Advanced Energy Materials最新文献_第3页

Two‐Step Inverted Perovskite Solar Cells with > 25% Efficiency Fabricated in Ambient Air

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-04-05 DOI: 10.1002/aenm.202500830

Guoxin Wu, Jiancun Wang, Xinzhuo Fang, Jiashuo Xu, Xinxin Xia, Jianwei Zhao, Liqiang Zheng, Maojie Zhang, Zhaolai Chen, Haibo Chen, Liang Wang, William W. Yu

{"title":"Two‐Step Inverted Perovskite Solar Cells with > 25% Efficiency Fabricated in Ambient Air","authors":"Guoxin Wu, Jiancun Wang, Xinzhuo Fang, Jiashuo Xu, Xinxin Xia, Jianwei Zhao, Liqiang Zheng, Maojie Zhang, Zhaolai Chen, Haibo Chen, Liang Wang, William W. Yu","doi":"10.1002/aenm.202500830","DOIUrl":"https://doi.org/10.1002/aenm.202500830","url":null,"abstract":"The two‐step method for perovskite solar cells (PSCs) offers a promising technology for scalable manufacturing, particularly under ambient air conditions, due to its inherent simplicity, high reproducibility, and operational convenience. With this approach, achieving high‐quality of lead iodide (PbI2) films during the initial stage is paramount to ensuring the overall performance and stability of the devices. However, during the ambient fabrication of PbI2, the residual high boiling point and hygroscopic dimethyl sulfoxide (DMSO) solvent significantly compromises the resulting film quality. Here, L‐Homoarginine hydrochloride (HargCl) is introduced into the PbI2 precursor solution, which greatly reduced the residual amount of PbI2·xDMSO and passivated the internal defects of perovskite (PVK) films. By leveraging this strategy, inverted perovskite solar cells entirely in the air are successfully prepared, achieving an impressive power conversion efficiency (PCE) of 25.05% — the highest reported efficiency to date for two‐step fully air‐processed inverted PSCs. In addition, these unencapsulated devices maintained 96% of their initial power conversion efficiency after 500 h storage in the air with 20–40% RH.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"59 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143782440","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Surface Reconstruction Activates Non-Noble Metal Cathode for Proton Exchange Membrane Water Electrolyzer

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-04-03 DOI: 10.1002/aenm.202405846

Rui Wu, Heng Liu, Jie Xu, Ming-Rong Qu, You-Yi Qin, Xu-Sheng Zheng, Jun-Fa Zhu, Hao Li, Xiao-Zhi Su, Shu-Hong Yu

{"title":"Surface Reconstruction Activates Non-Noble Metal Cathode for Proton Exchange Membrane Water Electrolyzer","authors":"Rui Wu, Heng Liu, Jie Xu, Ming-Rong Qu, You-Yi Qin, Xu-Sheng Zheng, Jun-Fa Zhu, Hao Li, Xiao-Zhi Su, Shu-Hong Yu","doi":"10.1002/aenm.202405846","DOIUrl":"https://doi.org/10.1002/aenm.202405846","url":null,"abstract":"Hydrogen generation via a proton exchange membrane (PEM) electrolyzer manifests the vertex of fundamental and practical studies on technology transferring electricity into hydrogen fuels. However, the harsh working conditions, especially the strong reductive acidic electrolyte-catalyst interface, make non-noble metal-based cathodes unsuitable for PEM electrolyzer. Here, a scale-up application of F modified CoP (CoP|F) cathode is demonstrated from 0.2 cm2 lab-scale three-electrode setup to a commercial 38 cm2 PEM electrolyzer. The operando X-ray absorption spectroscopy (XAS) and Raman results confirm that F modification can promote the breakage of Co─P bonds, reconstructed to amorphous metallic Co as true HER active sites. Density functional theory (DFT) calculations reveal that the presence of F in the CoP1-x lattice would lead to a more facile formation of P-vacancy under HER conditions, leading to more active zerovalent Co active sites for HER. This reconstructed surface shows high activity and tolerance in the reductive acidic electrolyte-catalyst interface. When used as a cathode in a commercial PEM electrolyzer, its performance is comparable to the state-of-the-art Pt/C catalyst, with a calculated hydrogen cost to be 2.17 $ kgH2−1. This work suggests a surface-reconstruction pathway to fabricate cost-saving and durable non-noble metal-based cathodes for commercial PEM electrolyzers.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"6 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776213","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

