ACS Applied Energy Materials最新文献

{"title":"Origin of the Different Trends of Experimental Activity on Perovskite Catalysts between OER and ORR","authors":"Anran Hou,&nbsp; and ,&nbsp;Runhai Ouyang*,&nbsp;","doi":"10.1021/acsaem.4c0300310.1021/acsaem.4c03003","DOIUrl":"https://doi.org/10.1021/acsaem.4c03003https://doi.org/10.1021/acsaem.4c03003","url":null,"abstract":"<p >Understanding the difference between the activities of catalysts in OER and ORR is crucial for designing a bifunctional catalyst for rechargeable fuel cells and metal–air batteries, which so far remains elusive. In this work, a wide range of 3d transition metal-based perovskite oxide catalysts were considered to uncover the difference in the trends between OER and ORR. By performing systematic symbolic regression on experimental data, we confirmed the previous descriptor (<i>d_B</i>, <i>n_B</i>) for OER activity and identified a new descriptor (<i>−d_B</i>, <i>–</i>|<i>e</i>_g – 0.8|) for ORR activity, where <i>d_B, n_B</i>, and <i>e</i>_g are the number of d-electrons, oxidation state, and <i>e</i>_g orbital occupancy of the transition-metal cation, respectively. To understand the descriptors, first-principles calculations based on multiple reaction mechanisms were performed. Results show that the dependence of activity on the B-site metal species of the ABO₃ perovskites exhibits a volcano-shaped relation in both OER and ORR. We found that the experimental activity descriptors can be explained by the computed results from multiple mechanisms (4e^– transfer). The difference between the experimental OER and ORR activity descriptors originates from that the volcano top of the OER performance against the 3d transition metal is located near the end of this period and that of the ORR is in the middle. For ORR, further calculations show that the 2e^– pathway was only important on Ni and Cu oxides on which the binding of *OOH is weak. These descriptors and insights can be helpful in guiding the design of perovskite catalysts for OER and ORR.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3481–3490 3481–3490"},"PeriodicalIF":5.4,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675675","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":"Synergistic Enhancement of Vectorial Separation of Photogenerated Charge Carriers via Heterojunction and Quantum Confinement Effects","authors":"Yachong Wang,&nbsp;Chaoyue Zheng,&nbsp;Youlin Wu,&nbsp;Teng Li,&nbsp;Jiangli Wang,&nbsp;Jihuai Wu,&nbsp;Fuda Yu*,&nbsp;Canzhong Lu* and Yiming Xie*,&nbsp;","doi":"10.1021/acsaem.4c0333110.1021/acsaem.4c03331","DOIUrl":"https://doi.org/10.1021/acsaem.4c03331https://doi.org/10.1021/acsaem.4c03331","url":null,"abstract":"<p >Solar-driven water splitting for hydrogen production is a promising solution to the energy crisis. Reducing the recombination of photogenerated charge carriers is a key strategy for enhancing the hydrogen evolution performance. In this study, a type-II heterojunction catalyst, CdS/Co₃O₄, was successfully prepared using a self-assembly method. The tight coupling between CdS and Co₃O₄ facilitates efficient electron transfer. The heterojunction promotes the separation of photogenerated electrons, thereby reducing the charge carrier recombination. Additionally, the quantum confinement effect of Co₃O₄ shortens the electron migration distance. Under illumination with a 10 W white light source, the hydrogen evolution rate of CdS/Co₃O₄ reached 21.07 mmol g^–1 h^–1, approximately three times that of pure CdS. Electron paramagnetic resonance and density functional theory calculations were employed to elucidate the electron transfer mechanism during the photocatalytic process. This study provides a theoretical foundation for the design and mechanistic investigation of quantum-dot-based heterojunction photocatalysts.