{"title":"Finding a Novel Borate Ferroelectric with Random Domain Structures for Deep-UV Quasi-Phase-Matching","authors":"Yabo Wu, Chen Cui, Zhongchang Wang, Junjie Li, Jian Han, Miriding Mutailipu, Shilie Pan","doi":"10.1002/adma.202505930","DOIUrl":"https://doi.org/10.1002/adma.202505930","url":null,"abstract":"Finding competitive nonlinear optical (NLO) crystals for practical deep-ultraviolet (deep-UV) lasers remains a fundamental yet challenging goal in photonic materials research. The production of deep-UV lasers through the mesoscopic domain structure of ferroelectric materials has been a popular research area via quasi-phase-matching (QPM). However, as of right present, no ferroelectric in the deep-UV area is able to provide QPM laser output. Here, a new room-temperature borate ferroelectric Ba<sub>3</sub>Mg<sub>3</sub>(BO<sub>3</sub>)<sub>3</sub>F<sub>3</sub> (BMBF) is presented. The ferroelectricity of BMBF crystals exhibits significant relaxor behavior and the random domain structure can relax the strict phase-matching conditions, rendering it a disordered NLO medium. Benefiting from its unique ferroelectric properties, BMBF crystal achieves a second-harmonic generation output energy of 3.55 µJ for 398 to 199 nm wavelength frequency conversion, even in the absence of birefringent phase-matching conditions. This result demonstrates that BMBF is a promising candidate for deep-UV QPM applications. Furthermore, this study expands the frontiers of borate ferroelectrics while the realization of deep-UV light output using BMBF crystal motivates and provides a path for its broader application.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"26 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177272","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}
{"title":"Tuning Surface Coordination Environment of Ni3N by Fluorine Modification for Efficient Methanol Electrooxidation Assisted Hydrogen Evolution","authors":"Hongye Qin, Jinhong Li, Guangliang Lin, Kangnan Yuan, Haocheng Yang, Yukun Ye, Ting Jin, Fangyi Cheng, Lifang Jiao","doi":"10.1002/adma.202507573","DOIUrl":"https://doi.org/10.1002/adma.202507573","url":null,"abstract":"Replacing the kinetically sluggish oxygen evolution reaction with the thermodynamically favorable methanol oxidation reaction (MOR) represents a promising strategy for energy-efficient hydrogen production. However, optimizing electrocatalytic performance in the coupled hydrogen evolution reaction (HER) and MOR requires precise regulation of the electrochemical coordination environment and a fundamental understanding of activity origins, posing a significant challenge. Here, a scalable strategy is developed that harnesses the high electronegativity of fluorine (F) to tailor the coordination environment of Ni<sub>3</sub>N, enhancing HER kinetics. Concurrently, adsorbed F ions induce rapid and extensive self-reconstruction of the Ni<sub>3</sub>N surface during MOR by dynamically modulating interfacial ion concentrations (OH⁻ and Ni species). This reconstruction enhances catalytic activity and enables the selective oxidation of methanol to formate via a sequential pathway, involving primary O-H bond activation followed by subsequent C-H bond cleavage at Ni active sites. Consequently, F<sub>10</sub>-Ni<sub>3</sub>N demonstrates exceptional bifunctional performance, delivering 2.02 V and remarkable stability (600 h) for MOR-coupled hydrogen production in a membrane electrode assembly-based flow electrolyzer at an industrially relevant current density of 200 mA cm<sup>−2</sup>. This work establishes a dual-regulation paradigm for electrocatalysts, offering mechanistic insights into surface reconstruction and a rational design framework for next-generation energy conversion systems.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"14 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177281","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}