The Nonsteady-State Structural and Chemical Reconstruction of Ni-Rich Cathodes During the Intermittent Resting after Charging

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-04-03 DOI: 10.1002/aenm.202405907

Weijing Yuan, Wei Peng, Changxu Wu, Na Liu, Chongheng Shen, Zuoguo Xiao, Jinquan Liu, Chenxi Li, Yi Guo, Qiqiang Huang, Peng Zhang, Hongkun Pan, Lianghao Wen, Lewei Shi, Languang Lu, Dongsheng Ren, Kai Wu, Minggao Ouyang, Xiang Liu

{"title":"The Nonsteady-State Structural and Chemical Reconstruction of Ni-Rich Cathodes During the Intermittent Resting after Charging","authors":"Weijing Yuan, Wei Peng, Changxu Wu, Na Liu, Chongheng Shen, Zuoguo Xiao, Jinquan Liu, Chenxi Li, Yi Guo, Qiqiang Huang, Peng Zhang, Hongkun Pan, Lianghao Wen, Lewei Shi, Languang Lu, Dongsheng Ren, Kai Wu, Minggao Ouyang, Xiang Liu","doi":"10.1002/aenm.202405907","DOIUrl":"https://doi.org/10.1002/aenm.202405907","url":null,"abstract":"Lithium-ion batteries are the main power source for portable devices and electric vehicles due to their high energy density and low self-discharge rate. In practical applications, batteries often experience extended resting periods at high charge levels after being fully charged. However, most studies focus on continuous cycling without considering intermittent resting, which can lead to flawed failure analysis and hinder optimization of Ni-rich cathode batteries. This study explores the degradation mechanisms of Ni-rich cathode full-cells subjected to intermittent resting after charging, revealing that Ni-rich cathodes undergo nonsteady-state structure transitions and chemical changes during high charge rest periods. The findings show that intermittent resting intensifies interfacial cracking within secondary particles due to coupled structure transitions and interfacial reactions, degrading lithium transport kinetics and creating lithium concentration gradients at multiple scales. Prolonged high anisotropy from delayed delithiation in the central region of primary particles, combined with surface-related multiple heterogeneous pinning effects, induces further intracrystalline damage. This damage is repeatedly reset and activated during intermittent resting, worsening mechanical degradation. These insights into the degradation pathways of Ni-rich cathodes provide a foundation for designing more durable materials and battery architectures to enhance the performance and longevity of lithium-ion batteries in practical applications.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"22 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143767141","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Sn-Mediated Local Atomic Ordering Enhances Reversible Anionic Redox Activity in Cation-Disordered Li1.3Mn0.4Nb0.3O2 Cathodes

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-04-02 DOI: 10.1002/aenm.202500217

Gang Sun, Dan Nie, Qingjun Zhu, Lijun Gao, Yi-Hung Chang, Han Liu, Jiayi Yang, Yang Ren, Yu-Cheng Shao, Hirofumi Ishii, Xulei Sui, PanPan Wang, Hsiao-Tsu Wang, Zhenbo Wang

