Advanced Materials最新文献

{"title":"Embedded Fe-Cu Pairs Enable Tandem Nitrate-to-Ammonia Electroreduction","authors":"Yuxiao Liu, Xia Zhang, Solmaz Feizpoor, Hsiao-Chien Chen, Linfeng Li, Yunpeng Zuo, Shengji Tian, Mengni Liu, Wenyu Hu, Muhammad Humayun, Kaifu Huo, Chade Lv, Yuanjie Pang, Dingsheng Wang, Xin Wang, Chundong Wang","doi":"10.1002/adma.202514840","DOIUrl":"https://doi.org/10.1002/adma.202514840","url":null,"abstract":"Electrochemical nitrate reduction (<i>e</i>-NO₃RR) to ammonia (NH₃) represents a transformative technology that seamlessly integrates environmental remediation with resource regeneration. This approach is crucial for restoring equilibrium in the global nitrogen cycling, advancing green chemistry, and accelerating the transition toward a sustainable circular economy. However, under pH-neutral conditions, the simultaneous occurrence of two competing reactions (Hydrogen Evolution Reaction and NO₃RR) at the same active sites results in considerable interference, significantly limiting the catalytic efficiency and selectivity. Here a Fe-Cu pair (Cu-N₃/Fe₃-N₈) electrocatalyst is meticulously designed, achieving a NH₃ production rate of 18.83 mg∙h^‒1∙mg_cat^‒1 at −0.65 V versus the reversible hydrogen electrode (RHE), accompanied with a Faradaic efficiency of 97.1%. This as-prepared Fe-Cu pair overcomes the limitations of conventional bimetallic catalysts, which typically rely on direct atomic coupling. The electron-deficient region formed by Cu–N₃ enhances the adsorption of nitrate, while the electron-rich domain generated by the Fe₃–N₈ cluster facilitates the adsorption of nitrite and promotes water activation. The spatially separated charge gradient optimizes the adsorption energies of multi-step reaction intermediates, thereby establishing a relay mechanism. The work provides valuable insights into the design of multi-active-site electrocatalysts and offers a promising approach to addressing critical challenges in nitrogen resource conversion.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"5 1","pages":"e14840"},"PeriodicalIF":29.4,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209744","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":"Al Pinning Effect in Birnessite for High-Performance Ammonium-Ion Storage","authors":"Chao Cheng, Shuyang Bian, Yurong You, Qiang Liu, Zhuoying Yang, Fei Ye, Wenshu Chen, Jun Cheng, Xuecheng Chen, Zilong Tang, Kongjun Zhu, Yuping Wu, Linfeng Hu","doi":"10.1002/adma.202512356","DOIUrl":"https://doi.org/10.1002/adma.202512356","url":null,"abstract":"Layered birnessite has attracted considerable attention for its cathode potential in various aqueous energy storage devices owing to its two-electron transfer reaction (Mn²⁺/Mn⁴⁺), open diffusion channels, and tunable interlayer spacings. However, birnessite for reversible ammonium (NH₄⁺) ion storage generally suffers from irreversible structural collapse originated from Jahn–Teller (J–T) effect of Mn³⁺ and the intrinsic slow ionic diffusion kinetics. Herein, an Al pinning effect in birnessite is found to address these two issues simultaneously, which promoted enhanced structural stability and resulted in fast ionic diffusion kinetics for excellent high-rate capability. Strikingly, a robust cycling stability over 5, 000 cycles at 1.0 A g⁻¹ is achieved in the optimal Na_0.7Al_0.1Mn_0.9O₂, which surpasses that of most previously reported ammonium-ion batteries. Density functional theory calculations revealed that the pinned [Al³⁺O₆] octahedra not only decrease the Mn³⁺ content in birnessite, but also strengthen the covalency of Mn─O bonds to resist the collinear elongation/compression direction of the [Mn³⁺O₆] octahedra. Furthermore, Al pinning in birnessite can increase the interlayer spacing due to the regulation of Mn³⁺─O/Mn⁴⁺─O bond length and decrease the diffusion barrier for NH₄⁺ ion in the interlayer of birnessite. Thus, an accelerated NH₄⁺ ion diffusion coefficient of 1.58 × 10⁻⁹ cm² s⁻¹ has been achieved, which is ≈5 times higher than of the pristine one and also higher than that in other cathode materials. The findings demonstrate that layered Na_0.7Al_0.1Mn_0.9O₂ is a very promising cathode candidate for NH₄⁺ ion battery, and the Al pinning effect in birnessite can effectively suppress the J–T effect and enhance the NH₄⁺ ion diffusion kinetics simultaneously.