ACS Applied Energy Materials最新文献

{"title":"Oxypnictide Anti-perovskite (Ca4Pn2–xNx)O and (Ca4–xMgx)Pn2O (Pn = P, As; 0.125 ≤ x ≤ 0.25) Materials as Promising Candidates for Solar Fuel Generation: Rational Insights from DFT","authors":"Ahmed N. Halool,&nbsp;Saeed A. Aissan,&nbsp;Abdesslem Jedidi,&nbsp;Bassim Arkook,&nbsp;A. M. Abdel-Daiem,&nbsp;Luigi Cavallo,&nbsp;Moussab Harb","doi":"10.1021/acsaem.6c01190","DOIUrl":"https://doi.org/10.1021/acsaem.6c01190","url":null,"abstract":"<p>We present the oxypnictide anti-perovskites A₄Pn₂O (A = Ca, Sr; Pn = P, As) as a class of visible-light-responsive photocatalytic materials. Substitutional doping is further explored through anionic N^3–@Pn^3– and cationic Mg²⁺@Ca²⁺ sites, yielding (Ca₄Pn_{2–<em>x</em>}N_<em>x</em>)O and (Ca_{4–<em>x</em>}Mg_<em>x</em>)Pn₂O (with <em>x</em> = 0.125, 0.25, and 0.50). All systems are examined using first-principles calculations based on DFT and DFPT. The GGA-PBE functional demonstrates reliable reproduction of the experimental structural parameters for the pristine materials. In addition, the optoelectronic and water redox properties are accurately calculated using the screened Coulomb hybrid HSE06 functional. These materials exhibit direct band gaps within the optimal solar range (2.00–2.40 eV), strong optical absorption coefficients (&gt;10⁵ cm^–1), high dielectric constants (26–85), weak exciton binding energies (&lt;25 meV), and small electron and hole effective masses (&lt; 0.50 m₀) along the [100/010] and [001] directions. This leads to good exciton dissociation ability, good charge-carrier transport with efficient charge separation, and small recombination rate in the bulk. However, their VBM energy position is not appropriate enough for OER, and therefore, the substitutional doping strategy was adopted to overcome this limitation. Among all investigated doped materials, (Ca₄Pn_{2–<em>x</em>}N_<em>x</em>)O and (Ca_{4–<em>x</em>}Mg_<em>x</em>)Pn₂O (for <em>x</em> = 0.25) achieve good thermodynamic stability and reveal the most suitable CBM and VBM energy positions for both H⁺ reduction and water oxidation while maintaining the excellent optoelectronic properties as in the pristine materials. This offers an opportunity for these promising candidates to be experimentally synthesized and tested for efficient solar-driven H₂ production and/or CO₂ reduction.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 17","pages":"11241–11258"},"PeriodicalIF":5.5,"publicationDate":"2026-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148950620","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Investigation on the Electronic, Optical, Mechanical, and Photovoltaic Properties of CuZn2InS4 Quaternary Chalcogenide","authors":"Namrata A. Tukadiya,&nbsp;Prafulla K. Jha","doi":"10.1021/acsaem.6c01592","DOIUrl":"https://doi.org/10.1021/acsaem.6c01592","url":null,"abstract":"<p>There is increasing interest in multifunctional materials for energy conversion devices worldwide. Chalcogenides remain at the center of attraction due to their significant applications in optoelectronics and photovoltaics. In this study, density functional theory is employed to investigate the structural, optical, electronic, mechanical, and photovoltaic properties of CuZn₂InS₄. Optimization of the structure shows that CuZn₂InS₄ crystallizes in t<em>etragonal</em> symmetry, and the calculated elastic constants meet the Born stability criterion. The HSE06-level electronic band structure reveals its semiconducting behavior with a direct band gap value of 1.94 eV. The material exhibits strong absorption in the visible and UV ranges, a high refractive index, and a dielectric response indicating its potential as a promising absorber-layer candidate. The elastic properties indicate that CuZn₂InS₄ is mechanically stable. The absence of imaginary phonon modes in the entire Brillouin zone (BZ) confirms its dynamical stability. The studied solar cell configuration suggests a power conversion efficiency of 18.72% with the device configuration Al/FTO/CdS/CuZn₂InS₄/Cu₂O/Ni under the considered simulation conditions. This study indicates that CuZn₂InS₄ is a promising material for further optoelectronic and absorber-layer investigations.