{"title":"Hydrogen-Deficient Chain-Like Molecular Structure Confined Hydride Electrolyte for High-Voltage All-Solid-State Lithium Metal Batteries.","authors":"Panyu Gao,Shunlong Ju,Tian Xu,Wubin Du,Yong Gao,Yaxiong Yang,Zhenglong Li,Hongyu Zhang,Yuqin Huang,Guanglin Xia,Fei Wang,Xuebin Yu","doi":"10.1002/adma.202508008","DOIUrl":"https://doi.org/10.1002/adma.202508008","url":null,"abstract":"The practical application of LiBH4 in all-solid-state Li metal batteries (ASSLMBs) is hindered by low Li-ion conductivity at room temperature, poor oxidative stability, and severe dendrite growth. Herein, porous [LiNBH]n with a hydrogen-deficient chain-like molecular structure are designed for in situ space-confining LiBH4, which enables strong attraction of negatively charged Hδ- atoms of [BH4]- anions by Li+ of [LiNBH]n chains that weakens Coulombic interaction between Li+ and [BH4]- anions and hence promotes Li ion diffusion. Additionally, the electron-withdrawing effect of [LiNBH]n chains induces the local electron localization of LiBH4 that enhances oxidative stability of LiBH4. Therefore, the Li ion conductivity of LiBH4 reaches 2.2 × 10-4 S cm-1 at 30 °C, nearly 4 orders of magnitude higher than that of LiBH4, with a voltage window of 5 V. Moreover, the interaction between Li metal and [LiNBH]n chains results in in situ formation of ultrathin layer composed of Li3N and LiB alloys that hinders Li dendrites growth, leading to a critical current density value of 7.5 mA cm-2 and a cycling life of 100 h at 4 mA cm-2 with an overpotential of 125 mV. Hence, LiCoO2|LiBH4-70LiNBH|Li cell at 0.5 C deliver a high capacity of 89.5 mA h g-1 after 400 cycles.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"11 1","pages":"e08008"},"PeriodicalIF":29.4,"publicationDate":"2025-07-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144669564","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-Dielectric-Layer-Based Iontronic Pressure Sensor Coupling Ultrahigh Sensitivity and Wide-Range Detection for Temperature/Pressure Dual-Mode Sensing.","authors":"Jianyu Pu,Yuantao Zhang,Huiming Ning,Yuanhao Tian,Chenxing Xiang,Hui Zhao,Yafeng Liu,Alamusi Lee,Xinglong Gong,Ning Hu,Tonghua Zhang,Shu Wang","doi":"10.1002/adma.202503926","DOIUrl":"https://doi.org/10.1002/adma.202503926","url":null,"abstract":"Iontronic pressure sensors are widely used in human motion monitoring and human-machine interactions owing to their high sensitivity, wide measurement range, and excellent resolution. However, conventional dielectric layer designs often involve complex fabrication processes, high costs, and limited performances. This paper proposes a novel sensor structure, the dual-dielectric-layer iontronic pressure sensor (DLIPS), which integrates high- and low-permittivity layers. Validated using silkworm cocoon ion gel and open-cell polyurethane foam as dielectrics, the DLIPS exhibited ultrahigh sensitivity (72548.7 kPa-1), a wide working pressure range (0.001-420 kPa), an exceptionally low detection limit (0.832 Pa), and remarkable durability exceeding 5000 cycles. By leveraging the distinct responses of the capacitance and resistance to pressure and temperature, the sensor can simultaneously measure both parameters. A deep learning regression model is integrated to decouple the mixed temperature and pressure signals, enabling accurate identification. Owing to its ultrahigh sensitivity and capability to detect minute pressure fluctuations, the DLIPS exhibited strong potential for skin-mounted silent speech recognition systems, achieving a recognition accuracy of up to 98.5%. Furthermore, the DLIPS provides a cost-effective and scalable approach for fabricating ultrahigh-sensitivity pressure sensors, underscoring its versatility in wearable technology applications.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"26 1","pages":"e03926"},"PeriodicalIF":29.4,"publicationDate":"2025-07-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144669588","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}
Rachel R Chan,Kaitlin M Landy,Kyle J Gibson,Sachin P Kulkarni,Junjing Deng,Byeongdu Lee,Joseph McCourt,Soenke Seifert,Olivier J G L Chevalier,Alexa M Wong,Chaojian Chen,Peter H Winegar,Koray Aydin,Chad A Mirkin
