Nature MaterialsPub Date : 2025-10-15DOI: 10.1038/s41563-025-02374-9
Vikalp Raj,Yixian Wang,Min Feng,Kaustubh G Naik,Manish Jain,Bairav S Vishnugopi,Shimao Deng,Noah B Schorr,Martin Salazar,Alexander M Heusser,Xiaojing Huang,Andrew Scott Manning,Sergiy Kalnaus,Yijin Liu,John Watt,Josefine D McBrayer,Brad L Boyce,Hong Fang,Puru Jena,Partha P Mukherjee,Yue Qi,David Mitlin
{"title":"Grain boundary zirconia-modified garnet solid-state electrolyte.","authors":"Vikalp Raj,Yixian Wang,Min Feng,Kaustubh G Naik,Manish Jain,Bairav S Vishnugopi,Shimao Deng,Noah B Schorr,Martin Salazar,Alexander M Heusser,Xiaojing Huang,Andrew Scott Manning,Sergiy Kalnaus,Yijin Liu,John Watt,Josefine D McBrayer,Brad L Boyce,Hong Fang,Puru Jena,Partha P Mukherjee,Yue Qi,David Mitlin","doi":"10.1038/s41563-025-02374-9","DOIUrl":"https://doi.org/10.1038/s41563-025-02374-9","url":null,"abstract":"We report a method for promoting electrochemical stability in garnet Li6.4La3Zr1.4Ta0.6O12 solid-state electrolyte based on a composite two-phase oxide-oxide microstructure. Grain boundary precipitation of the controlled distribution of amorphous zirconium oxide microparticles is achieved through the addition of reactive tantalum carbide. During ambient-atmosphere sintering, the carbide decomposes through an in situ reaction, the 'extra' Ta substituting for Zr within the Li6.4La3Zr1.4Ta0.6O12 lattice. Density functional theory (DFT) calculations identify a thermodynamically favourable reaction path and show how substituting Ta5+ at Zr4+ sites affects the crystal structure as well as bulk ionic and electronic conductivities. Quantitative stereology highlights that zirconia also acts as a sintering aid, reducing compact porosity. Cryogenic focused-ion-beam scanning electron microscopy and fractography analysis of cycled solid-state electrolytes illustrates that near-universally observed intergranular Li-metal dendrite propagation is suppressed by the two-phase microstructure, favouring transgranular dendrites instead. Importantly, DFT demonstrates that compared with the Li6.4La3Zr1.4Ta0.6O12 surface, the zirconium oxide surface per se is less electronically conductive and does not trap excess electrons to reduce Li ions. This is a key reason for the substantial improvement in the electrochemical properties over the single-phase baseline.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":"26 1","pages":""},"PeriodicalIF":41.2,"publicationDate":"2025-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145296177","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}
Nature MaterialsPub Date : 2025-10-15DOI: 10.1038/s41563-025-02356-x
Hari Ramachandran, Edward W Mu, Eder G Lomeli, Augustin Braun, Masato Goto, Kuan H Hsu, Jue Liu, Zhelong Jiang, Kipil Lim, Grace M Busse, Brian Moritz, Joshua J Kas, John Vinson, John J Rehr, Jungjin Park, Iwnetim I Abate, Yuichi Shimakawa, Edward I Solomon, Wanli Yang, William E Gent, Thomas P Devereaux, William C Chueh
{"title":"A formal Fe<sup>III/V</sup> redox couple in an intercalation electrode.","authors":"Hari Ramachandran, Edward W Mu, Eder G Lomeli, Augustin Braun, Masato Goto, Kuan H Hsu, Jue Liu, Zhelong Jiang, Kipil Lim, Grace M Busse, Brian Moritz, Joshua J Kas, John Vinson, John J Rehr, Jungjin Park, Iwnetim I Abate, Yuichi Shimakawa, Edward I Solomon, Wanli Yang, William E Gent, Thomas P Devereaux, William C Chueh","doi":"10.1038/s41563-025-02356-x","DOIUrl":"https://doi.org/10.1038/s41563-025-02356-x","url":null,"abstract":"<p><p>Iron redox cycling between low-valent oxidation states of Fe<sup>II</sup> and Fe<sup>III</sup> drives crucial processes in nature. The Fe<sup>II/III</sup> redox couple charge compensates the cycling of lithium iron phosphate, a positive electrode (cathode) for lithium-ion batteries. High-valent iron redox couples, involving formal oxidation higher than Fe<sup>III</sup>, could deliver higher electrochemical potentials and energy densities. However, because of the instability of high-valent Fe electrodes, they have proven difficult to probe and exploit in intercalation systems. Here we report and characterize a formal Fe<sup>III/V</sup> redox couple by revisiting the charge compensation mechanism of (de)lithiation in Li<sub>4</sub>FeSbO<sub>6</sub>. Valence-sensitive experimental and computational core-level spectroscopy reveal a direct transition from Fe<sup>III</sup> (3d<sup>5</sup>) to a negative-charge-transfer Fe<sup>V</sup> (3d<sup>5</sup>L<sup>2</sup>) ground state on delithiation, without forming Fe<sup>IV</sup>, or oxygen dimers. We identify that the cation ordering in Li<sub>4</sub>FeSbO<sub>6</sub> drives a templated phase transition to stabilize the unique Fe<sup>V</sup> species and demonstrate that disrupting cation ordering suppresses the Fe<sup>III/V</sup> redox couple. Exhibiting resistance to calendar aging, high operating potential and low voltage hysteresis, the Fe<sup>III/V</sup> redox couple in Li<sub>4</sub>FeSbO<sub>6</sub> provides a framework for developing sustainable, Fe-based intercalation cathodes for high-voltage applications.