span>S are investigated by means of classical molecular dynamics simulations. These materials are promising candidates for battery applications and the conductivity is thought to be essentially driven by the concentration of Na charge carriers. We first set up a Buckingham-Coulomb type potential able to describe the atomic structure and experimental structure functions (structure factor) in an improved fashion with respect to previous reported force fields. A systematic investigation of properties with modifier content Na<span><math><msub><mrow></mrow><mn>2</mn></msub></math></span>S (50 %<span><math><mo>≤</mo><mi>x</mi><mo>≤</mo></math></span>80 %) leads to an unexpected result, that is, a near constant behavior of the conductivity <span><math><mi>σ</mi><mfenced><mi>x</mi></mfenced></math></span> with Na<span><math><msub><mrow></mrow><mn>2</mn></msub></math></span>S increase for various isotherms in the liquid state. The analysis indicates that unlike Li-based electrolytes, the diffusivity ratio between network (Si,S) and modifier (Na) species is reduced, of about 6–8, and differs substantially with the corresponding lithium counterpart for which the same ratio is about 100. This leads to a contribution to conductivity dominated by (Si,S) atoms for the sodium system. While the concentration of network species in the range 66 %<span><math><mo>≤</mo><mi>x</mi><mo>≤</mo></math></span>80 % decreases, no dramatic increase in Na diffusivity is obtained, and the emergence of molecular Na<span><math><msub><mrow></mrow><mn>2</mn></msub></math></span>S in the structure at large modifier content also induces profound structural changes. Unlike Lithium glassy electrolytes, the design of Na-based batteries must, therefore, take into account the contribution of the network species.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"427 ","pages":"Article 116889"},"PeriodicalIF":3.0,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144097828","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Compatibility between Li1.5Al0.5Ge1.5(PO4)3-based solid electrolyte and LiNi1/3Co1/3Mn1/3O2 cathode","authors":"S.V. Pershina","doi":"10.1016/j.ssi.2025.116896","DOIUrl":"10.1016/j.ssi.2025.116896","url":null,"abstract":"<div><div>All-solid-state batteries (ASSBs) have a higher energy density and improved safety compared to traditional lithium-ion batteries. The problem of high interface resistance between the solid electrolyte and electrode materials needs to be addressed for the ASSBs production. Solid electrolytes of the Li<sub>1.5</sub>Al<sub>0.5</sub>Ge<sub>1.5</sub>(PO<sub>4</sub>)<sub>3</sub> (LAGP) family with the NASICON-type structure possess a high lithium-ion conductivity and stability in air. In this work, Si-modified LAGP glass-ceramics (LAGSP) with a total Li<sup>+</sup> conductivity of 3·10<sup>−4</sup> S cm<sup>−1</sup> at 25 °C and a compact microstructure is considered. LiNi<sub>1/3</sub>Co<sub>1/3</sub>Mn<sub>1/3</sub>O<sub>2</sub> (NCM) is a promising cathode material which offers a high specific capacity and better cycle performance. Chemical interaction between the above-mentioned components at high temperature for the solid-solid interface creation was studied. The thermal behavior of the mechanical mixture of solid electrolyte and cathode material was studied by DSC method at temperatures of up to 900 °C. The phase composition of their mechanical mixture after heat treatment at different temperatures (500, 730 and 800 °C) was investigated by XRD. It was shown that the structure of the initial phases did not change after heat treatment at 500 °C. However, Li<sub>3</sub>PO<sub>4</sub>, Li<sub>4</sub>P<sub>2</sub>O<sub>7</sub>, NiAl<sub>2</sub>O<sub>4</sub> and GeO<sub>2</sub> phases begin to appear after annealing at 730 °C, while Co<sub>2</sub>MnO<sub>4</sub>, LiCoPO<sub>4</sub>, SiO<sub>2</sub>, GeO<sub>2</sub>, Li<sub>3</sub>PO<sub>4</sub> and Li<sub>9</sub>Al<sub>3</sub>(P<sub>2</sub>O<sub>7</sub>)<sub>3</sub>(PO<sub>4</sub>)<sub>2</sub> formation was observed at 800 °C. Heating at 