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"7 1","pages":"e12356"},"PeriodicalIF":29.4,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209766","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":"Metal-Insulator Transition Driven by the Interplay of Vacancies and Charge Orders in Square-Net Materials GdSbxTe2-x-δ.","authors":"Qun Wang,Yifang Jiang,Songyuan Geng,Hanpu Liang,Yunbo Wu,Risi Guo,Fangjie Chen,Kangjie Li,Xin Wang,Bin Cao,Keyu An,Shengtao Cui,Zhe Sun,Mao Ye,Zhengtai Liu,Changming Yue,Shiming Lei,Haoxiang Li","doi":"10.1002/adma.202510303","DOIUrl":"https://doi.org/10.1002/adma.202510303","url":null,"abstract":"Engineering narrow-bandgap semiconductors remains a pivotal challenge for next-generation electronic and energy devices. Charge density wave (CDW) systems offer a promising platform for bandgap engineering. However, most 2D and 3D CDW systems remain metallic despite exhibiting Fermi surface nesting. Here, a doping-dependent metal-insulator transition (MIT) with tunable bandgaps is reported in square-net materials GdSbxTe2-x-δ and a cooperative interaction between CDWs and vacancies that drives the MIT is discovered. Angle-resolved photoemission spectroscopy (ARPES) reveals the MIT in the low Sb-content regime of GdSbxTe2-x-δ, with a maximum energy gap of Δ ≈ 98 meV at x = 0.16, corroborated by electrical transport measurements. Following the MIT, X-ray diffraction reveals a doping-dependent shift of the CDW wavevector toward a commensurate structure with q = 0.25 a*, concurrent with the appearance of Te vacancies in the square-net layers. Density functional theory (DFT) calculations attribute the gap formation to the ordered Te vacancies modulated by the 4×1×1 CDW superstructure, which suppresses the electronic states near the Fermi level. Contrasting with the partial gap scenarios in conventional CDW systems, this synergy between the CDW and the vacancy stabilizes the insulating phase, offering a distinct avenue for narrow bandgap engineering in electronic materials.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"99 1","pages":"e10303"},"PeriodicalIF":29.4,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145194681","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":"Neuroimmune Microenvironment Reprogramming via Immuno-piezoelectric Transducers for Synergistic Stem Cell Therapy in Traumatic Brain Injury.","authors":"Linlin Liang,Xin Li,Kai Hu,Pingqiang Cai,Jianwu Wang,Jing Yu,Shasha Wang,Yuwei Zhao,Changgeng Xu,Siwei Li,Hong Liu,Changyong Wang,Jin Zhou","doi":"10.1002/adma.202512810","DOIUrl":"https://doi.org/10.1002/adma.202512810","url":null,"abstract":"Secondary traumatic brain injury (TBI) induces a pro-inflammatory microenvironment that hampers neural stem cells (NSCs) therapy and tissue regeneration. To address this challenge, an immuno-piezoelectric transducer have been developed to create an anti-inflammatory immune microenvironment, deliver wireless electrical stimulation, and facilitate multimodal NSCs therapy. The immuno-piezoelectric transducer drives the polarization of microglia towards the anti-inflammatory M2 phenotype and secretion of anti-inflammatory cytokines. This modulation significantly reduces the inflammatory response, creating an optimal microenvironment for NSCs survival. Furthermore, the wireless electrical stimulation generated by ultrasound facilitates NSCs differentiation into glutamatergic and GABAergic neurons, enhances neurite complexity, upregulates synaptic proteins expression and neural integration in injured regions. The multimodal therapy demonstrates superior outcomes in restoring structural integrity, improving functional, and enhancing behavioral action in TBI rat models. This study integrates piezoelectric with immunomodulation to reprogram the neuroimmune microenvironment, providing novel therapeutic paradigm for brain injury repair.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"93 1","pages":"e12810"},"PeriodicalIF":29.4,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145194683","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":"Quasi-Solid Cathode Additive Enables Highly Reversible Four-Electron I-/I0/I+ Conversion in Aqueous Zn-I2 Batteries.","authors":"Han Wu,Shao-Jian Zhang,Jitraporn Vongsvivut,Yunling Jiang,Junnan Hao,Shi-Zhang Qiao","doi":"10.1002/adma.202511680","DOIUrl":"https://doi.org/10.1002/adma.202511680","url":null,"abstract":"Aqueous zinc-iodine (Zn-I2) batteries with four-electron (4e) I-/I0/I+ conversion (4eZIBs) offer high energy density but face both-step I-/I0 and I0/I+ challenges, including the polyiodide shuttle effect, sluggish I0/I+ conversion kinetics, and severe I+ hydrolysis. To mitigate these issues, a quasi-solid additive composed of 1-butyl-3-methylimidazolium chloride (BMICl) and carbon nanotubes (CNTs) is introduced into the cathode. Specifically, by co-grinding BMICl with CNTs, a homogeneous quasi-solid additive is formed due to the π-π stacking interactions between CNTs and imidazole rings. This additive not only suppresses the shuttle effect by binding with polyiodides in the first-step I-/I0 conversion, but also enhances I+ conversion kinetics by immobilizing Cl- inside the electrode and curbs I+ hydrolysis through forming a BMI-ICl2 complex in the second-step conversion. This innovative approach enables the 4eZIBs to achieve a near-theoretical specific capacity of 418.9 mA h g-1 at 0.5C, while