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3707–3714 3707–3714"},"PeriodicalIF":5.4,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675677","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":"Two-Dimensional Na-Ionic Conduction in Layered Cobaltate Na2Co2TeO6: A Combined Neutron Diffraction and Impedance Spectroscopy Study","authors":"Bikash Chandra Saha,&nbsp;Anup Kumar Bera* and Seikh Mohammad Yusuf*,&nbsp;","doi":"10.1021/acsaem.5c0001210.1021/acsaem.5c00012","DOIUrl":"https://doi.org/10.1021/acsaem.5c00012https://doi.org/10.1021/acsaem.5c00012","url":null,"abstract":"<p >We report the microscopic mechanism of Na-ionic conduction and the role of the underlying crystal structure in the ionic conduction in the two-dimensional (2D) layered battery material Na₂Co₂TeO₆ by combined neutron diffraction and impedance spectroscopy studies. Na₂Co₂TeO₆ consists of Na⁺-ion layers in the <i>ab</i> plane, which are well separated by intermediate magnetic (Co/Te)O₆ layers along the <i>c</i> axis. Within the layers, the Na⁺ ions, resided in trigonal prismatic NaO₆ coordination, and are distributed over three partially occupied crystallographic sites. Our temperature-dependent neutron diffraction study ensures that the crystal symmetry remains invariant over 300–723 K, with a nominal change (∼2%) in the unit cell volume. Further, the soft-bond valence sum (BVS) analyses of neutron diffraction patterns reveal 2D ionic conduction pathways within the Na layers. The impedance data have been analyzed to estimate the interlinked parameters, viz., dc ionic conductivity, ac ionic conductivity, and diffusivity, in addition to electrical modulus and dielectric constant, illustrating the microscopic mechanism of Na-ionic conduction. The conduction mechanism of Na⁺ ions involves a correlated barrier hopping (CBH) process. The conduction of the Na⁺ ions is found to be both thermally and frequency activated. A significant enhancement (∼10³ times) of the conductivity has been observed upon increasing the temperature from 343 to 473 K. Further, our study demonstrates that the Na-ionic conduction of Na₂Co₂TeO₆ is highly influenced by a disordered arrangement and partial occupation of Na ions within the 2D layers. The present comprehensive study, thus, provides an insight into the microscopic understanding of the ionic conduction properties and its intercorrelations with the crystal structure. The present work is significant for the progress of battery research, especially in the fabrication of highly efficient battery materials.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3779–3792 3779–3792"},"PeriodicalIF":5.4,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675755","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":"Surface Fluorination of PAN-Based Carbon Fibers Electrodes for High Energy Density Supercapacitor","authors":"Ui-Won Lee,&nbsp;Sang Goo Lee,&nbsp;Jisu Jang,&nbsp;Keun-Hwan Oh*,&nbsp;Younghyun Cho* and Hong Suk Kang*,&nbsp;","doi":"10.1021/acsaem.4c0321210.1021/acsaem.4c03212","DOIUrl":"https://doi.org/10.1021/acsaem.4c03212https://doi.org/10.1021/acsaem.4c03212","url":null,"abstract":"<p >This study aims to enhance the electrochemical performance of supercapacitors by maximizing the specific surface area and surface treatment of carbon-material electrodes through fluorination doping. Polyacrylonitrile (PAN)-based carbon fibers (PCFs) were produced via electrospinning and subsequently activated with potassium hydroxide (KOH) at 800 °C to obtain activated PAN-based carbon fibers (APCFs). Direct fluorination was then used to synthesize fluorinated PAN-based carbon fibers (FPCFs). The specific surface area of the electrode materials was maximized by adjusting the concentration of the electrospinning solution. The effect of fluorination on changes in surface elemental content was precisely managed to mitigate the decrease in porosity. The pore size distribution, vital for determining the specific capacitance of supercapacitors, was thoroughly assessed. After the activation and fluorination processes, the specific surface area of the FPCFs increased significantly to 1753.2 m² g^–1. This value is notably higher than that of commercial activated carbons, which typically range from 1200 to 1500 m² g^–1. The supercapacitor properties of the resulting materials were evaluated, revealing a specific capacitance of 176.2 F g^–1 for FPCF with an electrospun PAN concentration of 7 wt %.