ACS Applied Energy Materials最新文献

{"title":"Direct Catalytic Methanation of Biomass at Mild Conditions by a Sustainable Hydrochar-Supported Metal Catalyst","authors":"Chao Gai*,&nbsp;Yijing Tao and Nana Peng*,&nbsp;","doi":"10.1021/acsaem.4c0305510.1021/acsaem.4c03055","DOIUrl":"https://doi.org/10.1021/acsaem.4c03055https://doi.org/10.1021/acsaem.4c03055","url":null,"abstract":"<p >Direct conversion of waste biomass into methane via catalytic methanation at low and ambient temperatures is an attractive albeit elusive route in the quest for an effective, inexpensive, and sustainable catalyst. In this study, we tried to tackle this challenging task by designing a series of efficient yet cost-effective Ce-doped hydrochar-supported Ni catalysts. The optimized Ni_0.02/Ce_0.05-HC under optimal reaction conditions exhibited a markedly high activity at low temperature (350 °C) and atmospheric pressure for the direct methanation reaction, with 90.7% CH₄ selectivity, 33.5 MJ/Nm³ LHV_g, and 3629 mL/g CH₄ yield. On the basis of catalytic studies as well as structural characterizations, the active sites responsible for this exceptional activity can be associated with highly dispersed metallic Ni species maximized by the Ce dopant as well as favored electronic metal–support interactions. Moreover, the stable Ce-doped hydrochar framework and its covalently bridged oxygen-containing functional groups cooperatively contribute to the improved stability during the direct methanation process. These findings may provide a strong reference for developing more high-efficiency yet low-cost catalysts toward biomass methanation, thus leveraging the existing natural gas infrastructure to facilitate a seamless transition from fossil fuels to sustainable energy sources.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 5","pages":"2935–2946 2935–2946"},"PeriodicalIF":5.4,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576426","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":"NiFe on CeO₂, TiO₂, and ZrO₂ Supports as Efficient Oxygen Evolution Reaction Catalysts in Alkaline Media.","authors":"Neethu Kochukunnel Varghese, Elina Mkrtchian, Anshika Singh, Letizia Savio, Massimiliano Boccia, Vincenza Marzocchi, Antonio Comite","doi":"10.1021/acsaem.4c03268","DOIUrl":"10.1021/acsaem.4c03268","url":null,"abstract":"<p><p>The high cost and low energy efficiency of conventional water electrolysis methods continue to restrict the widespread adoption of green hydrogen. Anion exchange membrane (AEM) water electrolysis is a promising technology that can produce hydrogen using cost-effective transition-metal catalysts at high energy efficiency. Herein, we investigate the catalytic activity of nickel and iron nanoparticles dispersed on metal-oxide supports for the oxygen evolution reaction (OER), employing electrochemical testing with an anion exchange ionomer to evaluate their potential for application in AEM electrolyzers. We report the electrochemical performance of NiFe nanoparticles of varying Ni:Fe ratios on CeO₂ for OER reaction, assessing the overpotential, Tafel slope, and electrochemical stability of the catalysts. Our findings indicate that Ni₉₀Fe₁₀ has the highest catalytic activity as well as stability. To further understand the role of different supports, we assess the electrocatalytic performance of Ni₉₀Fe₁₀ nanoparticles on two more supports - TiO₂ and ZrO₂. While CeO₂ has the lowest overpotential, the other supports also show high activity and good performance at high current densities. TiO₂ exhibits superior stability and its overpotential after chronopotentiometry measurements approaches that of CeO₂ at high current densities. These results underscore the critical role of iron addition in enhancing nickel nanoparticles' catalytic activity and further emphasize the importance of metal oxide supports in improving catalyst stability and performance.