{"title":"Programming Defects and Cavities into Colloidal Crystals Engineered With DNA.","authors":"Rachel R Chan,Kaitlin M Landy,Kyle J Gibson,Sachin P Kulkarni,Junjing Deng,Byeongdu Lee,Joseph McCourt,Soenke Seifert,Olivier J G L Chevalier,Alexa M Wong,Chaojian Chen,Peter H Winegar,Koray Aydin,Chad A Mirkin","doi":"10.1002/adma.202503522","DOIUrl":"https://doi.org/10.1002/adma.202503522","url":null,"abstract":"Taking inspiration from seed-mediated crystal growth in atomic and molecular systems, a strategy is developed for incorporating particle and volume defects into the interior of colloidal crystals consisting of programmable atom equivalents (PAEs, oligonucleotide-functionalized nanoparticles) assembled with DNA. Discrete PAEs spanning a range of shapes, sizes, and compositions serve as nucleation sites for seed-mediated colloidal crystal growth and are incorporated into the centers of colloidal crystal lattices as cavities. Importantly, seed PAE shapes or sizes that are geometrically mismatched with the colloidal crystal lattice symmetry introduce defects such as local lattice disorder and long-range grain boundaries that arise through geometric frustration. Colloidal crystals synthesized with plasmonic seed particles exhibit near-infrared (NIR) wavelength scattering cross-sections that are highly dependent upon cavity/particle size and shape. Taken together, these findings establish a platform for the deliberate introduction of 2 and 3D defects into colloidal crystals, which may inform the design of structures and materials for thermal management, sensing, and catalysis.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"14 1","pages":"e03522"},"PeriodicalIF":29.4,"publicationDate":"2025-07-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144669562","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":"Topological Transformation of MXenes to Non-Van Der Waals Artificial Solids with Well-Defined Structure.","authors":"Yu Guo,Shihao Wu,Zhihui Liu,Zhiguo Du,Shubin Yang","doi":"10.1002/adma.202507705","DOIUrl":"https://doi.org/10.1002/adma.202507705","url":null,"abstract":"Two-dimensional (2D) transition metal carbides, nitrides, or carbonitrides (MXenes) have become an ideal platform to produce some derivatives with tunable chemical compositions and structures, possessing unique physical and chemical properties beyond their counterparts. Here, a well-defined non-van der Waals artificial solid is developed on the basis of the topological transformation of Cl-terminated MXenes, which involves the substitution of -Cl with -S terminations to enlarge the interlayer spacing of MXenes and subsequent configuration with transition-metal (Cu, Fe, Co, Ni, and Sn) atoms. After the topological transformation, the MXene layers are chemically bonded, showing a higher thermal stability up to 550 °C in air than that of MXenes. The resultant artificial solids with well-defined atomic metal layers exhibit a high electrocatalytic activity to I2/I- redox reaction and a strong adsorption capability toward iodine species. As a result, Zn-I2 batteries deliver a good rate performance of 104 mAh g-1 at 32 C and a long cycling stability of up to 2000 cycles at 8 C.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"5 1","pages":"e07705"},"PeriodicalIF":29.4,"publicationDate":"2025-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144652786","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":"Achieving Ultrafast Monovalent ZnCl+ Ion Transport in MOF-Based Zn Ion Solid-State Electrolyte through Polyanion Strategy.","authors":"Xiaoyun Xu,Songmei Li,Rongrong Guo,Chuangchuang Zhang,Jia Zhou,Mei Yu,Juan Du,Jinyan Zhong,Shubin Yang,Bin Li","doi":"10.1002/adma.202508925","DOIUrl":"https://doi.org/10.1002/adma.202508925","url":null,"abstract":"Solid-state transport of high-valence ions is a huge challenge, such as the transport of divalent zinc ions. Herein, a polyanion strategy is proposed to decrease divalent Zn2+ to monovalent ZnCl+, realizing ultrafast ion transport in solid-state electrolyte. An amorphous metal-organic framework (ZGB-MOF) is designed and constructed as the matrix for solid-state electrolyte. The ZGB-MOF matrix is obtained by the Zn2+/Ga3+ competitive coordination process, enriching O-Ga-Cl polyanion clusters, nanopores and C═O/oxygen vacancies active sites. The polyanion property of Ga3+ and physical limiting domains of nanopores promote the formation of ZnCl+. Abundant C═O and oxygen vacancies provide more transport sites, decreasing transport energy barriers for ZnCl+ (only 0.12 eV). Eventually, the obtained Zinc ion solid-state electrolyte (ZGBC) achieves high ionic conductivity of 5.2 × 10-3 S cm-1 and high transference number of 0.873. More importantly, the ZGBC electrolyte exhibits wide electrochemical window (up to 2.88 V) and high charging voltage (2.4 V), and achieves dendrite-free deposition of Zn-metal and stabilization of cathode materials. Full cells with ZGBC electrolyte and zinc hexacyanoferrate cathode exhibit excellent cycling stability, with no capacity degradation after 5000 cycles. This discovery could trigger new waves of enthusiasm for exploring new ion transport mechanisms beyond divalent Zn2+ transport.