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3606–3615 3606–3615"},"PeriodicalIF":5.4,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675719","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":"Enhancement Effects on Visible-Light-Driven Water Oxidation by a Bifunctional Fe-Co-deposited SnOx Catalyst Layer Deposited on an N-Doped CuWO4 Photoanode","authors":"Tomohiro Katsuki,&nbsp;Junsuke Hatayama,&nbsp;Zaki N. Zahran,&nbsp;Yuta Tsubonouchi,&nbsp;Debraj Chandra and Masayuki Yagi*,&nbsp;","doi":"10.1021/acsaem.4c0321410.1021/acsaem.4c03214","DOIUrl":"https://doi.org/10.1021/acsaem.4c03214https://doi.org/10.1021/acsaem.4c03214","url":null,"abstract":"<p >Efficient photoanodes for visible-light-driven water oxidation are eagerly desired to construct practical water splitting systems to produce O₂ and H₂ using solar energy, which is one of the most prospective approaches for sustainable H₂ production. To further improve photoelectrochemical (PEC) water oxidation by a unique nitrogen-doped CuWO₄ (N-CuWO₄) photoanode, a Fe-co-deposited SnO_<i>x</i> (Fe-SnO_<i>x</i>) layer was formed on the photoanode surface by photoassisted electrodeposition. The incident photon-to-current conversion efficiency (IPCE) of the N-CuWO₄ photoanode was improved by 1.9 times at 1.23 V vs a reverse hydrogen electrode (RHE) by the Fe-SnO_<i>x</i> layer, which is contributed by the increased catalytic efficiency (η_cat) from 41.7 to 67.0%. Photoelectrochemical impedance spectroscopy (PEIS) measurement showed that the rate constant (<i>k</i>_O₂) of water oxidation at the surface increased from 5.5 to 10.2 s^–1 and the rate constant (<i>k</i>_rec) of surface recombination of photogenerated carriers decreased a little from 8.9 to 8.6 s^–1 by the Fe-SnO_<i>x</i> layer. This indicates a bifunctional role of the Fe-SnO_<i>x</i> catalyst layer in promoting the water oxidation reaction at the surface and suppressing the surface recombination of photogenerated carriers. For comparison with the case of a SnO_<i>x</i> layer (no Fe-<i>co</i>-deposition), the <i>k</i>_O₂ value (6.7 s^–1) of SnO_<i>x</i>/N-CuWO₄ electrodes was lower than that (10.2 s^–1) for the Fe-SnO_<i>x</i>/N-CuWO₄ electrode but higher than that (5.5 s^–1) for bare N-CuWO₄. Both SnO_<i>x</i> and Fe-SnO_<i>x</i> layers on the N-CuWO₄ surface improved <i>k</i>_O₂; however, the mechanism of improved <i>k</i>_O₂ is distinct between these layers: passivation effect of the SnO_<i>x</i> layer to prevent electron tunneling at the interface of the N-CuWO₄ surface/electrolyte and promotion effect of the Fe-SnO_<i>x</i> layer on water oxidation at the surface. The <i>k</i>_rec value (6.9 s^–1) for the SnO_<i>x</i>/N-CuWO₄ electrode was 1.3 times lower than that (8.9 s^–1) of the bare N-CuWO₄ electrode, which clearly shows the effect of the passivating SnO_<i>x</i> layer on the suppression of the surface recombination of photogenerated carriers.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3616–3627 3616–3627"},"PeriodicalIF":5.4,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675676","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":"Promising Multicomponent Cubic Alloys for Hydrogen Storage: Insights from First-Principles Calculations and Machine Learning","authors":"Zeineb Nefzi*,&nbsp;Celine Barreteau,&nbsp;Lucas Levrel and Jean-Claude Crivello*,&nbsp;","doi":"10.1021/acsaem.4c0272810.1021/acsaem.4c02728","DOIUrl":"https://doi.org/10.1021/acsaem.4c02728https://doi.org/10.1021/acsaem.4c02728","url":null,"abstract":"<p >An extensive exploration of the chemical space was conducted to design and identify promising multicomponent cubic alloys with appropriate enthalpy of reaction for hydrogen storage applications. We aim to identify alloys with suitable hydrogen absorption conditions for ambient conditions, according to favorable thermodynamic criteria, while addressing computational challenges in modeling large-scale systems. 18 elements were selected, leading to the systematic investigation of over 8000 quinary alloy systems across four distinct crystal phases (within solid–solution alloys, mono- and dihydrides). This effort resulted in a comprehensive data set of more than 34,000 equimolar <i>M</i>H_<i>x</i> structures, where <i>M</i> represents a combination of 5 elements chosen among the 18 selected atoms. To handle the computational demands of density functional theory (DFT) calculations on such a large scale of disordered supercells designed by the special quasirandom structure (SQS) method, a machine learning (ML) approach was introduced to accurately predict the enthalpy of hydride formation. By training the ML model on a strategically chosen subset of the data, high predictive accuracy was achieved while significantly reducing computational costs. By applying filtering parameters constrained by thermodynamic considerations, such as the value of plateau pressure or the presence of a single plateau, the integrated DFT-SQS-ML framework successfully identified 568 quinary alloy systems as ideal candidates for hydrogen storage. The findings establish a solid foundation for experimental validation and further advancements in the field of hydrogen storage materials.