maintaining a robust lifespan of over 600 cycles with a capacity retention of 93.4% at 1C. Moreover, pouch cells under a high areal capacity of 7.1 mA h cm-2 for each side of the cathode demonstrate a high-capacity retention of 95.8% after 150 cycles at 6.3 mA cm-2 (≈0.5C).","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"23 1","pages":"e11680"},"PeriodicalIF":29.4,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145194680","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":"Hydrogel-Based ROS-Regulating Strategy: Reprogramming the Oxidative Stress Imbalance in Advanced Diabetic Wound Repair.","authors":"Qiaoling Zhou,Yu Zhuang,Xiaoling Deng,Weidong Jiang,Xudong Wang,Changyong Yuan,Kaili Lin","doi":"10.1002/adma.202512719","DOIUrl":"https://doi.org/10.1002/adma.202512719","url":null,"abstract":"Due to hyperglycemia and redox imbalance, diabetic wounds are prone to recurrent ulceration and non-healing, severely affecting patients' quality of life. Excessive reactive oxygen species (ROS) in wounds impede repair by damaging proteins and nucleic acids, activating inflammation, and suppressing immunity. A growing body of evidence suggests that harnessing the high oxidative stress within the microenvironment and modulating ROS levels to overcome repair barriers has become a breakthrough in treating chronic diabetic wounds. Hydrogels, with excellent biocompatibility and designability, are key for intelligent ROS regulation. Here, the role of ROS in the progression of diabetic skin wounds is detailed, which includes inducing oxidative damage, exacerbating inflammation and immune imbalance, as well as degrading the extracellular matrix (ECM), hindering neovascularization, and inhibiting nerve repair. Then, the ROS-regulating strategy based on the hydrogel platform is discussed. Engineered hydrogels adjust ROS levels via external stimulus such as light, ultrasound, and electricity, or the microenvironment of hyperglycemia, oxidative stress, and acidity in wounds, and even bidirectionally in specific spatiotemporal contexts. Furthermore, the therapeutic and repair potential of ROS-regulated hydrogels in the healing process of diabetic wounds is outlined, the current deficiencies in the field of diabetic wounds treatment are addressed, and prospects for the future are proposed.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"26 1","pages":"e12719"},"PeriodicalIF":29.4,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145194628","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":"Correction to \"Directionally Modulated Zinc Deposition by a Robust Zincophilic Cu-Phthalocyanine Protective Layer in Dendrite-Free Aqueous Zinc Ion Batteries\".","authors":"","doi":"10.1002/adma.202518638","DOIUrl":"https://doi.org/10.1002/adma.202518638","url":null,"abstract":"","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":" ","pages":"e18638"},"PeriodicalIF":26.8,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145197438","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":"Calcium Phosphate Nanoparticle-Immobilized Macrophage-Derived Extracellular Vesicle Nanohybrid Facilitates Diabetic Bone Regeneration.","authors":"Xiaolan Wu,Shanshan Jin,Qibo Wang,Liyuan Chen,Xinjia Cai,Min Yu,Houzuo Guo,He Zhang,Hangbo Liu,Chang Li,Shiying Zhang,Xinmeng Shi,Lifang Feng,Shiqiang Gong,Dan Luo,Cunyu Wang,Yan Liu","doi":"10.1002/adma.202509410","DOIUrl":"https://doi.org/10.1002/adma.202509410","url":null,"abstract":"Diabetes significantly hinders bone regeneration, and existing tissue engineering therapies struggle to improve the hyperglycemia-induced inflammatory microenvironment, resulting in unbalanced bone remodeling. M2-macrophage-derived extracellular vesicles (M2EVs) possess inherent immunomodulatory properties and promote stem cell differentiation; however, their therapeutic potential in diabetic bone regeneration is significantly limited by poor stability and insufficient osteoinductive capacity. Inspired by biomineralization, a calcium phosphate nanoparticle-immobilized macrophage-derived small extracellular vesicle nanohybrid (M2EV@CaP) is developed by in situ growth of inorganic nanocrystals on M2EV surfaces. In the nanohybrid system, the chemically inert CaP-nanoparticle-reinforced shell provides structural protection for M2EV, inhibiting vesicle aggregation caused by membrane protein denaturation/cross-linking or lipid phase transition through physical barrier. More importantly, M2EV@CaP provides bioavailable calcium/phosphorus ion reservoirs and signaling molecules for bone regeneration and releases responsively under inflammation-induced acidic conditions. In vitro, M2EV@CaP significantly enhances macrophage polarization toward a reparative M2 phenotype, and promotes stem cell osteogenic differentiation under high-glucose inflammatory conditions by activating the Ca2+-Akt signaling axis. In vivo, hydrogel-assisted delivery of M2EV@CaP significantly promotes bone regeneration in diabetic rat calvarial defects through immunomodulation and osteoinduction. This study proposes a nanohybridization strategy based on inorganic nanoparticles reinforcing biostructures, offering a promising extracellular vesicle therapy for complex pathological conditions.