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"2 1","pages":"e08925"},"PeriodicalIF":29.4,"publicationDate":"2025-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144652787","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":"Synchronous Phase Transformation for Efficient Wide-Bandgap Perovskite Photovoltaics.","authors":"Yifan Li,Xinmin Zhao,Ni Meng,Shuo Dong,Shan Yan,Man Yang,Changjiu Sun,Zhiqiang Li,Shaopeng Yang,Mingjian Yuan,Tingwei He","doi":"10.1002/adma.202505694","DOIUrl":"https://doi.org/10.1002/adma.202505694","url":null,"abstract":"Mixed-halogen wide-bandgap (WBG) perovskite materials are employed in tandem solar cells (TSCs) due to their continuous tunability of bandgap. However, inhomogeneous halogen phases are often observed in bromine-rich perovskite films, which restricts the performance of WBG perovskite solar cells (PSCs) and TSCs. Here, homogeneous halogen-phase perovskite is proposed to form film by a synchronous halogen-phase transformation strategy. 1,3-Dimethyl-2-imidazolidinone (DMI) is introduced into the perovskite precursor solution, due to its stronger binding energy with lead halide (PbX2). The homogeneous DMI-PbX2 adducted intermediate phase is stable in precursor solution and at spin-coating stage. And it then synchronously transforms into a homogeneous halide-phase perovskite film at the annealing stage. Benefited from efficient carrier extraction and suppressed carrier recombination, the resulting 1.76 eV-bandgap PSC achieves a record power conversion efficiency (PCE) of 21.42% (certified 21.18%) among devices with a bandgap wider than 1.74 eV. Based on the high transmittance of semitransparent-WBG PSC, a 4-terminal all-perovskite TSC achieves a PCE of 29.66%.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"18 1","pages":"e05694"},"PeriodicalIF":29.4,"publicationDate":"2025-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144652824","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}
Lingbo Yao,Lvzhang Jiang,Yichao Wang,Xiaowei Chi,Yu Liu
{"title":"A 1000 Wh Kg-1 Cathode Facilitated by In Situ Mineralized Electrolyte with Electron Potential Well for High-Energy Aqueous Zinc Batteries.","authors":"Lingbo Yao,Lvzhang Jiang,Yichao Wang,Xiaowei Chi,Yu Liu","doi":"10.1002/adma.202505342","DOIUrl":"https://doi.org/10.1002/adma.202505342","url":null,"abstract":"The practical applications of aqueous zinc-ion batteries (AZMBs) are hindered by challenges such as low energy density and limited cycle life, which stem from the one-electron transfer at the cathode and dendrite formation at the anode. Herein, inspired by the biomineralization phenomenon in nature, an in situ mineralized electrolyte (IME) containing Prussian blue analogs (PBAs) as an electron potential well is designed. This in situ mineralization strategy promotes uniform, rapid, and reversible charge transfer at the electrode/electrolyte interfaces, enabling the Iodine (I₂) cathode to achieve a specific capacity of 286.4 mAh g⁻¹ at 1 A g⁻¹ and an energy density of 330.8 Wh kg⁻¹. Simultaneously, the potential well facilitates the in situ recovery of Zn dendrites into active Zn2⁺ ions, ensuring stable Zn anode cycling with a practical areal capacity of 5 mAh cm⁻2 for 1500 h. Furthermore, the mediation of iodine-bromine chemistry enables highly reversible Br⁰/Br⁻ and I⁺/I⁰/I⁻ reactions, achieving an energy density of more than 1000 Wh kg-1. Additionally, an enhanced energy density of 503 Wh kg⁻1 and a high energy efficiency of 86.73% over 6000 cycles are achieved. In summary, the in situ mineralization of an electron potential well in electrolyte offers a novel pathway for developing high-energy and long-lifespan AZMBs.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"49 1","pages":"e05342"},"PeriodicalIF":29.4,"publicationDate":"2025-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144652825","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":"Biohybrid Microrobot Enteric-Coated Microcapsule for Oral Treatment of Colorectal Cancer.","authors":"Yong Kang,Yaoguang She,Yang Zang,Mengyu Yuan,Gaoli Niu,Xinghua Tian,Lei Zhang,Jingjing Lin,Mengxiang Yang,Zhengcun Pei,Ximo Wang,Xiaoyuan Ji","doi":"10.1002/adma.202420586","DOIUrl":"https://doi.org/10.1002/adma.202420586","url":null,"abstract":"The oral treatment of colorectal cancer is highly desirable due to its noninvasiveness and potential for localized drug action, yet it remains challenged by gastrointestinal barriers and limited intratumoral penetration. This study presents the first oral biohybrid microrobot system that integrates ultrasound-activated piezoelectric catalysis with bacterial therapy, achieving synergistic tumor targeting, reactive oxygen species generation, and immune activation. By leveraging Enterobacter aerogenes (EA) and BaTiO3 nanoparticles, this strategy induces immunogenic tumor cell death and metabolic remodeling. It utilizes BaTiO3 incorporated into EA (EA@BTO) microrobots, which are encapsulated in enteric microcapsules. These microcapsules, encapsulated in enteric microcapsules via photocurable 3D printing, protect during digestion, target tumors, penetrate mucus, and release gases. They thrive in anaerobic, acidic environments, enabling precise, responsive delivery within the intestinal tract. Once the microrobots reach the tumor, the BaTiO3 nanoparticles catalyze reduction and oxidation reactions upon ultrasound irradiation, leading to the induction of immunogenic tumor cell death. Notably, the consumption of lactic acid by BaTiO3 and EA alleviates the immunosuppressive microenvironment within the tumor. This promotes the maturation of dendritic cells and the polarization of macrophages toward the M1 phenotype, thereby reducing the proportion of regulatory T cells and enhancing the population of effector T cells.