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 5","pages":"3087-3095"},"PeriodicalIF":5.4,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11902787/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143622833","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A Boron-Based Anion-Receptor Additive for High-Loading Lithium–Sulfur Batteries under Lean Electrolyte Conditions","authors":"Veka Sri Ganesan,&nbsp;Sudhan Nagarajan and Leela Mohana Reddy Arava*,&nbsp;","doi":"10.1021/acsaem.4c0285610.1021/acsaem.4c02856","DOIUrl":"https://doi.org/10.1021/acsaem.4c02856https://doi.org/10.1021/acsaem.4c02856","url":null,"abstract":"<p >Although Li–S batteries offer significant promise as replacements for conventional lithium-ion batteries in terms of sustainability and performance, their practical implementation remains challenging. Designing cathodes with high sulfur loading (≥5 mg/cm²) under lean electrolyte conditions (E/S ≤ 5 μL/mg) presents specific obstacles, including sluggish reaction kinetics, poor sulfur utilization, and increased interfacial resistance, often driven by the saturation of lithium polysulfide species in the electrolyte. To overcome these issues, the development of solvents and additives that can enhance sulfur utilization/dissolution while mitigating the polysulfide shuttle effect has become crucial. To address this, we introduce a boron-based anion receptor, tris(trimethyl)silyl borate (TMSB), as an electrolyte additive for Li–S batteries to improve the dissolution of polysulfide species in the electrolyte. Due to its Lewis-acid ability, TMSB was found to dissolve more anionic polysulfide species (Lewis bases) in DOL/DME-based electrolytes. Surface analysis of cycled cathodes revealed that TMSB also aids in scavenging decomposition products at the cathode surface by coordinating with anions, including sulfates and thiosulfates. At high-loading (5 mg/cm²) and lean electrolyte (<i>E</i>/<i>S</i> = 8 μL/mg) conditions, results show that 5 wt % TMSB in the electrolyte reduced the overpotential by 850 mV. Further, the addition of TMSB also enabled stable cycling at a 0.2C rate for 100 cycles compared to the intermittent cycling in the blank electrolyte. Hence, this study shows that TMSB as an electrolyte additive helps in improving sulfur utilization and reducing interfacial resistance for high-loading lithium–sulfur batteries under lean electrolyte conditions.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 5","pages":"2810–2818 2810–2818"},"PeriodicalIF":5.4,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576415","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":"Single-Ion Conducting Polymer Electrolyte with Excellent Interfacial Stability toward the Lithium Metal","authors":"Houang Phong Khanh Ngo,&nbsp;Yunfan Shao,&nbsp;Tony Bertaux,&nbsp;Thi Khanh Ly Nguyen,&nbsp;Justine Solier,&nbsp;Emilie Planes,&nbsp;Patrick Judeinstein,&nbsp;Fannie Alloin,&nbsp;Jean-Yves Sanchez and Cristina Iojoiu*,&nbsp;","doi":"10.1021/acsaem.4c0285910.1021/acsaem.4c02859","DOIUrl":"https://doi.org/10.1021/acsaem.4c02859https://doi.org/10.1021/acsaem.4c02859","url":null,"abstract":"<p >To improve the safety and energy density of lithium metal batteries, polymer electrolytes address the challenge by replacing flammable liquid electrolytes. We herein design an amorphous solid-state single-ion conducting polymer electrolyte (SIPE) with a strict alternating sequence of perfluorosulfonate lithium salt and poly(ethylene glycol) (PEG) with a very homogeneous dispersion of lithium salt in the electrolyte. Amorphous SIPE tailored with a moderate cross-link degree and reinforced with nanocrystals cellulose (NCC) exhibits a high Li⁺ conductivity exceeding 10^–5 S cm^–1 at 60 °C with a lithium transference number close to unity and excellent stability with Li metal. Long-term lithium stripping and plating were achieved in symmetric Li|SIPE|Li cells for over 80 days without dendrite growth. The Li|SIPE|LiFePO₄ cells provide an excellent rate capability performance with a high specific capacity of 163 and 132 mA h g^–1 at C/20 and C, respectively. The long-term cycling tests exhibited good performance and an average Coulombic efficiency of 99.9% for over 160 cycles. These excellent results confirmed the potential of the rationally designed single-ion conducting polymers as a safe and efficient solid-state electrolyte for next-generation high-performance energy storage.