{"title":"Origami Silicon Anodes: Geometric Design for Structural Elasticity and Connectivity","authors":"Haimei Li, Ziyun Zhao, Mengwei Sun, Nannan Kuang, Yingxin Liu, Yong Guo, Yibo Zhang, Fanqi Chen, Qinyi Zhan, Anni Liu, Yue Zhai, Qing He, Yunpei Yue, Yun Tian, Shichao Wu, Quan‐Hong Yang","doi":"10.1002/adma.202503745","DOIUrl":"https://doi.org/10.1002/adma.202503745","url":null,"abstract":"Achieving stable cycling of high‐capacity battery electrodes with large volume changes remains a significant challenge, with their mechanical failure and sluggish kinetics, primarily due to inadequate structural accommodation and inefficient transport pathways. Here, a magnesiothermic crystallization approach is presented to construct origami capsule (OC) architectures, imparting flexibility and conformability to inherently brittle silicon, featuring highly interconnected 2D silicon nanosheets (2.5 nm thickness) with built‐in nanopores encapsulated within a pressure‐tolerant conformal microshell. The design leverages geometric features at both the nanoscale (within nanosheets) and microscale (capsule assembly) to impart structural elasticity and connectivity for efficient stress dissipation, enhancing mechanical integrity and rapid transport kinetics. Consequently, the OC anode exhibits low electrode swelling (14.7%) at 2945 mAh g<jats:sup>−1</jats:sup> and exceptional rate capability, delivering a high capacity and ≈100% retention after 470 cycles at a large current density of 6 A g<jats:sup>−1</jats:sup>. This work bridges geometric design and materials science, opening new avenues for high‐performance energy storage solutions.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"51 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144176593","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}
Kai Wang, Youqi Chu, Zhencheng Huang, Hang Yang, Ming Yang, Yongbiao Mu, Xinhua Tan, Guanjie He, Mingjian Zhang, Lin Zeng, Biao Li, Feng Pan, Jiangtao Hu
{"title":"Unleashing the Kinetic Limitation of Co-Free Li-Rich Mn-Based Cathodes via Ionic/Electronic Dual-Regulation","authors":"Kai Wang, Youqi Chu, Zhencheng Huang, Hang Yang, Ming Yang, Yongbiao Mu, Xinhua Tan, Guanjie He, Mingjian Zhang, Lin Zeng, Biao Li, Feng Pan, Jiangtao Hu","doi":"10.1002/adma.202504642","DOIUrl":"https://doi.org/10.1002/adma.202504642","url":null,"abstract":"Li-rich Mn-based oxide (LRMO) are promising cathode candidates for next-generation Li-ion batteries with combined cost-effectiveness and high specific capacity. Designing Co-free LRMO can further leverage the low cost of this class of cathodes given the capacity can be maintained. However, implementing cobalt-free LRMO cathode materials are hampered by their sluggish kinetics, resulting in low capacity and poor rate performance that underperform compared with their Co-containing counterparts. Here, it is confirmed that the slow kinetics of Co-free LRMO originates from the structural disorder caused by transition metals (TMs) migration at high voltages (above 4.5 V Vs. Li<sup>+</sup>/Li) and consequent irreversible oxygen redox process. Aware of this, Na<sup>+</sup>/F<sup>−</sup> is introduced in surficial lattice to alleviate these issues, ultimately achieving improved discharge voltage (≈0.2 V above 1 C, 1 C = 0.25 A g<sup>−1</sup>), exceptional cycle stability in pouch-type cell (95.1% capacity retention in 1 C after 400 cycles at 25 °C, and 80.9% capacity retention after 300 cycles in 0.5 C at 45 °C) and excellent C-rate performance (≈150 mA h g<sup>−1</sup> at 5 C). The newly developed Na<sup>+</sup>/F<sup>−</sup> gradient design unleashes the surficial charge transfer kinetics limitation and greatly improves the lattice structure stability, consequently providing valuable guidelines for future high-capacity LRMO cathode design.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"43 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177163","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}