800 °C leads to a complete degradation of the solid electrolyte. Therefore, it was proposed to create a LAGSP | NCM interface using a liquid electrolyte. LiPF<sub>6</sub>-based liquid electrolyte was used as a buffer layer between solid electrolyte and cathode for enhancing the interfacial contact. Symmetrical NCM | solid electrolyte | NCM and NCM |LiPF<sub>6</sub> | solid electrolyte | LiPF<sub>6</sub> | NCM cells are assembled and their resistance at room temperature is measured. It was established that modified cells had the lowest resistance at room temperature (1.2 kΩ·cm<sup>2</sup>) compared to unmodified cells (162 kΩ·cm<sup>2</sup>).</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"427 ","pages":"Article 116896"},"PeriodicalIF":3.0,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144098908","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Sodium hydrosulfide hydrate as sodium precursor for low-cost synthesis of Na3SbS4 ionic conductor","authors":"Pierre Gibot, Christine Surcin, Jean-Noël Chotard","doi":"10.1016/j.ssi.2025.116892","DOIUrl":"10.1016/j.ssi.2025.116892","url":null,"abstract":"<div><div>Solid-state batteries (SSBs), an alternative to liquid-electrolyte lithium/sodium batteries, are a hot topic of research in the field of electrochemical energy storage. Sodium tetrathioantimonate Na<sub>3</sub>SbS<sub>4</sub>, a promising sodium ion-conductor solid electrolyte, can be synthesized via solution chemistry; a suitable, less energy-consuming and efficient method for mass production compared to dry processes (solid-solid reactions, mechanochemistry). The current work proposes to replace anhydrous sodium sulfide (Na<sub>2</sub>S, Na-precursor) with sodium hydrosulfide (NaSH.xH<sub>2</sub>O), a cheaper product that considerably reduces the cost of material production, a limiting factor from an up-scaling.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"427 ","pages":"Article 116892"},"PeriodicalIF":3.0,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144098907","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Peng Xu, Haiwei Wu, Haiwen Li, Hanbin Liu, Zhijian Li
{"title":"Synergistic effect of ball milling time and Mn-Fe ratio on the electrochemical performance of paper-based LiMn1-XFeXPO4/C cathodes for Lithium-ion batteries","authors":"Peng Xu, Haiwei Wu, Haiwen Li, Hanbin Liu, Zhijian Li","doi":"10.1016/j.ssi.2025.116898","DOIUrl":"10.1016/j.ssi.2025.116898","url":null,"abstract":"<div><div>In recent years, with the continuous development of high-voltage cathode materials for lithium-ion (Li<sup>+</sup>) batteries, the LiMn<sub>1-X</sub>Fe<sub>X</sub>PO<sub>4</sub> solid solution obtained by using Mn element to replace part of Fe on the basis of LiFePO<sub>4</sub> (LFP) has received extensive attention. It shows significantly improved voltage and capacity than LFP, which is currently regarded as a leading update for the traditional LFP cathode. At present, preparation of high-performance LiMn<sub>1-X</sub>Fe<sub>X</sub>PO<sub>4</sub> using common high-temperature solid-state method is still challenging and the basic intricate coupling of the Mn-Fe ratio and ball milling time parameters on its electrochemical performance is still need to be fully studied due to the parametric complexity. Herein, the carbon wrapped LiMn<sub>1-X</sub>Fe<sub>X</sub>PO<sub>4</sub>/C material was prepared by high-temperature solid-phase method, and paper-based LiMn<sub>1-X</sub>Fe<sub>X</sub>PO<sub>4</sub>/C electrodes were also fabricated to fully study the synergistic effects of ball milling times (0.5 h, 1 h, 2 h) and Mn-Fe ratios (5:5, 6:4, 7:3, 8:2) on their electrochemical performance. It was found that there happened to be optimized ball milling time for each Mn-Fe ratio based LiMn<sub>1-X</sub>Fe<sub>X</sub>PO<sub>4</sub>/C materials. The higher Mn-Fe ratio, the longer ball milling time that is needed to achieve high electrochemical performance of paper-based LiMn<sub>1-X</sub>Fe<sub>X</sub>PO<sub>4</sub>/C cathodes. Through detailed analysis of cyclic voltammetry (CV) curves, cycling and rate performance, it was found that LiMn<sub>1-X</sub>Fe<sub>X</sub>PO<sub>4</sub>/C cathode prepared by ball milling for 1 h and Mn-Fe ratio of 7:3 has the best optimized voltage, cycling and rate performance.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"427 ","pages":"Article 116898"},"PeriodicalIF":3.0,"publicationDate":"2025-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144072109","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xin Qiao , Yahao Mu , Jian Peng , Bo Pei , Shuo Wang