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 5","pages":"2819–2827 2819–2827"},"PeriodicalIF":5.4,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576678","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":"Optimizing Piezoelectricity and Temperature Stability in Sodium Potassium Niobate Ceramics through Phase Regulation and Texturing","authors":"Yuzhi Zhai,&nbsp;Jie Wang,&nbsp;Juan Du*,&nbsp;Limei Zheng* and Shiyi Guo*,&nbsp;","doi":"10.1021/acsaem.5c0016310.1021/acsaem.5c00163","DOIUrl":"https://doi.org/10.1021/acsaem.5c00163https://doi.org/10.1021/acsaem.5c00163","url":null,"abstract":"<p >This study aims to optimize the electromechanical performance and temperature stability of lead-free potassium sodium niobate-based piezoelectric ceramics. (1–<i>x</i>)K_0.525Na_0.475Nb_0.96Sb_0.04O₃-<i>x</i>Bi_0.5Na_0.5Zr_0.5Hf_0.5O₃ ceramics are investigated by manipulating the phase structure and texturing. The addition of Bi_0.5Na_0.5Zr_0.5Hf_0.5O₃ effectively adjusts the phase structure of the ceramics. Notably, the textured <i>x</i> = 0.03 ceramics exhibit excellent overall properties: piezoelectric strain coefficient <i>d</i>₃₃ ∼ 590 pC/N, piezoelectric voltage coefficient <i>g</i>₃₃ ∼ 57.7 × 10^–3 Vm/N, and dielectric loss tan δ ∼ 0.043. The enhanced piezoelectric coefficient increases its potential for application in piezoelectric energy harvesting. Moreover, the <i>d</i>₃₃ of the textured <i>x</i> = 0.05 ceramics demonstrates good temperature stability, with a <i>d</i>₃₃ of 360 pC/N and fluctuating within 10% in the temperature range of 25 to 170 °C. The results indicate that combining texturing with phase structure modulation is a promising approach to enhancing the application potential of lead-free potassium sodium niobate-based piezoelectric ceramics.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 5","pages":"3209–3216 3209–3216"},"PeriodicalIF":5.4,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576674","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":"Mild-Annealed Molecular Layer Deposition (MLD) Tincone Thin Film as Photoelectrochemically Stable and Efficient Electron Transport Layer for Si Photocathodes","authors":"Hyuenwoo Yang,&nbsp;Christopher J. Oldham,&nbsp;Carrie L. Donley,&nbsp;Renato N. Sampaio,&nbsp;John C. Dickenson,&nbsp;Pierpaolo Vecchi,&nbsp;K. Arun Joshi Reddy,&nbsp;Paul A. Maggard,&nbsp;Gerald J. Meyer and Gregory N. Parsons*,&nbsp;","doi":"10.1021/acsaem.4c0299710.1021/acsaem.4c02997","DOIUrl":"https://doi.org/10.1021/acsaem.4c02997https://doi.org/10.1021/acsaem.4c02997","url":null,"abstract":"<p >Metalcone thin films, composed of inorganic–organic hybrids, are synthesized using molecular layer deposition (MLD) through reactions between organometallic precursors (e.g., Sn, Al, and Ti) and organic reactants (e.g., ethylene glycol and glycerol). Despite their unique properties, metalcones exhibit significant vulnerability to water due to their organic components, limiting their potential in electrochemical applications. This study focuses on enhancing the photoelectrochemical stability of tincone thin films in aqueous electrolyte while preserving their hybrid characteristics through mild annealing in air at 250 °C. As-deposited and vacuum-annealed tincone thin films exhibited significant degradation under these conditions, while high-temperature-annealed (500 °C) tincone thin films offered improved stability with a significant decline in charge transfer efficiency. In contrast, mild annealing in air maintained the C–O bond at half level and improved the stability and charge transport without compromising the unique characteristics of tincone. This was confirmed by ellipsometry, X-ray photoelectron spectroscopy (XPS), and Fourier transform infrared spectroscopy (FTIR). Mild-annealed tincone deposited on a lightly doped p-type silicon (p-Si) photocathode produced a 20-fold increase in CO volume compared to high-temperature annealed tincone in a CO₂-saturated potassium bicarbonate (KHCO₃) electrolyte with dispersed graphene oxide–cobalt phthalocyanine (GO-CoPc) under 1 sun illumination at 0.9 V vs reversible hydrogen electrode (RHE), while maintaining the faradaic efficiency for CO and H₂. These results suggest that mild-annealed tincone thin films hold significant potential as protective charge transport layers on silicon photocathodes for the aqueous CO₂ reduction reaction (CO₂RR).