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 17","pages":"11454–11465"},"PeriodicalIF":5.5,"publicationDate":"2026-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148950869","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Decoupling Electrothermal Transport in the YbAl3 Kondo Lattice via Itinerant-Electron Magnetic Fluctuations","authors":"Zheng Wang,&nbsp;Danqi He,&nbsp;Tiantian Chen,&nbsp;Mingxu Wei,&nbsp;Zhong Li,&nbsp;Ping Wei,&nbsp;Wanting Zhu,&nbsp;Xiaolei Nie,&nbsp;Jian Yu,&nbsp;Wenyu Zhao,&nbsp;Qingjie Zhang","doi":"10.1021/acsaem.6c01819","DOIUrl":"https://doi.org/10.1021/acsaem.6c01819","url":null,"abstract":"<p>The thermoelectric optimization of metallic heavy-fermion systems, such as the YbAl₃ Kondo lattice, is fundamentally constrained by an excessively high electronic thermal conductivity (κ_E) that stems from an inherently high carrier concentration. Herein, we propose an approach to decouple electrothermal transport in YbAl₃ by incorporating the soft magnetic alloy LaFe_10.4Co_0.8Si_1.8 (LFS) as a functional second phase. Our results demonstrate that itinerant-electron magnetic fluctuations arising from the LFS phase near its Curie temperature (<em>T</em>_C ≈ 292.5 K) act as a dynamic regulator of the Kondo environment. The incorporation of LFS elevates the Kondo temperature and enhances the Kondo interaction while simultaneously reducing the carrier concentration, resulting in a suppression of electrical conductivity. Crucially, this regulation results in a significant reduction in total thermal conductivity (κ), where the decline in κ_E accounts for 61% of the κ reduction, highlighting the dominance of electronic transport management in metallic TE systems. Simultaneously, magnetoresistance modeling confirms that strong spin–phonon coupling further curtails the phonon mean free path and reduces the lattice thermal conductivity by 34.9% at 300 K. Consequently, a peak <em>zT</em> of 0.38 is achieved at 300 K for the 0.3 wt % LFS composite, representing a 26.7% improvement over pristine YbAl₃. This work provides profound insights into leveraging itinerant-electron magnetic degrees of freedom to transcend the metallic transport bottleneck in advanced heavy-fermion thermoelectric materials.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 17","pages":"11696–11705"},"PeriodicalIF":5.5,"publicationDate":"2026-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148950890","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A Descriptor and Tool for Guiding Composition Design toward Developing Single- or Mixed/Hybrid-Phase “Layered” Transition Metal Oxide Cathode Materials for Na-Ion Batteries","authors":"Brijesh Yadav,&nbsp;Velaga Srihari,&nbsp;Himanshu K. Poswal,&nbsp;Ali Zavabeti,&nbsp;Parama Chakraborty Banerjee,&nbsp;Mainak Majumder,&nbsp;Amartya Mukhopadhyay","doi":"10.1021/acsaem.6c01167","DOIUrl":"https://doi.org/10.1021/acsaem.6c01167","url":null,"abstract":"<p>The structure type and phase assemblage of “layered” Na-transition metal (T_M) oxides dictate their performance as cathode materials, resulting in an impetus toward developing biphasic or hybrid Na-T_M-oxides. However, a fundamental understanding as to what drives the formation of such biphasic structures, instead of a single phase, remains unestablished. This also means that a coherent strategy to rationally design hybrid Na-T_M-oxides and tune the relative contents of the constituent phases is missing. Against this backdrop, we report a simple strategy and an associated descriptor, that is based on the overall covalency of cation−oxygen bonds in the T_MO₂-“slab”, <em>viz.</em>, the average charge-to-radius ratio of the cation combination in the T_M-layer. Tuning the above parameter gives access to compositions leading to either phase-pure or biphase/hybrid O3/P2-type structures with varied relative contents of the constituent phases (at least in qualitative terms) for a fixed Na-content. The usage of this simple descriptor and the associated phase map has been successfully demonstrated here by developing a series of phase-pure and hybrid P2/O3-structured Na-T_M-oxides based on two Na-contents using the same synthesis protocol. This confirms the suitability of this rational design strategy across various compositions, which can be adapted for widespread development of biphasic/hybrid “layered” T_M-oxides for usage as cathode materials for Na-ion batteries and beyond.