{"title":"Sn-Mediated Local Atomic Ordering Enhances Reversible Anionic Redox Activity in Cation-Disordered Li1.3Mn0.4Nb0.3O2 Cathodes","authors":"Gang Sun, Dan Nie, Qingjun Zhu, Lijun Gao, Yi-Hung Chang, Han Liu, Jiayi Yang, Yang Ren, Yu-Cheng Shao, Hirofumi Ishii, Xulei Sui, PanPan Wang, Hsiao-Tsu Wang, Zhenbo Wang","doi":"10.1002/aenm.202500217","DOIUrl":"https://doi.org/10.1002/aenm.202500217","url":null,"abstract":"Recent advances in lithium-ion batteries have revealed the potential of Li-excess cation-disordered rock salt (DRX) cathodes, which expand the design space for cathode materials. The evidence of facile lattice substitution further provides a key strategy for activating redox reaction centers and enhancing the cycling performance of such materials. Here, the study explores how Sn-mediated local atomic ordering enhances reversible anionic redox activity in Li1.3Mn0.4Nb0.3O2 through the use of aberration-corrected scanning transmission electron microscopy, ex/in situ X-ray techniques, and theoretical calculation. The results demonstrate that Sn incorporation optimizes the local atomic structure, fostering the formation of rapid Li+ diffusion “elevator” pathways and short-range ordered structures, thereby enhancing the Li+ transport network. Additionally, quantitative analysis of the redox pathways and degree of participation for Mn and O during charge–discharge cycles reveals that the Sn-mediated electrode exhibits enhanced anionic O redox activity at high charging voltages, maintaining elevated activity throughout subsequent cycling. This sustained performance not only indicates increased redox capabilities but also suggests improved structural stability. By elucidating the complex interplay between composition, local structure, and performance, this study advances the understanding of DRX materials and underscores the potential of strategic elemental substitution for optimizing disordered cathode materials in next-generation energy storage systems.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"22 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758524","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Industrial Scalability of Zinc-Ion Batteries: Enhanced Electrochemical Performance with High Mass Loading Electrodes on Graphene-Coated Metal Current Collectors

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-04-02 DOI: 10.1002/aenm.202500261

Heeyeon Heo, Jaeyeon Lee, Yong-Ryun Jo, Geon-Hyoung An

{"title":"Industrial Scalability of Zinc-Ion Batteries: Enhanced Electrochemical Performance with High Mass Loading Electrodes on Graphene-Coated Metal Current Collectors","authors":"Heeyeon Heo, Jaeyeon Lee, Yong-Ryun Jo, Geon-Hyoung An","doi":"10.1002/aenm.202500261","DOIUrl":"https://doi.org/10.1002/aenm.202500261","url":null,"abstract":"Zinc-ion batteries (ZIBs) have emerged as a promising energy storage solution due to their inherent safety, environmental sustainability, and cost-effectiveness. Utilizing water-based electrolytes, ZIBs eliminate fire risks and thermal runaway concerns, making them ideal for large-scale energy storage systems. The high theoretical capacity, low cost, high abundance, and low toxicity of zinc further enhance its suitability for grid-scale applications. However, conventional current collectors such as graphite foil exhibit limitations in scalability and mechanical properties, which make them unsuitable for industrial roll-to-roll manufacturing processes. This study addresses these limitations by exploring graphene-coated stainless steel foil as an alternative current collector. Here, graphene coating followed by heat treatment to remove the surface oxides improves the conductivity and corrosion resistance of the material. As a result, the fabricated ZIB exhibits high specific capacities of 1.90 and 0.91 mAh cm−2 at current densities of 0.3 and 2.0 C, respectively, and demonstrate a remarkable long cycle life with a capacity retention of 88.7% for up to 1500 cycles at a current density of 1.0 C, despite a high electrode loading of 13.27 mg cm−2. This innovation enhances the electrochemical performance and cycling stability, thereby advancing large-scale ZIBs as a safe, scalable, and high-performance solution.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"66 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758525","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Ru Single Atoms Anchored on Co3O4 Nanorods for Efficient Overall Water Splitting under pH-Universal Conditions

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-04-02 DOI: 10.1002/aenm.202500700