</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 5","pages":"2982–2992 2982–2992"},"PeriodicalIF":5.4,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576662","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":"Rapid Screening Strategy of 2D Materials for Li-Ion Battery (LIB) Electrode Based on Deep Neural Networks (DNN)","authors":"Zhi Yang,&nbsp;Jianping Sun*,&nbsp;Yu Yang,&nbsp;Yuxin Chai and Yuyang Liu,&nbsp;","doi":"10.1021/acsaem.4c0320910.1021/acsaem.4c03209","DOIUrl":"https://doi.org/10.1021/acsaem.4c03209https://doi.org/10.1021/acsaem.4c03209","url":null,"abstract":"<p >The development of electrode materials is crucial for achieving an optimal performance in secondary ion batteries. Previous research has accumulated a substantial amount of data on electrode materials, creating varied data sets that include information on ion species, voltage, and other relevant characteristics. In this study, we processed the latest data and employed a deep neural network (DNN) machine learning (ML) platform to construct a regression model. The model relies on easily accessible input information, such as the initial structure, and utilizes high-quality data to validate its reliability. The two-dimensional material data set containing only the material structure is taken as the target set to predict the average discharge voltage (<i>U</i>_av), according to which more than 2500 potential electrode materials are selected. From this pool, we rigorously selected a subset of anode materials for detailed density functional theory (DFT) calculations. These materials exhibit promising elemental compositions and have not been previously investigated as electrode materials. The results of DFT calculations confirmed the reliability of the ML model’s predictions, demonstrating that the combination of ML and DFT calculations can effectively screen data sets lacking expensive DFT-calculated data. This strategy can significantly reduce computational costs by predicting specific performance metrics and conducting preliminary screenings.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 5","pages":"3058–3065 3058–3065"},"PeriodicalIF":5.4,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576660","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":"Improving the Catalytic Performances of Cu–Co Bimetallic Nanoparticles through Carbon Coating","authors":"Ning Huang,&nbsp;He Yang,&nbsp;Guillaume Wang,&nbsp;Sophie Nowak,&nbsp;Philippe Decorse,&nbsp;Stéphanie Lau-Truong,&nbsp;Wenjie Shen,&nbsp;Lorette Sicard* and Jean-Yves Piquemal*,&nbsp;","doi":"10.1021/acsaem.5c0028610.1021/acsaem.5c00286","DOIUrl":"https://doi.org/10.1021/acsaem.5c00286https://doi.org/10.1021/acsaem.5c00286","url":null,"abstract":"<p >In this study, we describe an easy-to-implement procedure to encapsulate CuCo bimetallic nanoparticles within carbon shells of variable thicknesses in the range of ca. 1–5 nm. The resulting nanostructures were thoroughly characterized by X-ray diffraction (XRD), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), N₂ physisorption, bright-field transmission electron microscopy (BFTEM), high-resolution transmission electron microscopy (HRTEM), scanning transmission electron microscopy (STEM), and high-angle annular dark field-scanning transmission electron microscopy (HAADF-STEM). All results agreed to show that the particles are individually coated with a relatively regular shell of carbon and a well-crystallized alloyed metal core, while the isotropic morphology and the mean size of the particles were preserved after the carbon deposition process. The catalytic properties of the carbon-coated particles were first evaluated for the liquid-phase acceptorless dehydrogenation of alcohols, and the results were compared to those of the uncoated parent materials. The results show that the carbon protective layer is not detrimental to catalytic activity and allows obtaining excellent stability even after four consecutive tests (about 100 h reaction time) at 185 °C. The carbon-coated particles have further been implemented for the gas-phase hydrogenation reactions of acetone and CO₂, where they performed stably at elevated temperatures and exhibited pronounced selectivities toward the desired products.