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3327–3337 3327–3337"},"PeriodicalIF":5.4,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675722","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":"Room-Temperature Hybrid Solid Polymer Electrolytes Incorporating Poly(vinylidene fluoride-co-hexafluoropropylene), Ionic Liquids, and Ceramic Particles for Solid-State Batteries","authors":"Maria Lucas,&nbsp;Renato Gonçalves,&nbsp;Tanja Kallio,&nbsp;Sara Pakseresht,&nbsp;Filipp Obrezkov,&nbsp;Stéphane Clain,&nbsp;Maria T. Malheiro,&nbsp;Senentxu Lanceros-Mendez and Carlos M. Costa*,&nbsp;","doi":"10.1021/acsaem.5c0018610.1021/acsaem.5c00186","DOIUrl":"https://doi.org/10.1021/acsaem.5c00186https://doi.org/10.1021/acsaem.5c00186","url":null,"abstract":"<p >This work presents the development of solid polymer electrolytes (SPEs) for next-generation solid-state batteries. Solid polymer electrolytes were prepared based on a polymer matrix (poly(vinylidene fluoride)-<i>co</i>-hexafluoropropylene (PVDF-HFP)) doped with 16 wt % ceramic particles (barium titanate oxide (BTO), barium strontium titanate (BST), and lead zirconate titanate (PZT)) and an ionic liquid (IL, [PMPyr][TFSI]) at 40 wt %. The ionic liquid allows improvement of the ionic conductivity of the system, whereas the ceramic particles are included to enhance the mechanical strength and thermal stability of the system. The physical, morphological, and electrochemical characteristics of the SPEs were studied. The addition of ceramic particles and ionic liquids does not affect the morphology, which remains a compact morphology. In the same way, the degree of crystallinity, polymer phase, and thermal properties of the SPE remain similar to the pristine polymer after filler addition. The inclusion of both ceramic particles and the ionic liquid allowed improvement of battery performance. Ionic conductivity in the order of 2.41 × 10^–5 S cm^–1 was achieved, accompanied by a battery capacity performance very close to theoretical values. Battery performance with PVDF-HFP/BST/IL (153 mAh g^–1) and PVDF-HFP/BTO/IL (148.2 mAh g^–1) composites proved to be successful in long-life cycling, bearing a higher capacity and stability compared to PVDF-HFP/IL (121.3 mAh g^–1). When varying C rates were applied, the PVDF-HFP/BST/IL sample presented superior results, revealing higher stability when compared to the other SPE samples. In conclusion, the fine-tuning of the ceramic particle type within SPE formulations offers an avenue for battery performance optimization. In particular, the inclusion of BST in the hybrid SPE composite allows improvement of battery cycling stability.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3904–3915 3904–3915"},"PeriodicalIF":5.4,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675720","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":"Sulfur Nanoparticles-Reinforced Hierarchical Assemblies of Carbon Nanotubes: Toward the Development of Efficient Lithium–Sulfur Micro-Battery Cathodes","authors":"Bikram Mondal,&nbsp;Saddam Hussain,&nbsp;Renqian Zhou,&nbsp;Mutalifu Abulikemu,&nbsp;Osman M. Bakr and Shahab Ahmad*,&nbsp;","doi":"10.1021/acsaem.5c0016210.1021/acsaem.5c00162","DOIUrl":"https://doi.org/10.1021/acsaem.5c00162https://doi.org/10.1021/acsaem.5c00162","url":null,"abstract":"<p >Lithium–sulfur (Li–S) battery technology provides one of the most promising alternatives to conventional lithium-ion batteries (LIBs). However, these Li–S batteries suffer from polysulfide dissolution leading to a shuttle effect, insulating nature, and volume expansion associated with sulfur particles. To mitigate these challenges, we present an approach of using sulfur nanoparticle (S NP)-reinforced patterned vertically aligned carbon nanotube (S@P-VACNT)-based microstructures as S cathodes for Li–S batteries. Engineered P-VACNT microstructures offer efficient charge transport pathways, trap lithium polysulfides (LiPSs), and reduce volume expansion of S NPs, which improve the performance of Li–S batteries. The demonstrated S@P-VACNT cathodes have delivered an excellent stable average discharge-specific capacity of ∼1030 mAhg^–1 for 100 cycles at 0.1 C with an average capacity decay of only ∼0.043% per cycle. Additionally, S cathodes have shown a remarkable average discharge-specific capacity of ∼890.03 mAh g^–1 for 500 cycles at 1.0 C, with a high-capacity retention of ∼99.81%, and ∼636.46 mAhg^–1 for 1000 cycles at 2.0 C. The structural integrity of P-VACNT and LiPS trapping is confirmed by postmortem FESEM and XPS studies of cycled cathodes, respectively. The demonstrated S@P-VACNT cathodes provide an out-of-the-box solution to overcome the long-standing technical challenges associated with Li–S batteries.