Composite structures created from metal‒organic framework (MOF) matrices are reviewed in this work. Depending on the nature of the second component apart from the MOF platform, several synergistic properties may arise; at the same time, the initial features of the single constituent materials are usually maintained, and individual shortcomings are mitigated. Currently, timely energy and environmental challenges necessitate the quest for more advanced materials and technologies. Significant developments in MOF-nanocomposites have enabled their application across a wide range of modern and traditional fields. This review demonstrates in an exhaustive and critical way a broad range of MOF-based nanocomposites, namely, MOF/perovskite nanoparticles (NPs), MOF/metal (non-iron) oxide NPs, MOF/Fe3O4 NPs, MOF/metal chalcogenide NPs, MOF/metal NPs, and MOF/carbon-based materials, as well as nanocomposites of MOFs with other semiconductor NPs. Key points related to the synthesis, characterization, and applications of these materials are provided. Depending on their configuration, the composites under discussion can be applied in domains such as photoelectrochemical sensing, antibiotic/dye degradation, optoelectronics, photovoltaics, catalysis, solar cells, supercapacitors, batteries, water remediation, and drug loading. Sometimes, MOFs can undergo certain processes (e.g. pyrolysis) and act as precursors for composite materials with appealing characteristics. Therefore, a special section in the manuscript is devoted to MOF-derived NP composites. Toward the end of the text, we conclude while also describing the challenges and possibilities for further investigations in the umbrella of material categories analyzed herein. Despite the progress achieved, key questions remain to be answered regarding the relationships among the morphology, properties, and polyvalent activity of these materials. The present work aims to shed light on most of their aspects and innovative prospects, facilitating a deeper comprehension of the underlying phenomena, functionality, and mechanistic insights governing their behavior.
{"title":"State-of-the-Art, Insights, and Perspectives for MOFs-Nanocomposites and MOF-Derived (Nano)Materials","authors":"Stefanos Mourdikoudis, Subhajit Dutta, Saqib Kamal, Sergio Gómez-Graña, Isabel Pastoriza-Santos, Stefan Wuttke, Lakshminarayana Polavarapu","doi":"10.1002/adma.202415399","DOIUrl":"https://doi.org/10.1002/adma.202415399","url":null,"abstract":"Composite structures created from metal‒organic framework (MOF) matrices are reviewed in this work. Depending on the nature of the second component apart from the MOF platform, several synergistic properties may arise; at the same time, the initial features of the single constituent materials are usually maintained, and individual shortcomings are mitigated. Currently, timely energy and environmental challenges necessitate the quest for more advanced materials and technologies. Significant developments in MOF-nanocomposites have enabled their application across a wide range of modern and traditional fields. This review demonstrates in an exhaustive and critical way a broad range of MOF-based nanocomposites, namely, MOF/perovskite nanoparticles (NPs), MOF/metal (non-iron) oxide NPs, MOF/Fe<sub>3</sub>O<sub>4</sub> NPs, MOF/metal chalcogenide NPs, MOF/metal NPs, and MOF/carbon-based materials, as well as nanocomposites of MOFs with other semiconductor NPs. Key points related to the synthesis, characterization, and applications of these materials are provided. Depending on their configuration, the composites under discussion can be applied in domains such as photoelectrochemical sensing, antibiotic/dye degradation, optoelectronics, photovoltaics, catalysis, solar cells, supercapacitors, batteries, water remediation, and drug loading. Sometimes, MOFs can undergo certain processes (e.g. pyrolysis) and act as precursors for composite materials with appealing characteristics. Therefore, a special section in the manuscript is devoted to MOF-derived NP composites. Toward the end of the text, we conclude while also describing the challenges and possibilities for further investigations in the umbrella of material categories analyzed herein. Despite the progress achieved, key questions remain to be answered regarding the relationships among the morphology, properties, and polyvalent activity of these materials. The present work aims to shed light on most of their aspects and innovative prospects, facilitating a deeper comprehension of the underlying phenomena, functionality, and mechanistic insights governing their behavior.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"35 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853806","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}
Lisa-Marie Kern, Vladyslav M. Kuchkin, Victor Deinhart, Christopher Klose, Themistoklis Sidiropoulos, Maike Auer, Simon Gaebel, Kathinka Gerlinger, Riccardo Battistelli, Steffen Wittrock, Tamer Karaman, Michael Schneider, Christian M. Günther, Dieter Engel, Ingo Will, Sebastian Wintz, Markus Weigand, Felix Büttner, Katja Höflich, Stefan Eisebitt, Bastian Pfau
Topologically non-trivial magnetic solitons are complex spin textures with a distinct single-particle nature. Although magnetic skyrmions, especially those with unity topological charge, have attracted substantial interest due to their potential applications, more complex topological textures remain largely theoretical. In this work, the stabilization of isolated higher-order skyrmion bags beyond the prototypical π-skyrmion in ferromagnetic thin films is experimentally demonstrate, which has posed considerable challenges to date. Specifically, controlled generation of skyrmionium (2π-skyrmion), target skyrmion (3π-skyrmion), and skyrmion bags (with variable topological charge) are achieved through the introduction of artificially engineered anisotropy defects via local ion irradiation. They act as preferential sites for the field- or laser-induced nucleation of skyrmion bags. Remarkably, ultrafast laser pulses achieve a substantially higher conversion rate transforming skyrmions into higher-order skyrmion bags compared to their formation driven by magnetic fields. High-resolution x-ray imaging enables direct observation of the resulting skyrmion bags. Complementary micromagnetic simulations reveal the pivotal role of defect geometry–particularly diameter–in stabilizing closed-loop domain textures. The findings not only broaden the experimental horizon for skyrmion research, but also suggest strategies for exploiting complex topological spin textures within a unified material platform for practical applications.