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 17","pages":"11229–11240"},"PeriodicalIF":5.5,"publicationDate":"2026-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148950912","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Safer Sodium Storage through Carbon Coatings on Aluminum Current Collectors for Anode-less Metal Batteries","authors":"David Patrun,&nbsp;Ziyaad Aytuna,&nbsp;Si Zhao,&nbsp;Junjie Liu,&nbsp;Yasuyuki Kondo,&nbsp;Katsumasa Torii,&nbsp;Yu Katayama,&nbsp;Thomas Fischer,&nbsp;Tohru Sekino,&nbsp;Zhensheng Hong,&nbsp;Yuki Yamada,&nbsp;Sanjay Mathur","doi":"10.1021/acsaem.6c01559","DOIUrl":"https://doi.org/10.1021/acsaem.6c01559","url":null,"abstract":"<p>Dendrite growth and formation of an unstable solid electrolyte interphase (SEI) remain major obstacles for anode-less sodium metal batteries (SMBs). Surface modification of current collectors (CCs) is a key strategy for suppressing dendrite formation and stabilizing the SEI, leading to safer and longer-lasting SMBs. Herein, we developed a carbon-coated aluminum foil, enabling &gt;99.9% retention in coulombic efficiency and 600 plating/stripping cycles at 2 mA cm^–2. Additionally, high reversibility was demonstrated in cycling performance, even after cycling at higher current densities of up to 6 mA cm^–2. A careful optimization of the coating thickness was conducted to minimize electrode volume and weight, yielding a thin (∼700 nm) and ultralight (&lt;0.05 mg/cm²) carbon modification on Al current collectors in an anode-less configuration, while maintaining enhanced performance. The sodiophilic nature of the porous, carbon overlayer deposited by plasma-enhanced chemical vapor deposition suppresses the formation of dead sodium and stabilizes the SEI, as proven by correlative analyses using SEM, EIS, EDS, and XPS. C@Al||NVP full-cells delivered 87.8 mAh g^–1 after 45 cycles at 1C and rate stability with an average capacity of 67.8 mAh g^–1 at 5C. Our carbon-coated aluminum foil offers a cost-effective and abundant CC for SMBs, which suppresses the formation of sodium dendrites to enhance battery lifetime.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 17","pages":"11416–11428"},"PeriodicalIF":5.5,"publicationDate":"2026-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148950935","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"High-Temperature Synthesis of PtCo Nanoparticles Supported on a Nitrogen-Doped Carbon Carrier as a Catalyst for the Oxygen Reduction Reaction","authors":"Alina Nevelskaya,&nbsp;Anna Gavrilova,&nbsp;Yulia Bayan,&nbsp;Nikolay Lyanguzov,&nbsp;Egor Beskopylny,&nbsp;Ilya Pankov,&nbsp;Andrey Kokhanov,&nbsp;Anna Kremneva,&nbsp;Sergey Belenov","doi":"10.1021/acsaem.6c01627","DOIUrl":"https://doi.org/10.1021/acsaem.6c01627","url":null,"abstract":"<p>This work presents a promising method for synthesizing high-performance PtCo/C–N catalysts based on Pt/C material on an N-doped carbon carrier. The effect of treatment temperature of Pt/C–N materials with deposited cobalt precursors on the structure and catalytic activity of PtCo/C–N catalysts has been studied. It was found that an increase in the treatment temperature from 600 to 800 °C leads to a slight growth in nanoparticle size from 2.2 to 2.6 nm (according to XRD) and a decrease in the electrochemical surface area from 90 to 69 m²/g(Pt). After high-temperature synthesis, the activity of the resulting bimetallic PtCo/C–N catalysts is 3–4 times higher than that of the initial Pt/C–N material or the commercial Pt/C benchmark in the potential range of 0.95–0.87 V. The PtCo/C–N material after treatment at 600 °C demonstrated the highest oxygen reduction reaction activity after accelerated stress testing. The obtained PtCo/C–N catalysts are promising materials for the further optimization of the membrane electrode assembly (MEA) catalyst layer and for investigating their long-term stability in MEAs to assess their potential for use in commercial proton-exchange membrane fuel cells (PEMFCs).