Yongfang Zhou, Yu Mao, Cuizhu Ye, Ziyun Wang, Shanghai Wei, John V. Kennedy, Yufei Zhao, Hui Yang, Bruce C. C. Cowie, Geoffrey I. N. Waterhouse

{"title":"Ru Single Atoms Anchored on Co3O4 Nanorods for Efficient Overall Water Splitting under pH-Universal Conditions","authors":"Yongfang Zhou, Yu Mao, Cuizhu Ye, Ziyun Wang, Shanghai Wei, John V. Kennedy, Yufei Zhao, Hui Yang, Bruce C. C. Cowie, Geoffrey I. N. Waterhouse","doi":"10.1002/aenm.202500700","DOIUrl":"https://doi.org/10.1002/aenm.202500700","url":null,"abstract":"Single-atom catalysts (SACs) show great promise for electrocatalytic water splitting due to their exceptional metal atom utilization efficiency. Herein, it is demonstrated that Ru single atoms (SAs) anchored on Co3O4 nanorod arrays (Rux-Co3O4, where x is the Ru loading in weight percent) afford outstanding electrocatalytic performance and durability for the oxygen evolution reaction (OER), hydrogen evolution reaction (HER), and overall water splitting across a wide pH range (0.3–14). Ru8%-Co3O4 achieves 10 mA cm⁻2 at overpotentials of only 214, 286, and 138 mV for OER, and 13, 72, and 59 mV for HER, in 1 m KOH, 0.1 m PBS, and 0.5 m H2SO4, respectively, outperforming benchmark RuO2 and Pt/C catalysts. When Ru8%-Co3O4 is utilized as the anode and cathode catalysts in an anion exchange membrane water electrolyzer (AEMWE), a cell voltage of only 2.06 V is required to achieve 1 A cm⁻2. Chronopotentiometry verified Ru8%-Co3O4 possesses excellent stability during both OER and HER at 100 mA cm⁻2 in acidic, neutral, and alkaline media. Density functional theory (DFT) calculations reveal that the abundant Ru-O-Co interfaces in Ru8%-Co3O4 shift the d-band center from −1.72 eV (for Ru cluster/Co3O4) to −1.58 eV (for Ru SA/Co3O4), creating more energetically favorable pathways for OER and HER.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"58 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758526","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

A “Cool” Route to Battery Electrode Material Recovery

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-04-02 DOI: 10.1002/aenm.202405924

Lin Chen, Brij Kishore, Bowen Liu, Tengfei Song, Yazid Lakhdar, Osaze Omoregbe, Melanie M Britton, Peter R Slater, Emma Kendrick

{"title":"A “Cool” Route to Battery Electrode Material Recovery","authors":"Lin Chen, Brij Kishore, Bowen Liu, Tengfei Song, Yazid Lakhdar, Osaze Omoregbe, Melanie M Britton, Peter R Slater, Emma Kendrick","doi":"10.1002/aenm.202405924","DOIUrl":"https://doi.org/10.1002/aenm.202405924","url":null,"abstract":"The increasing demand for alkali metal-ion batteries necessitates efficient and sustainable recycling solutions for both end-of-life batteries and production scrap. This study introduces a novel, cost-effective, and scalable electrode delamination technique, termed “ice-stripping,” which employs sub-zero freezing to achieve near-complete (>90%) recovery of electrode coatings. Water is sprayed onto the electrode surface and placed on a sub-zero surface; the water freezes, forming a strong interfacial bond of the electrode coating to the cold plate. This enables the current collector to be stripped away from the electrode due to the stronger adhesion of the electrode to the plate. Unlike conventional thermal or chemical delamination methods, ice-stripping minimizes energy consumption, eliminates hazardous chemicals, and preserves the morphology and integrity of reclaimed materials. The technique is successfully applied to scrap and end-of-life lithium-ion and sodium-ion battery electrodes with various binder systems. Case studies focus on the recovery efficiencies and potential for direct recycling of Prussian white and hard carbon electrodes, graphite from end-of-life cells, and cathode and anode manufacturing scrap. Scalability and integration are also discussed. Given its efficiency and sustainability, ice-stripping represents a transformative step forward in battery recycling technology, reducing environmental impact and promoting material circularity.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"25 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758527","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Zinc Ion Transport Kinetics in Zinc-based Batteries and Its Regulation Strategy