{"title":"Effects of depth of discharge on the electrochemical performance of LiFePO4-graphite pouch cells","authors":"Xin Qiao , Yahao Mu , Jian Peng , Bo Pei , Shuo Wang","doi":"10.1016/j.ssi.2025.116900","DOIUrl":"10.1016/j.ssi.2025.116900","url":null,"abstract":"<div><div>Lithium iron phosphate-graphite (LFP-C) batteries are widely used in energy storage and electric vehicles due to their high safety and good cycling stability. However, there is still a lack of in-depth research to investigate the impact of depth of discharge (DOD) on LFP-C pouch cells. In this work, we systematically investigate the influence of DOD (2.5 V and 1.5 V) on the cycling performance of LFP-C pouch cells, and the evolution of the cathode–electrolyte interphase (CEI) and solid electrolyte interphase (SEI) layers. In comparison to a DOD of 2.5 V, the cell with a DOD of 1.5 V exhibits a rapid capacity degradation after 50 cycles. Combined with comprehensive characterizations, the mechanism of battery decay has been revealed. A deeper discharge to 1.5 V results in an increase in the disorder of graphite. Additionally, the organic components in the SEI layer decreases, while the Li<sub>2</sub>CO<sub>3</sub>, LiF, and Li<sub>3</sub>PO<sub>4</sub> inorganic products enrich due to the continued decomposition of electrolyte. Meanwhile, the pouch cells generate a considerable quantity of H<sub>2</sub> and minor CH<sub>4</sub> gases. This study will pave the way to understand the effects of overdischarge on the electrochemical performance of commercial pouch cells and the evolution mechanism of CEI/SEI layers.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"427 ","pages":"Article 116900"},"PeriodicalIF":3.0,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144072108","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Mechanical-electrochemical coupling patterns in all-solid-state lithium batteries employing sulfide- and halide-based solid electrolytes","authors":"Jing Zhu , Hailong Yu , Liubin Ben , Junfeng Hao , Qiangfu Sun , Xinxin Zhang , Ronghan Qiao , Guanjun Cen , Xiayin Yao , Heng Zhang , Xuejie Huang","doi":"10.1016/j.ssi.2025.116887","DOIUrl":"10.1016/j.ssi.2025.116887","url":null,"abstract":"<div><div>The mechanical properties of inorganic solid electrolytes are strongly coupled with their electrochemical performance in all-solid-state lithium batteries (ASSLBs). Herein, we report distinct mechanical-electrochemical coupling patterns between sulfide- and halide-based solid electrolytes through dynamic pressure modulation. We designed a multi-channel pressure-electrochemistry coupling platform (pressure range: 0–380 MPa, resolution: ± 0.01 MPa) to elucidate how pressure conditions govern interfacial contact stability and cycling performance. For sulfide-based systems (e.g., Li<sub>6</sub>PS<sub>5</sub>Cl, LPSC), a dynamic pressure controlling protocol allows the regulation of electrolyte creep behavior, enabling sustained interfacial contact for electrochemical reactions. This approach achieves an specific capacity of 227.3 mAh g<sup>−1</sup> and capacity retention of 89.1 % after 300 cycles for a typical Li-In||LiNi<sub>0.93</sub>Co<sub>0.02</sub>Mn<sub>0.05</sub>O<sub>2</sub> cell. In contrast, halide-based systems employing Li<sub>3</sub>InCl<sub>6</sub> (LIC) require a constant and high external pressure to maintain electrochemical stability. Mechanistic studies attribute the enhanced performance of LPSC to its stress-adaptive creep behavior, which dynamically stabilizes interfaces during cycling. Conversely, the lower resilience and toughness of LIC necessitate sustained external pressure to preserve solid-solid contacts in both bulk electrolyte and composite cathodes. These findings establish tailored pressure management protocol for sulfide- and halide-based electrolytes, providing guidelines for further optimization of the electrochemical performance of ASSLBs via mechanical-electrochemical coupling strategies.