{"title":"Flexible and High-Performance Solution-Processable Single-Detector Organic Spectrometer","authors":"Yu Zhu, Zhe Zhang, Hao Qin, Yanqing Yang, Jing Zhang, Zhaoyang Yao, Guanghui Li, Yongsheng Chen","doi":"10.1002/adma.202502608","DOIUrl":"https://doi.org/10.1002/adma.202502608","url":null,"abstract":"Spectrometers are indispensable tools for civil and military-related optoelectronic applications. To meet the requirements of the revolutionary data/AI-driven era, next-generation spectrometers must not only be flexible with minimal sizes but exhibit high accuracy and resolution. In this study, a compact, high-performance, and flexible organic spectrometer is reported, fabricated using solution processing, which employs an optical cascade architecture by integrating organic electrochromic devices and photodetectors. This organic spectrometer can not only achieve a resolution of 0.56 nm, an accuracy of 0.14 nm, and a broad detection range from 400 to 1000 nm but also realize a vital absolute spectral irradiance measurement ranging from 10<sup>−8</sup> to 10<sup>−4</sup> W cm<sup>−2</sup> nm<sup>−1</sup>. Additionally, its intrinsic flexibility and highly replaceable feasibility of bandgap-tunable organic materials enable their high applicability with excellent portability and adaptability in the upcoming data/AI-driven era or scenarios.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"5 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177277","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}
{"title":"Dual Strategy of Ca2+ Influx and Collagen Denaturation to Remodel the Extracellular Matrix and Amplify Sonopiezoelectric Therapy","authors":"Chenghao Yu, Desheng Chen, Dingcheng Zhu, Lili Feng, Lu Yang, Elyor Berdimurodov, Pengyu Zang, Yanlin Zhu, Yaoyu Hu, Jiaxu Sang, Piaoping Yang","doi":"10.1002/adma.202501642","DOIUrl":"https://doi.org/10.1002/adma.202501642","url":null,"abstract":"Extracellular matrix (ECM), a core member of tumor microenvironment, is ≈1.5-fold harder than the surrounding normal tissues. Regulating the stiffness of ECM can significantly impact physiological activities of tumor cells, such as growth, differentiation, and migration. Herein, a sonopiezoelectric-response nanoplatform consisting of Cu<sub>3</sub>BiS<sub>3</sub> nanospheres (CBS NSs) is constructed for ECM remodeling. Sonopiezoelectric therapy (SPT) and chemodynamic therapy (CDT) are conducted using ultrasound (US) and near-infrared irradiation. Under US irradiation, the mechanical strain of CBS NSs causes piezoelectric polarization and promotes a redox reaction through energy band bending. The built-in electric field generated by US irradiation amplifies the efficiency of the Fenton-like reaction and substantially enhances reactive oxygen species production. Moreover, piezoelectric property-mediated electrical signals can allow Ca<sup>2+</sup> influx, upregulating the levels of matrix metalloproteinase (MMP)-2 and MMP-9. Integrating US irradiation with near-infrared irradiation generates localized heat, which can effectively denature tumor collagen, reduce tumor stiffness, and enhance the permeability of CBS NSs into solid tumors, thus improving the SPT effect. The combination of MMP upregulation and collagen degradation can maximize the benefits of ECM remodeling and synergistically enhance the cancer therapeutic efficacy of SPT/CDT. This SPT/CDT synergistic therapy and ECM remodeling platform is an innovative strategy for cancer therapy.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"2 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177365","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}
Le Li, Jianjun Xu, Lei Fang, Zewu Feng, Hailong Huang, Yanbo Wang, Yansen Guo, Shuilong Kang, Hui Wang, Yujie Han, Yi Ji, Huanyu Zhang, Yong Ding, Mohammad Khaja Nazeeruddin, Bin Ding, Xiaohong Zhang, Jun Peng