</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 17","pages":"11498–11507"},"PeriodicalIF":5.5,"publicationDate":"2026-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148950732","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Enhanced Mass Activity for CO2 Electroreduction to CO via Confined Ultrasmall Au Nanoparticles","authors":"Pengxuan Wu,&nbsp;Yusong Ding,&nbsp;Bingshuang Li,&nbsp;Yunxia He,&nbsp;Qian Liu,&nbsp;Xiaoxi Huang","doi":"10.1021/acsaem.6c01972","DOIUrl":"https://doi.org/10.1021/acsaem.6c01972","url":null,"abstract":"<p>This study reports a mesoporous carbon confinement strategy for enhancing the mass activity and structural durability of Au-based catalysts toward electrochemical CO₂ reduction reaction (CO₂RR) to CO. Glutathione-protected Au clusters were introduced into polyaniline-derived mesoporous carbon (PDMC), followed by thermal ligand removal, producing ultrasmall Au nanoparticles uniformly embedded within a conductive N-doped carbon framework. The mesoporous carbon matrix effectively restricts Au growth and suppresses nanoparticle aggregation, thereby preserving abundant low-coordinated Au surface sites while maintaining accessible channels for charge and mass transport. The optimized Au@PDMC-30 catalyst delivers a CO Faradaic efficiency of 90.0 ± 1.3% at –0.9 V vs reversible hydrogen electrode in an H-type cell and maintains stable CO production for over 24 h without obvious Au aggregation. More importantly, under flow-cell conditions, Au@PDMC-30 achieves a high CO mass activity of 1192.4 mA mg^–1, approximately twice that of commercial Au/C, demonstrating greatly improved precious-metal utilization. In situ Fourier transform infrared spectroscopy and density functional theory calculations reveal that the confined low-coordinated Au sites possess an optimized electronic structure that facilitates *COOH formation, thereby accelerating the CO₂ to CO pathway. This work highlights confinement engineering of ultrasmall noble-metal nanoparticles as an effective route to improve catalytic selectivity, durability, and mass-normalized activity for CO₂RR.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 17","pages":"11887–11895"},"PeriodicalIF":5.5,"publicationDate":"2026-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148950763","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"High Mass Activity of Co-Sputtered Ir−Ru Thin Films on TiC for Acidic Oxygen Evolution Reaction","authors":"Young-Woo Kim,&nbsp;Hoyeon Shin,&nbsp;Kyu-Su Kim,&nbsp;Sang-Mun Jung,&nbsp;Yong-Tae Kim","doi":"10.1021/acsaem.6c01690","DOIUrl":"https://doi.org/10.1021/acsaem.6c01690","url":null,"abstract":"<p>Reducing the precious metal loading while maintaining high activity remains a main challenge for acidic oxygen evolution reaction (OER) anodes in proton exchange membrane water electrolysis. Herein, we report ultralow-loading, uniformly dispersed Ir−Ru thin-film electrodes fabricated via precursor-free physical vapor deposition (PVD) on conductive TiC substrates. By employing RF magnetron cosputtering, we prepared ultrathin (∼3 nm) composition-controlled Ir−Ru films with a total platinum group metal (PGM) loading of ∼4 μg cm⁻², achieving uniform dispersion that overcomes the limitations of conventional solution-based methods. In addition, the TiC substrate improved the activity−stability factor of the Ir−Ru films, possibly by mitigating excessive surface oxidation and lattice-oxygen-associated degradation. As a result, the cosputtered Ir₆₉Ru₃₁ thin-film electrode delivers extraordinary mass activities of 3.11 and 23.5 A mg_PGM⁻¹ at 1.53 and 1.70 V vs RHE, respectively, exceeding conventional Ir-based benchmarks by over two orders of magnitude. These results demonstrate that PVD-derived thin films can serve as a scalable platform for improving precious-metal utilization in acidic OER.