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"427 ","pages":"Article 116887"},"PeriodicalIF":3.0,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143947686","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
C.J. Vijaykumar , Soumya S. Bulla , Chetan Chavan , Rajashekhar F. Bhajantri , K. Sakthipandi
{"title":"One-step fabrication of sodium-ion conducting cotton-based solid-state electrolyte for primary battery applications","authors":"C.J. Vijaykumar , Soumya S. Bulla , Chetan Chavan , Rajashekhar F. Bhajantri , K. Sakthipandi","doi":"10.1016/j.ssi.2025.116897","DOIUrl":"10.1016/j.ssi.2025.116897","url":null,"abstract":"<div><div>Lithium-ion batteries and liquid electrolyte-based energy storage systems face intrinsic limitations that necessitate alternative solutions. Sodium-ion batteries with solid-state electrolytes, particularly biopolymer electrolytes, have emerged as promising candidates for sustainable battery technologies. This study developed a biopolymer electrolyte using cotton cellulose and explored its structural, dielectric, and transport properties upon doping with sodium nitrate (<span><math><mi>NaN</mi><msub><mi>O</mi><mn>3</mn></msub></math></span>) salt and bismuth oxide (<span><math><mi>B</mi><msub><mi>i</mi><mn>2</mn></msub><msub><mi>O</mi><mn>3</mn></msub></math></span>) nanoparticles (NPs). Three samples, pristine cotton (PC), <span><math><mi>NaN</mi><msub><mi>O</mi><mn>3</mn></msub></math></span>-doped cotton (PCS), and <span><math><mi>NaN</mi><msub><mi>O</mi><mn>3</mn></msub></math></span> with <span><math><mi>B</mi><msub><mi>i</mi><mn>2</mn></msub><msub><mi>O</mi><mn>3</mn></msub></math></span> NPs-doped cotton (PCSN) were prepared using a polymer adsorption palletization technique. XRD, FTIR, and SEM with EDX confirmed successful doping, revealing changes in crystallinity, chemical interactions, and microstructural modifications respectively. The impedance spectroscopy and dielectric studies showed insulating behaviour for pristine cotton, while <span><math><mi>NaN</mi><msub><mi>O</mi><mn>3</mn></msub></math></span>-doped cotton and <span><math><mi>NaN</mi><msub><mi>O</mi><mn>3</mn></msub></math></span> with <span><math><mi>B</mi><msub><mi>i</mi><mn>2</mn></msub><msub><mi>O</mi><mn>3</mn></msub></math></span> NPs-doped cotton exhibited ionic conductivities of <span><math><mn>1.71</mn><mo>×</mo><msup><mn>10</mn><mrow><mo>−</mo><mn>4</mn></mrow></msup><mspace></mspace><mi>S</mi><msup><mi>cm</mi><mrow><mo>−</mo><mn>1</mn></mrow></msup></math></span> and <span><math><mn>3</mn><mo>.</mo><mn>81</mn><mo>×</mo><msup><mn>10</mn><mrow><mo>−</mo><mn>5</mn></mrow></msup><mspace></mspace><mi>S</mi><msup><mi>cm</mi><mrow><mo>−</mo><mn>1</mn></mrow></msup></math></span> respectively. PCS-based cells demonstrated superior performance with open circuit voltage of <span><math><mn>2.2</mn><mspace></mspace><mi>V</mi></math></span>, current density of <span><math><mn>3.55</mn><mspace></mspace><mi>μA</mi><msup><mi>cm</mi><mrow><mo>−</mo><mn>2</mn></mrow></msup></math></span>, power density of <span><math><mn>0.29</mn><mspace></mspace><mi>W</mi><msup><mi>Kg</mi><mrow><mo>−</mo><mn>1</mn></mrow></msup></math></span>, energy density of <span><math><mn>7.09</mn><mspace></mspace><mi>Wh</mi><msup><mi>Kg</mi><mrow><mo>−</mo><mn>1</mn></mrow></msup></math></span>, and discharge capacity of <span><math><mn>2.32</mn><mspace></mspace><mi>μA</mi><msup><mi>h</mi><mrow><mo>−</mo><mn>1</mn></mrow></msup></math></span>.