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"3 1","pages":"e20586"},"PeriodicalIF":29.4,"publicationDate":"2025-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144652823","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":"Giant Flexoelectric-Like Response via Macroscopic Symmetry Design.","authors":"Yongkang Zhang,Zhaonan Yan,Shuhai Liu,Yong Qin","doi":"10.1002/adma.202501160","DOIUrl":"https://doi.org/10.1002/adma.202501160","url":null,"abstract":"Flexoelectricity is enabled by symmetry in all materials. However, flexoelectric material application is limited by the normally low charge density produced in bulk materials. In this study, a universal strategy involving a macroscopic symmetry design is proposed to enhance the flexoelectricity. Through theoretical derivation, flexoelectricity can be improved by designing the macroscopic symmetry of the material parameter distribution (including the piezoelectric coefficients) and device structure. As a demonstration, typical piezoelectric bimorph cantilevers (PBCs; Ag/PZT-5H/Ag/PZT-5H/Ag) are constructed with the two PZT-5H layers arranged in \"head-to-tail\" polarization (mirror symmetry) and \"tail-to-tail\" polarization (centrosymmetry), to design the macroscopic symmetry and thus to tune the flexoelectricity. The theoretical predictions and experimental results show that the tail-to-tail PBC achieves a flexoelectric coefficient (1.47 × 106 nC m-1), 20 times higher than that of the head-to-tail PBC (7 × 104 nC m-1) and conventional piezoelectric cantilevers (Ag/PZT-5H/Ag). Furthermore, by introducing spaced-interdigitated electrodes, the macroscopic symmetry of the head-to-tail PBC can be transformed from mirror to centrosymmetry, yielding a giant flexoelectric coefficient of 2.53 × 106 nC m-1. This strategy offers a dimension beyond traditional approaches for understanding and enhancing flexoelectricity, paving the way for its practical application.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"30 1","pages":"e01160"},"PeriodicalIF":29.4,"publicationDate":"2025-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144652788","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":"Anisotropic Excitation-Modulated Multi-Color Three-photon Excited Luminescence in Ln-MOF Heterostructure.","authors":"Hongjun Li,Yujie Cai,Lin Zhang,Enlai Hu,Jiaojiao Yang,Hai Guo,Yuanjing Cui,Banglin Chen,Guodong Qian","doi":"10.1002/adma.202509590","DOIUrl":"https://doi.org/10.1002/adma.202509590","url":null,"abstract":"Multi-photon excited luminescence (MPEL) modulation is of great application value for optoelectronics, especially MPEL with the characteristics of multi-color emission and optical anisotropy. However, it still suffers from the obstacles in highly-integrating and orientedly-assembly of various MPEL units. Herein, a hierarchical assembly-in situ doping strategy is proposed to establish a novel lanthanide-graded metal-organic framework based heterostructure. Well-designed ligand and Ln3+ ions are respectively selected as the MPEL energy donor and acceptor units (MEDU and MEAU). Through utilizing the effective energy transfer between them, the as-obtained triblock heterostructure displays multi-dimensional three-photon excited luminescence (3PEL) modulation, where the emission band and intensity can be switched by manipulating excited regions and excitation polarization based on a single pump source. This is attributed to the precise integration and orientation of photonic units. As a result, the heterostructure exhibits multi-color 3PEL with a record-high MPEL color gamut (>30% of sRGB area) in MOFs and high degree of linear polarization values (max ≈88.6%). Such anisotropic 3PEL modulation shows promising potential in nonlinear optical switches, programmable logic gates, and multi-level optical barcodes. These findings open up an intriguing way to develop up-conversion luminescent materials with functions on demand toward photonic modulation.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"15 1","pages":"e09590"},"PeriodicalIF":29.4,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144652867","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}