</p>","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":" ","pages":""},"PeriodicalIF":38.5,"publicationDate":"2025-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145302307","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":"Rapid synthesis of subnanoscale high-entropy alloys with ultrahigh durability.","authors":"Chao Zhang,Zhongliao Wang,Chang Liu,Yu Bai,Changhao Liang,Jingxiang Low,Yujie Xiong","doi":"10.1038/s41563-025-02358-9","DOIUrl":"https://doi.org/10.1038/s41563-025-02358-9","url":null,"abstract":"Subnanoscale (<2 nm) high-entropy alloys (SHEAs) have garnered increasing attention for their unique physicochemical properties that enable high catalytic performance. However, this potential is offset by reduced stability, a characteristic typically associated with high-entropy alloys, due to their high reactivity at this scale. Here we circumvent this obstacle by using the localized surface plasmon resonance effect along with laser fragmentation in liquids for synthesizing SHEAs. Localized-surface-plasmon-resonance-generated hot electrons from gold nanoparticles facilitate metal ion reduction, whereas the 7-ns laser pulse induces ultrafast heating and cooling cycles, fusing multiple metals into SHEAs with enhanced stability. This method enables the incorporation of up to ten elements into SHEAs. The selected AuPtRuRhIr SHEAs demonstrate high stability to work under 2 A cm-2 at 2.12 V for over 1,200 h in a proton exchange membrane electrolyser. This work presents a general strategy for the preparation of SHEAs, applicable across a wide range of fields.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":"25 1","pages":""},"PeriodicalIF":41.2,"publicationDate":"2025-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145296179","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}
Nature MaterialsPub Date : 2025-10-15DOI: 10.1038/s41563-025-02383-8
Namit Chaudhary,Kathryn A Whitehead
{"title":"Designing around immune memory to counter PEG immunogenicity.","authors":"Namit Chaudhary,Kathryn A Whitehead","doi":"10.1038/s41563-025-02383-8","DOIUrl":"https://doi.org/10.1038/s41563-025-02383-8","url":null,"abstract":"","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":"28 1","pages":""},"PeriodicalIF":41.2,"publicationDate":"2025-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145296180","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}
Nature MaterialsPub Date : 2025-10-13DOI: 10.1038/s41563-025-02379-4
Maurizio Monti,Khalid M Siddiqui,Daniel Perez-Salinas,Naman Agarwal,Martin Bremholm,Xiang Li,Dharmalingam Prabhakaran,Xin Liu,Danylo Babich,Mathias Sander,Yunpei Deng,Henrik T Lemke,Roman Mankowsky,Xuerong Liu,Simon E Wall
{"title":"Ultrafast surface melting of orbital order in La0.5Sr1.5MnO4.","authors":"Maurizio Monti,Khalid M Siddiqui,Daniel Perez-Salinas,Naman Agarwal,Martin Bremholm,Xiang Li,Dharmalingam Prabhakaran,Xin Liu,Danylo Babich,Mathias Sander,Yunpei Deng,Henrik T Lemke,Roman Mankowsky,Xuerong Liu,Simon E Wall","doi":"10.1038/s41563-025-02379-4","DOIUrl":"https://doi.org/10.1038/s41563-025-02379-4","url":null,"abstract":"Understanding how light modifies long-range order in quantum materials is key to improving our ability to control functionality. However, this is challenging if the response is heterogeneous. Here we address the most common form of light-induced heterogeneity-surface melting-and measure the dynamics of orbital order in the layered manganite La0.5Sr1.5MnO4. We isolate the surface dynamics from the bulk by measuring the orbital truncation rod and orbital Bragg peak. After photoexcitation, the orbital Bragg peak shows an unusual narrowing, which suggests an increase in correlation length of the probed volume. By contrast, the correlation length at the surface decreases. These differences can be reconciled if the material is heterogeneous, and light melts a less ordered surface. By isolating the surface response, we determine that the loss of long-range order is an incoherent process, which is probably accompanied by the formation of local polarons.