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 17","pages":"11589–11599"},"PeriodicalIF":5.5,"publicationDate":"2026-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148950781","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"TTE-Mediated Anode/Electrolyte Interface Modification of SN-Plasticized PEO/PVDF-HFP Solid Polymer Electrolyte for Room-Temperature Applications","authors":"Kun-Rong Lu,&nbsp;Dong-Yang Li,&nbsp;Hong-Yu Wang,&nbsp;Yue-Xi Han,&nbsp;Fa-Nian Shi,&nbsp;Peng-Fei Wang,&nbsp;Yu-Hang Zhang","doi":"10.1021/acsaem.6c01301","DOIUrl":"https://doi.org/10.1021/acsaem.6c01301","url":null,"abstract":"<p>Polyethylene oxide (PEO)-based polymer electrolytes hold promise for application in solid-state lithium metal batteries. However, the high crystallinity of PEO poses a significant challenge to ion transport, particularly limiting its room-temperature performance. Poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP), a semi-crystalline polymer with rigid fluorocarbon chains, can provide robust mechanical support to the electrolyte system. Herein, a quasi-solid electrolyte (QSE) was fabricated by using PEO and PVDF-HFP, in which succinonitrile (SN) was introduced as a plasticizer to enhance the electrochemical properties at room temperature. Innovatively, 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE) was employed as a shield layer to prevent direct contact between the Li anode and the prepared SN-modified PEO/PVDF-HFP-QSE, thus forming a stable anode/electrolyte interface. The obtained TTE-P₈P₂S(12%)-QSE exhibits high room-temperature electrochemical properties, with an ionic conductivity of 4.02 × 10^–4 S cm^–1, a lithium-ion transport number of 0.47, and a wide electrochemical window of 5.4 V vs. Li⁺/Li. By interfacial modification, TTE-P₈P₂S(12%)-QSE can enable long-term cycling of LiCoO₂ cathodes and Li anodes, with an initial discharge capacity of 126.9 mAh g^–1, and achieve an average capacity of 142.8 mAh g^–1 within 100 cycles at room temperature. Characterizations reveal that the incorporation of TTE preserves the structural integrity of the lithium electrodes, promotes efficient utilization of active lithium ions, and tailors the composition and structure of the solid-electrolyte interphase (SEI) on the lithium metal anode, thereby substantially enhancing interfacial stability. This work provides a feasible strategy for building high-energy-density lithium metal batteries for room-temperature applications.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 17","pages":"11272–11284"},"PeriodicalIF":5.5,"publicationDate":"2026-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148950707","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Electrochemical and Spectroscopic Evaluation of Li7Si2S7I Solid Electrolyte in All-Solid-State Batteries","authors":"Andrés Acín-Lalanza,&nbsp;Johannes Hartel,&nbsp;Jingxuan Zhang,&nbsp;Marvin A. Kraft,&nbsp;Ruiyong Chen,&nbsp;Luke M. Daniels,&nbsp;Wolfgang G. Zeier,&nbsp;Laurence J. Hardwick,&nbsp;Matthew J. Rosseinsky","doi":"10.1021/acsaem.6c01833","DOIUrl":"https://doi.org/10.1021/acsaem.6c01833","url":null,"abstract":"<p>All-solid-state batteries require solid electrolytes with sufficient oxidative and reductive stability; however, the interfacial behavior of emerging silicon-based sulfide electrolytes remains poorly understood. In particular, the electrochemical stability of Li₇Si₂S₇I under practical cell operation and the separate effects of cathode and anode interfaces on performance degradation have not been clarified. Here, we systematically evaluate Li₇Si₂S₇I in LiNi_0.82Mn_0.07Co_0.11O₂ (NMC82) | solid electrolyte | Li-In all-solid-state cells using two- and three-electrode configurations combined with impedance analysis and ex situ Raman and X-ray photoelectron spectroscopy. Three-electrode measurements decouple the interfacial reactions and reveal concurrent interfacial decomposition at both the cathode and anode sides, with dominating effect from the cathode side. Symmetric cell tests using Li-In/Li₇Si₂S₇I composite electrodes confirm slight reductive instability against Li-In for Li₇Si₂S₇I as an anolyte. Spectroscopic analysis identifies polysulfides, oxidized iodide, and oxygenated SiO_<em>x</em> and SO_<em>x</em> species at the Li₇Si₂S₇I/NMC82 interface, as well as In₂S₃ formation at the Li₇Si₂S₇I/Li-In interface. Our findings provide mechanistic insight into the interfacial reactions of Si-based sulfide electrolytes and highlight the importance of electrode-decoupled diagnostics for evaluating the compatibility with electrode materials in all-solid-state batteries.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 17","pages":"11669–11680"},"PeriodicalIF":5.5,"publicationDate":"2026-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148950721","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}