{"title":"Active Passivation Charge Transport in n-i-p Perovskite Solar Cells Approaching 26% Efficiency","authors":"Le Li, Jianjun Xu, Lei Fang, Zewu Feng, Hailong Huang, Yanbo Wang, Yansen Guo, Shuilong Kang, Hui Wang, Yujie Han, Yi Ji, Huanyu Zhang, Yong Ding, Mohammad Khaja Nazeeruddin, Bin Ding, Xiaohong Zhang, Jun Peng","doi":"10.1002/adma.202503903","DOIUrl":"https://doi.org/10.1002/adma.202503903","url":null,"abstract":"In n-i-p planar perovskite solar cells (PSCs), the electron transport layer (ETL) and the hole transporting layer play a crucial role in realizing high power conversion efficiency (PCE). Herein, a TiO<sub>2</sub>-SDBA-SnO<sub>2</sub> stacked ETL is reported, where 4,4′-sulfonyldibenzoic acid (SDBA) serves as an active passivation agent to suppress charge recombination and enhance interface quality. SDBA effectively passivates oxygen vacancies in sputtered TiO<sub>2</sub>, while simultaneously promoting SnO<sub>2</sub> nucleation and improving film quality. Moreover, its molecular structure increases the surface free energy of the ETL, facilitating the formation of high-quality perovskite films with larger grain sizes and fewer defects. As a result, PSCs with this optimized ETL achieve a PCE of 25.94% with excellent stability. This approach also enables the fabrication of perovskite solar modules with a certified efficiency of 22.55% over a 26.02 cm<sup>2</sup> aperture area.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"43 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177278","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}
Ying-Chun Cheng, Xun Tang, Rajat Walia, Tong-Yuan Zhang, Xiao-Chun Fan, Jia Yu, Kai Wang, Chihaya Adachi, Xian-Kai Chen, Xiao-Hong Zhang
{"title":"High-Efficiency and High Color Purity Solution-Processable Deep-Blue OLEDs Enabled by Linearly Fully Fused Acceptor-Donor-Acceptor Molecular Design","authors":"Ying-Chun Cheng, Xun Tang, Rajat Walia, Tong-Yuan Zhang, Xiao-Chun Fan, Jia Yu, Kai Wang, Chihaya Adachi, Xian-Kai Chen, Xiao-Hong Zhang","doi":"10.1002/adma.202500010","DOIUrl":"https://doi.org/10.1002/adma.202500010","url":null,"abstract":"Solution-processable organic light-emitting diodes (OLEDs) have attracted much attention from academia and industry because of their advantages such as low production cost and suitability for large-scale production. However, solution-processable deep-blue OLEDs that simultaneously have high efficiencies and satisfy the BT.2020 standard remain still a great challenge. To address this issue, here a tetraboron multiresonance thermally activated delayed fluorescence (MR-TADF) emitter, tBO-4B, embedded with two soluble 2,12-di-tert-butyl-5,9-dioxa-13b-boranaphtho[3,2,1-de]anthracene groups is designed and synthesized with a linearly fully fused acceptor–donor–acceptor-type molecular structure. tBO-4B not only achieves an ultranarrow full width at half maximum of 12 nm but also has a negligibly small singlet-triplet energy gap and large spin‒orbit coupling, eventually leading to very fast reverse intersystem crossing rate (4.23 × 10<sup>6</sup> s<sup>−1</sup>). The sensitizer-free solution-processed OLED exploiting tBO-4B as the emitter achieves an ultrahigh maximum external quantum efficiency (EQE<sub>max</sub>) of 30.3%, with Commission Internationale de l’Éclairage (CIE) coordinates of (0.147, 0.042) meeting the BT.2020 blue standard. In addition, the corresponding sensitizer-free vacuum-processed deep-blue devices also exhibit an impressive EQE<sub>max</sub> of 39.6% and mild efficiency roll-off with CIE coordinates of (0.147, 0.043). This work will facilitate the development of high-efficiency ultrapure deep-blue MR-TADF materials for solution- and vacuum-processed OLEDs.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"27 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177159","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}
Lingbin Ye, Yun Gao, Yifeng Feng, Xiaofang Zhu, Zichao Ma, Dingshuo Zhang, Yifan He, Haiping He, Zhizhen Ye, Xingliang Dai