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3877–3891 3877–3891"},"PeriodicalIF":5.4,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675881","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":"Boron-Containing Ternary Electrolyte for Excellent Li-Ion Transference and Stabilization of LiNMC-Based Cells","authors":"Zhaohan Liu,&nbsp;Amarshi Patra and Noriyoshi Matsumi*,&nbsp;","doi":"10.1021/acsaem.4c0280610.1021/acsaem.4c02806","DOIUrl":"https://doi.org/10.1021/acsaem.4c02806https://doi.org/10.1021/acsaem.4c02806","url":null,"abstract":"<p >In traditional carbonate electrolytes, lithium mobility is limited owing to the strong solvation effect between lithium ions and solvent sheaths. As a result, the lithium-ion transference number (t_Li⁺) is lower than 0.5 (mostly between 0.2 and 0.4), which indicates that anion transference is dominant in electrolyte’s charge conduction. In order to enhance lithium mobility in electrolytes, a low-polarity organic boron compound, mesityldimethoxyborane (MDMB), was added to conventional carbonate electrolytes to increase lithium-ion mobility. Two electrolyte systems with different MDMB ratios exhibited high t_Li⁺ as 0.93 for 111 (EC:DEC:MDMB = 1:1:1, volume ratio) and 0.86 for 112 (EC:DEC:MDMB = 1:1:2). Moreover, the stability of LiNMC cathodic half-cell was also improved by using 111 and 112 which form robust B-rich CEI. The activation energy for lithiation and resistance of CEI were decreased by MDMB. The durability of LiNMC cathodic half-cell was enhanced substantially under 1C CCCV mode. Cells with 111 and 112 electrolyte systems underwent more than twice as many cycles as conventional electrolytes.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3360–3368 3360–3368"},"PeriodicalIF":5.4,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675944","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":"Carbon-Supported In2O3 Cathode with a Solution-to-Solid Conversion Chemistry Enables Fast-Charging and Durable Aluminum Battery","authors":"Xin Tong,&nbsp;Yibo Song,&nbsp;Meng Zhang,&nbsp;Yuanguo Chen,&nbsp;Yakun Liu,&nbsp;Jinghui Chen,&nbsp;Weixiao Wang,&nbsp;Cheng Zhou,&nbsp;Fang Liu* and Jiashen Meng*,&nbsp;","doi":"10.1021/acsaem.4c0312810.1021/acsaem.4c03128","DOIUrl":"https://doi.org/10.1021/acsaem.4c03128https://doi.org/10.1021/acsaem.4c03128","url":null,"abstract":"<p >Conversion-type materials are promising cathodes with high theoretical capacities for rechargeable aluminum batteries (RABs). However, the cathodes are mainly based on a solid-to-solid conversion chemistry with sluggish reaction kinetics, resulting in a large volume change and severe electrode pulverization during cycling. Herein, a solution-to-solid conversion chemistry which resolves the cycling problems is found in carbon-supported In₂O₃ (In₂O₃@C) cathode, which exhibits fast-charging rate capability and excellent cycling stability in RABs. The In₂O₃@C architecture is featured with rod-shaped hollow carbon decorated with ultrafine In₂O₃ nanoparticles. The solid In₂O₃ converse into soluble InCl (In⁺) in the first discharge. In the following cycles, a reversible solution-to-solid conversion reaction occurs between soluble InCl (In⁺) and sparingly soluble InCl₃. The highly conductive carbon skeleton provides sufficient reaction sites to guarantee the reversible precipitation of solid InCl₃ as a charge product. Meanwhile, due to fast oxidation kinetics and the self-healing property of the solution phase, the Al|In₂O₃@C cell exhibits a high capacity of 335 mA h g^–1 with marginal cell overpotential of just 50 mV at 0.2 A g^–1, superior charging rate capability, and outstanding cycling stability at 5 A g^–1. This work provides insights into the development of cathode materials with a solution-to-solid reaction mechanism for high-performance RABs.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3553–3562 3553–3562"},"PeriodicalIF":5.4,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675943","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}