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"73 1","pages":"e09410"},"PeriodicalIF":29.4,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145194684","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":"Spatiotemporal Self-Encrypted Interlock-Cascade-Hashing Optical Storage Based on Multicolor Photochromic Lithographic Array.","authors":"Zan Xu,Mingze Liu,Xue Bai,Rongbao Feng,Zeyulong Wen,Yingzhu Zi,Xinhao Cai,Yueteng Zhang,Chenchen Yang,Asif Ali Haider,Haidong Niu,Yue Liu,Yangke Cun,Anjun Huang,Zhiguo Song,Jianbei Qiu,Jiayan Liao,Ting Xu,Ji Zhou,Zhengwen Yang","doi":"10.1002/adma.202506247","DOIUrl":"https://doi.org/10.1002/adma.202506247","url":null,"abstract":"Continuing deve7lopments in artificial intelligence and quantum computing challenge the information security of physical assets and intellectual property. Photochromic materials have emerged as promising candidates for optical encryption and storage applications due to their intrinsic reversible, real-time light absorption modulation capability. Although all-inorganic devices exhibit pronounced stability and fatigue resistance, single-component multicolor photochromic systems remain exceedingly rare. Here, a multicolor photochromic phenomenon is reported in PbMoO4 microcrystal, demonstrating both volatility and non-volatility through distinct photochromic channels. The input, output, and control signals of this material are all different wavelengths of light, which operate in an all-optical and non-destructive manner. Moreover, the all-solid-state nature of PbMoO4 ensures its stable modulation capability after multiple photoresponse cycles with upconversion luminescence modulation up to 99%. By combining experimental characterizations with ab-initio molecular dynamics (AIMD) simulations, the mechanisms of each photochromic channel are revealed. Employing lithography and mask patterning, on-chip arrays are fabricated to demonstrate the feasibility of spatiotemporal self-encrypted optical information storage and interlock-cascade-hashing encryption. This work holds significant promise for advancing anti-cloning and anti-cracking technologies for high-value devices, assets, and information.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"78 1","pages":"e06247"},"PeriodicalIF":29.4,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145194748","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":"Heterogenized Copper(II) Phenanthroline Catalysts for Electroreduction of CO2 to C2 Compounds: Substitution on the Ligand Causes Structural Changes to the Molecular Framework and Stability Enhancement.","authors":"Na Liu,Trang Minh Pham,Yanan Han,Linfeng Yang,Olga S Bokareva,Stephan Bartling,Armin Springer,Anke Spannenberg,Christoph Kubis,Jana Weiss,Dmitry E Doronkin,Wen Ju,Robert Francke","doi":"10.1002/adma.202513702","DOIUrl":"https://doi.org/10.1002/adma.202513702","url":null,"abstract":"Molecular Cu catalysts have shown promise for electrochemical CO2 reduction (eCO2RR) to multi-carbon products. Unlike metallic Cu facets, they offer precise control over the active site's electronic and steric configuration. However, prior studies identified critical challenges related to irreversible potential-induced formation of Cu particles, which participate in the eCO2RR and obscure the role of molecular motifs. Based on a previously reported binuclear Cu(II) phenanthroline catalyst, a structurally modified second-generation system with enhanced stability is developed. By introducing methoxy groups to the phenanthroline ligand, the molecular framework changes from a binuclear complex to an oligonuclear step-like structure consisting of Cu(II) ions linked by µ2- and µ3-OH groups. When immobilized on a gas diffusion electrode, stable operation with a Faradaic efficiency of >70% for C2 products is achieved at elevated current densities. In situ XAS spectroscopy shows only negligible changes of the Cu coordination environment up to 50 mA cm-2. When approaching 250 mA cm-2, partial and reversible phase evolution occurs under Cu2+ valence state reduction, followed by phase recovery upon bias removal. This system combines structural robustness with adaptive redox behavior, demonstrating a route for implementing molecular electrocatalysts in eCO2RR processes at industrial current densities.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"24 1","pages":"e13702"},"PeriodicalIF":29.4,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145194747","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}