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 5","pages":"3229–3242 3229–3242"},"PeriodicalIF":5.4,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576575","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":"Plasticized Composite Electrolyte with Al2O3 Nanofiller-Reinforced PVDF-HFP for Solid-State Lithium–Metal Batteries","authors":"Viet Cuong Nguyen,&nbsp;Tapabrata Dam,&nbsp;Hyeon-Bin Na and Chan-Jin Park*,&nbsp;","doi":"10.1021/acsaem.4c0330110.1021/acsaem.4c03301","DOIUrl":"https://doi.org/10.1021/acsaem.4c03301https://doi.org/10.1021/acsaem.4c03301","url":null,"abstract":"<p >Solid-state lithium–metal batteries (LMB) are promising next-generation energy storage systems (NESS), offering improved safety and higher energy density over liquid electrolyte-based batteries. This study presents a composite electrolyte based on a poly(vinylidene fluoride-<i>co</i>-hexafluoropropylene) (PVDF-HFP), one-dimensional Al₂O₃ nanofillers and plastic crystal plasticizer succinonitrile. The Al₂O₃ nanofillers, synthesized via electrospinning, facilitate the formation of efficient ion migration pathways and significantly enhance lithium-ion conductivity. The addition of nanofillers enhances the electrolyte’s mechanical strength, battery’s safety, performance, and durability. The optimized electrolyte exhibits an impressive ionic conductivity of 6.46 × 10^–4 S cm^–1, a Li⁺ ion transference number of 0.69, and an electrochemical stability window extending to 4.9 V at 60 °C. It also shows excellent compatibility with lithium metal anodes, enabling stable cycling in lithium symmetric cells for over 800 h at 0.1 mA cm^–2. When paired with high-voltage NCM622, the cells deliver a high discharge capacity of 158.2 mAh g^–1 at 0.1 C and maintain a capacity retention of 75% over 100 cycles at 1 C and 60 °C. These results demonstrate the potential of PVDF-HFP based composite electrolyte to enhance solid-state LMB performance and safety, with improved ionic conductivity, mechanical strength, and cycling stability, making it a promising candidate for NESS.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 5","pages":"3120–3131 3120–3131"},"PeriodicalIF":5.4,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576576","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":"Improve the Lithophilicity of Garnet Solid Electrolyte by Ultrasonic Sprayed Al2O3 Layer","authors":"Yang Hu,&nbsp;Pingmei Li,&nbsp;Shiyu Yu,&nbsp;Shihao Fu,&nbsp;Yibo Liu,&nbsp;Yaqing Wei,&nbsp;De Li,&nbsp;Liang Yang,&nbsp;Daming Chen*,&nbsp;Ning Wang and Yong Chen,&nbsp;","doi":"10.1021/acsaem.4c0299410.1021/acsaem.4c02994","DOIUrl":"https://doi.org/10.1021/acsaem.4c02994https://doi.org/10.1021/acsaem.4c02994","url":null,"abstract":"<p >Garnet-type solid electrolyte Li_6.25Ga_0.25La₃Zr₂O₁₂(LGLZO) is considered as one of the most promising solid electrolytes because of its high ionic conductivity, broad electrochemical window, and excellent stability toward lithium. However, contaminants such as lithiophobic Li₂CO₃/LiOH have inevitably formed on the electrolyte surface, leading to an increasing interfacial impedance and lithium dendrite formation. Herein, Al₂O₃ was introduced via ultrasonic spraying on the surface of LGLZO, and in situ converted Li₂CO₃ into LiAlO₂, resulting in Al₂O₃/LiAlO₂ mixed conductive layer (MCL) during the annealing. Experiments and density functional theory (DFT) calculations showed that this MCL interface not only effectively improved the wettability but also suppressed the dendrite growth. The interfacial area-specific resistance (IASR) is decreased from 700 to 8 Ω cm², while the critical current density (CCD) is increased from 0.34 to 1.4 mA cm^–2. Simultaneously, the Li/MCL@LGLZO/Li cell exhibited a prolonged cycle life of 5500 h at a current density of 0.15 mA cm^–2. Especially in the high voltage range of 2.5–4.5 V, the Li/MCL@LGLZO/LFP full cell delivers excellent rate and prolonged cycle lifespan. These results mean that introducing MCL is a strategy for improving the lithiophobic of the garnet electrolyte.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 5","pages":"2928–2934 2928–2934"},"PeriodicalIF":5.4,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576501","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}