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-04-02 DOI: 10.1002/aenm.202500316

Yunting Yang, Zhoujie Tang, Shuyang Bian, Yalan Gu, Fei Ye, Wenshu Chen, Kongjun Zhu, Yuping Wu, Linfeng Hu

{"title":"Zinc Ion Transport Kinetics in Zinc-based Batteries and Its Regulation Strategy","authors":"Yunting Yang, Zhoujie Tang, Shuyang Bian, Yalan Gu, Fei Ye, Wenshu Chen, Kongjun Zhu, Yuping Wu, Linfeng Hu","doi":"10.1002/aenm.202500316","DOIUrl":"https://doi.org/10.1002/aenm.202500316","url":null,"abstract":"Rechargeable zinc-ion batteries (ZIBs) have gained significant attention as potential next-generation energy storage systems, owing to their inherent safety, environmental benignity, and cost-effectiveness. However, the substantial electrostatic repulsion of Zn ion results in a sluggish kinetics for its insertion into the cathode material. Meanwhile, the formation of hydrated ionic groups with increased mass and volume in the aqueous electrolyte further hampers the transport ability of zinc ions, significantly impacting the overall electrochemical performance (including capacity, energy density, rate-capability, and cyclability) of aqueous zinc-ion batteries. This review systematically summarized the recent progress in the regulation strategy of the zinc-ion transport kinetics. The as-reported mechanisms are introduced for zinc ion transport in ZIBs (Zn2+ insertion/extraction mechanism, H+ or H2O/ Zn2+ co-insertion/extraction mechanism, conversion reaction mechanism, and coordination reaction mechanism). Then, cathode material design for fast zinc-ion transport kinetics including soft lattice construction, doping effects, defect introduction, morphology control, and interface design is systematically summarized. Finally, it is concluded with future research directions, such as high-entropy design, multi-scale simulation, and machine study, providing a roadmap for developing high-performance zinc ion batteries at ultralow operation temperatures.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"32 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758528","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Tuning Polysulfides into Clustered-States via Non-coordinating Molecular Encapsulation to Achieve an Alternative Kinetics in Li─S Batteries 通过非配位分子封装将多硫化物调谐成团簇态，在锂离子电池中实现替代动力学

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-04-02 DOI: 10.1002/aenm.202500802

Qingyi Zheng, Leyuan Cui, Xiaojiao Zhao, Ruming Yuan, Chutao Wang, Kun Wang, Jingmin Fan, Mingsen Zheng, Quanfeng Dong

{"title":"Tuning Polysulfides into Clustered-States via Non-coordinating Molecular Encapsulation to Achieve an Alternative Kinetics in Li─S Batteries","authors":"Qingyi Zheng, Leyuan Cui, Xiaojiao Zhao, Ruming Yuan, Chutao Wang, Kun Wang, Jingmin Fan, Mingsen Zheng, Quanfeng Dong","doi":"10.1002/aenm.202500802","DOIUrl":"https://doi.org/10.1002/aenm.202500802","url":null,"abstract":"The practical application of lithium–sulfur batteries is hindered by the polysulfide shuttle effect and sluggish kinetics inherent in solid–liquid–solid conversion mechanism, particularly under lean electrolyte conditions (<5 µL mg⁻¹). Weakly solvating electrolytes and localized high-concentration electrolytes can suppress polysulfide dissolution and enable a quasi-solid-phase mechanism but suffer from severely limited reaction kinetics. Herein, a clustered-polysulfide-mediated sulfur conversion mechanism enabled by a novel electrolyte composed of 1,2-dimethylbenzene (DTL) and 1,2-dimethoxyethane (DME) is proposed. The encapsulation effect of DTL and the coordination of TFSI⁻ with polysulfides drives the aggregation of polysulfides so that the clustered polysulfides with virtual shell boundaries can be the new basic reactive that bridges the gap between the traditional dissolution-dominated mechanism and quasi-solid-state mechanism. The clustered polysulfide electrolyte (CPE) not only suppresses the shuttle effect and stabilizes the lithium anode by mitigating parasitic reactions but also enables alternative reaction kinetics and promotes 3D Li₂S deposition, minimizing electrode passivation. Ultimately, lithium–sulfur batteries can achieve excellent electrochemical performance and can stably operate under lean electrolyte (<4.0 µL mg⁻¹) with an area capacity of >4 mAh cm−2. This work elucidates the relationship between polysulfide dissolution behavior and redox kinetics, providing a new insight into the understanding of complex sulfur conversion mechanisms.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"199 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758593","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