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"427 ","pages":"Article 116897"},"PeriodicalIF":3.0,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143943247","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Eco-selective purification to high-capacity LiFePO4: Transforming natural Iron sources via alkali-mediated green synthesis","authors":"Zhihong Yang, Yongjia Li, Yingjuan Li, Zhenhua Zhang, Xingzhi Zhang","doi":"10.1016/j.ssi.2025.116894","DOIUrl":"10.1016/j.ssi.2025.116894","url":null,"abstract":"<div><div>Lithium iron phosphate (LiFePO<sub>4</sub>), renowned for its thermal stability and structural safety, faces cost limitations in conventional synthesis routes. This study presents a transformative approach utilizing natural hematite concentrate through an integrated impurity engineering and structural activation strategy. Thermodynamic analysis guided a two-stage alkaline sintering process that selectively removes detrimental impurities via NaOH-mediated conversion to water-soluble Na<sub>2</sub>O·Al<sub>2</sub>O<sub>3</sub>/Na<sub>2</sub>O·SiO<sub>2</sub> complexes, while preserving beneficial Mg dopants for enhanced ionic conductivity. Subsequent rapid quenching induces metastable Fe<sub>2</sub>O<sub>3</sub> amorphization (68.79 wt% Fe purity) with fractured nanorod morphologies. The optimized LiFePO<sub>4</sub> cathode exhibits exceptional electrochemical performance, delivering 155.7 mAh g<sup>−1</sup> at 0.1C with minimal polarization, and maintains 110.7 mAh g<sup>−1</sup> at ultrahigh 15C rates. Long-term cycling reveals 89.9 % capacity retention after 1000 cycles at 1.0C. reducing charge transfer resistance by 59 % versus conventional synthesis. This synergistic impurity removal-amorphization mechanism enables the preparation of LiFePO<sub>4</sub> from low-grade ores, opening up a scalable route for the production of cost-competitive LiFePO<sub>4</sub> anodes and concurrently realizing the value-added utilization of natural mineral resources. This method combines materials engineering with sustainable battery production, greatly reducing the cost of precursors compared to traditional iron sources.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"426 ","pages":"Article 116894"},"PeriodicalIF":3.0,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143934720","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Na Li, Xinze Li, Ling Li, Yanwei Li, Jiefeng Hai, Bin Huang
{"title":"Nano Co3O4 coating endows LiNi0.9Co0.05Mn0.05O2 with high cycling performance and suppressed air sensitivity","authors":"Na Li, Xinze Li, Ling Li, Yanwei Li, Jiefeng Hai, Bin Huang","doi":"10.1016/j.ssi.2025.116893","DOIUrl":"10.1016/j.ssi.2025.116893","url":null,"abstract":"<div><div>In this study, ultra-high nickel LiNi<sub>0.9</sub>Co<sub>0.05</sub>Mn<sub>0.05</sub>O<sub>2</sub> is coated by Co<sub>3</sub>O<sub>4</sub> nanoparticles through a facile solid-state process. A systematic investigation is conducted to evaluate the impacts of the Co<sub>3</sub>O<sub>4</sub> coating on the crystal structure, microstructure, cycling performance, electrochemical reaction kinetics, and electrochemical diffusion kinetics of the material. X-ray diffraction and scanning electron microscopy analyses reveal that the Co<sub>3</sub>O<sub>4</sub> coating has no obvious effect on the crystal and microstructural properties of LiNi<sub>0.9</sub>Co<sub>0.05</sub>Mn<sub>0.05</sub>O<sub>2</sub>. Under both room temperature (25 °C) and high temperature (55 °C) conditions, the Co<sub>3</sub>O<sub>4</sub>-coated LiNi<sub>0.9</sub>Co<sub>0.05</sub>Mn<sub>0.05</sub>O<sub>2</sub> exhibits superior cycling performance compared to the pure LiNi<sub>0.9</sub>Co<sub>0.05</sub>Mn<sub>0.05</sub>O<sub>2</sub>. Additionally, the Co<sub>3</sub>O<sub>4</sub> coating accelerates the electrochemical reaction kinetics. This research provides insights into the preparation of ultra-high Ni layered cathode materials with high-performance.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"427 ","pages":"Article 116893"},"PeriodicalIF":3.0,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143937913","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}