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":"1 1","pages":""},"PeriodicalIF":41.2,"publicationDate":"2025-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145283996","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":"Near-100% spontaneous rolling up of polar van der Waals materials.","authors":"Zhi Zhang,Yuwei Zhang,Kangjun Lu,Jun-Jie Zhang,Nannan Zhang,Rui Feng,Haoran Ye,Xiaoli Zhou,Linglong Li,Dongyang Wan,Junpeng Lu,Zhenhua Ni,Jinlan Wang,Qian Chen,Jiong Lu,Zejun Li","doi":"10.1038/s41563-025-02357-w","DOIUrl":"https://doi.org/10.1038/s41563-025-02357-w","url":null,"abstract":"Rolling two-dimensional materials into one-dimensional nanoscrolls introduces curvature, chirality and symmetry breaking, enabling emergent properties. Conventional methods relying on external driving forces, however, exhibit poor control, low yield and limited reproducibility. Here we report spontaneous scrolling in polar van der Waals materials via an electrochemical intercalation/exfoliation process, enabling scalable nanoscroll production. This self-rolling is driven intrinsically by out-of-plane electric polarization (P⊥), where the magnitude of P⊥ is modulated by the intercalant size. Validated across eight polar materials, this approach achieves virtually 100% yield and reproducibility with defined scrolling direction, surpassing external driving force limitations. The nanoscrolls exhibit layer-independent inversion symmetry breaking and coherently enhanced second-harmonic generation, exceeding two-dimensional flakes by ~100-fold and rivalling leading two-dimensional nonlinear materials. Electrochemical initiation further facilitates metal-ion co-intercalation, yielding ten hybrid nanoscroll architectures. These findings establish a scalable route to create one-dimensional nanostructures and hybrid heterostructures, paving the way for designer quantum solids and van der Waals superlattices in quantum nanodevices.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":"41 1","pages":""},"PeriodicalIF":41.2,"publicationDate":"2025-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145283995","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":"Reprogrammable snapping morphogenesis in ribbon-cluster meta-units using stored elastic energy.","authors":"Yaoye Hong,Caizhi Zhou,Haitao Qing,Yinding Chi,Jie Yin","doi":"10.1038/s41563-025-02370-z","DOIUrl":"https://doi.org/10.1038/s41563-025-02370-z","url":null,"abstract":"Snapping, driven by stored elastic energy, enables versatile and rapid shape changes in nature; yet replicating such autonomous, reprogrammable morphogenesis in free-standing volumetric structures remains elusive. Here we report a lantern-shaped ribbon-cluster meta-unit that harnesses programmable and reprogrammable elastic energy to achieve over 13 distinct volumetric snapping morphologies from a single unit. Governed by three Euler angles, the meta-unit post-fabrication offers a tunable mechanical design space spanning up to quadrastable states. Unlike single-ribbon or mechanism-based designs, our system autonomously selects snapping pathways via nastic coupling between multiple ribbons, enabling the inverse design of complex snapping morphologies. We harness magnetically actuated bud-to-bloom and tristable morphogenesis to enable fast, non-invasive grasping and remote flow regulation in confined environments. These results establish a general framework for architected materials with programmable shape, stability and function, offering potential applications in soft robotics, deployable devices and mechanical logic.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":"2 1","pages":""},"PeriodicalIF":41.2,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145261084","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}
Nature MaterialsPub Date : 2025-10-10DOI: 10.1038/s41563-025-02371-y
Michael D Dickey
{"title":"Using light to print metal oxides.","authors":"Michael D Dickey","doi":"10.1038/s41563-025-02371-y","DOIUrl":"https://doi.org/10.1038/s41563-025-02371-y","url":null,"abstract":"","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":"11 1","pages":""},"PeriodicalIF":41.2,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145261088","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}