{"title":"Suppressing Interlayer Ion Migration in CsPbX3 Nanocrystal Films for Realizing Efficient and Stable Electroluminescence","authors":"Lingbin Ye, Yun Gao, Yifeng Feng, Xiaofang Zhu, Zichao Ma, Dingshuo Zhang, Yifan He, Haiping He, Zhizhen Ye, Xingliang Dai","doi":"10.1002/adma.202505214","DOIUrl":"https://doi.org/10.1002/adma.202505214","url":null,"abstract":"Mixed-halide perovskite light-emitting diodes (PeLEDs) face the critical challenge of field-dependent phase separation. Discrete colloidal CsPbX<sub>3</sub> nanocrystals anchored with ligands are promising to suppress phase separation, yet it remains a mystery how ion migration proceeds when integrated into LEDs as emissive films. Specifically, the influence of ion migration inside a single nanocrystal or across the nanocrystals along the electric field on the performance of PeLEDs needs to be decoupled. Here, a low-temperature-assisted transfer-printing method is developed to construct a model PeLED containing a clear CsPbBr<sub>3</sub>-CsPbI<sub>3</sub> nanocrystal film interface for tracing the ion migration between perovskite nanocrystal films along the direction of electric fields. The comprehensive study demonstrates that halogen ions crossing the nanocrystal film interface lead to severe phase separation and poor device stability, rather than the horizontal intra-layer diffusion. The monolayer CsPbX<sub>3</sub> nanocrystal film prevents the field-dependent phase separation caused by interlayer ion migration, significantly improving electroluminescent stability, including spectrum and lifetime. The optimized structure achieves a high external quantum efficiency of 26.9% and a remarkably improved operational half-lifetime of 61.2 h at an initial luminance of 100 cd m<sup>−2</sup> in pure-red PeLEDs based on mixed-halide CsPb(I<sub>x</sub>/Br<sub>1-x</sub>)<sub>3</sub>, more than 300 times longer than the control device using multilayer nanocrystals.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"82 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177367","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}
Nicole C. Mitchell, Oliver O. Thomas, Benjamin G. Meyer, Mirian Garcia-Fernandez, Ke-Jin Zhou, Patrick S. Grant, Peter G. Bruce, Richard Heap, Ruth Sayers, Robert A. House
{"title":"Influence of Ion Size on Structure and Redox Chemistry in Na-Rich and Li-Rich Disordered Rocksalt Battery Cathodes","authors":"Nicole C. Mitchell, Oliver O. Thomas, Benjamin G. Meyer, Mirian Garcia-Fernandez, Ke-Jin Zhou, Patrick S. Grant, Peter G. Bruce, Richard Heap, Ruth Sayers, Robert A. House","doi":"10.1002/adma.202419878","DOIUrl":"https://doi.org/10.1002/adma.202419878","url":null,"abstract":"Li-rich disordered rocksalts are promising next-generation cathode materials for Li-ion batteries. Recent reports have shown it is also possible to obtain Na-rich disordered rocksalts, however, it is currently poorly understood how the knowledge of the structural and redox chemistry translates from the Li-rich to the Na-rich analogs. Here, the properties of Li<sub>2</sub>MnO<sub>2</sub>F and Na<sub>2</sub>MnO<sub>2</sub>F are compared, which have different ion sizes (Li<sup>+</sup> = 0.76 vs Na<sup>+</sup> = 1.02 Å) but the same disordered rocksalt structure and stoichiometry. It is found that Na<sub>2</sub>MnO<sub>2</sub>F exhibits lower voltage Mn- and O-redox couples, opening access to a wider compositional range within the same voltage limits. Furthermore, the intercalation mechanism switches from predominantly single-phase solid solution behavior in Li<sub>2</sub>MnO<sub>2</sub>F to a two-phase transition in Na<sub>2</sub>MnO<sub>2</sub>F, accompanied by a greater decrease in the average Mn─O/F bond length. Li<sub>2</sub>MnO<sub>2</sub>F retains its long-range disordered rocksalt structure throughout the first cycle. In contrast, Na<sub>2</sub>MnO<sub>2</sub>F becomes completely amorphous during charge and develops a local structure characteristic of a post-spinel. This amorphization is partially reversible on discharge. The results show how the ion intercalation behavior of disordered rocksalts differs dramatically when changing from Li- to Na-ions and offers routes to control the electrochemical properties of these high-energy-density cathodes.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"9 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177162","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}
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