A Novel Ti12-Based Metal-Organic Framework for Photocatalytic Hydrogen Evolution

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-04-01 DOI: 10.1002/aenm.202500211

Bingbing Chen, Asma Mansouri, Celia M. Rueda-Navarro, Iurii Dovgaliuk, Philippe Boullay, Arianna Melillo, Juan José Ramírez-Hernández, Beibei Xiao, Dong Fan, Lokuge Aravindani Fernando, Gilles Patriarche, Ieuan Cornu, Pierre Florian, Guillaume Maurin, Sergio Navalón, Hermenegildo Garcia, Georges Mouchaham, Christian Serre

{"title":"A Novel Ti12-Based Metal-Organic Framework for Photocatalytic Hydrogen Evolution","authors":"Bingbing Chen, Asma Mansouri, Celia M. Rueda-Navarro, Iurii Dovgaliuk, Philippe Boullay, Arianna Melillo, Juan José Ramírez-Hernández, Beibei Xiao, Dong Fan, Lokuge Aravindani Fernando, Gilles Patriarche, Ieuan Cornu, Pierre Florian, Guillaume Maurin, Sergio Navalón, Hermenegildo Garcia, Georges Mouchaham, Christian Serre","doi":"10.1002/aenm.202500211","DOIUrl":"https://doi.org/10.1002/aenm.202500211","url":null,"abstract":"A new microporous titanium-based metal-organic framework (Ti-MOF), labeled as MIP-209(Ti) (MIP: Materials from Institute of Porous Materials of Paris), features nitro terephthalate ligands and Ti12O15 oxo-clusters, as revealed by continuous rotation electron diffraction (cRED). MIP-209(Ti) can be obtained using two different terephthalate (1, 4-BDC2−) derivatives such as NO2-BDC and 2Cl-BDC in an eco-friendly solvent, suggesting the isostructural versatility of Ti12-MOFs. Alternatively, its Ti-oxo-cluster can be tuned, similarly to MIP-177(Ti)-LT bearing the same Ti12O15 sub-unit. Typically, low percentage Cr3+ doping (≤5 at%) in MIP-209(Ti) favorably enhances the water stability. MIP-209(Ti-Cr)-NO2 shows a significant hydrogen production rate, with good reusability and stability under simulated solar light irradiation. Compared to the benchmark Ti-MOF IEF-11, the hydrogen production of MIP-209(Ti-Cr)-NO2 with 5 at% Cr doping has a fourfold enhancement in photocatalytic hydrogen evolution from water splitting reaction (HER) during 5 h in presence of methanol (5 812 µmol/gcat against 1 391 µmol/gcat), as well as, without any noble metal co-catalyst, a sixfold enhancement in overall water splitting reaction (OWS) (681 and 325 µmol/gcat of H2 and O2, respectively, against 94 and 53 µmol/gcat of H2 and O2, respectively). This work represents a leap forward in the synthesis of Ti-MOFs and their practical photocatalytic applications.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"32 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745394","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0