{"title":"Controlled Formation of Skyrmion Bags","authors":"Lisa-Marie Kern, Vladyslav M. Kuchkin, Victor Deinhart, Christopher Klose, Themistoklis Sidiropoulos, Maike Auer, Simon Gaebel, Kathinka Gerlinger, Riccardo Battistelli, Steffen Wittrock, Tamer Karaman, Michael Schneider, Christian M. Günther, Dieter Engel, Ingo Will, Sebastian Wintz, Markus Weigand, Felix Büttner, Katja Höflich, Stefan Eisebitt, Bastian Pfau","doi":"10.1002/adma.202501250","DOIUrl":"https://doi.org/10.1002/adma.202501250","url":null,"abstract":"Topologically non-trivial magnetic solitons are complex spin textures with a distinct single-particle nature. Although magnetic skyrmions, especially those with unity topological charge, have attracted substantial interest due to their potential applications, more complex topological textures remain largely theoretical. In this work, the stabilization of isolated higher-order skyrmion bags beyond the prototypical π-skyrmion in ferromagnetic thin films is experimentally demonstrate, which has posed considerable challenges to date. Specifically, controlled generation of skyrmionium (2π-skyrmion), target skyrmion (3π-skyrmion), and skyrmion bags (with variable topological charge) are achieved through the introduction of artificially engineered anisotropy defects via local ion irradiation. They act as preferential sites for the field- or laser-induced nucleation of skyrmion bags. Remarkably, ultrafast laser pulses achieve a substantially higher conversion rate transforming skyrmions into higher-order skyrmion bags compared to their formation driven by magnetic fields. High-resolution x-ray imaging enables direct observation of the resulting skyrmion bags. Complementary micromagnetic simulations reveal the pivotal role of defect geometry–particularly diameter–in stabilizing closed-loop domain textures. The findings not only broaden the experimental horizon for skyrmion research, but also suggest strategies for exploiting complex topological spin textures within a unified material platform for practical applications.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"11 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853808","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}
During past decades, the construction of morphotropic phase boundary (MPB) behavior in ceramic-based relaxor ferroelectrics has successfully led to a significant enhancement in the piezoelectric coefficient for actuators, transducers, and sensors application. However, MPB-like behavior is achieved only in the ferroelectric state in flexible ferroelectric polymers such as poly(vinylidene fluoride-trifluoroethylene) with the highest piezoelectric coefficients of ≈−63.5 pC/N, due to the lack of a rational design in polymer chain structure and composition. Here, the study reports the first MPB-like behavior observed in a relaxor ferroelectric polymer synthesized by fully hydrogenating poly(vinylidene fluoride-chlorotrifluoroethylene), which are primarily linked in a head-to-head/tail-to-tail manner, and trifluoroethylene units are randomly dispersed along the molecular chain. The unique polymer chain structure is found to be responsible for the formation of conformations disorder, thus strong relaxor behavior, and phase transition from an all-trans conformation to 3/1 helix, thus inducing phase boundary behavior. As a result, an outstanding longitudinal piezoelectric coefficient of −107 pC/N, more than five times higher than that of commercial poly(vinylidene fluoride) (−20 pC/N), is observed. This work opens up a new gate for next-generation high-performance flexible devices.
{"title":"Ultrahigh Piezoelectric Coefficients Achieved by Tailoring the Sequence and Nano-Domain Structure of P(VDF-TrFE)","authors":"Ba Qin, Guo-Tong Ding, Xiao-Yu Yang, Wen-Xuan Li, Yi-Jin He, An-Yi Ren, Wan-Li Xing, Shao-Bo Tan, Xiao-Yong Wei, Zhi-Cheng Zhang","doi":"10.1002/adma.202502708","DOIUrl":"https://doi.org/10.1002/adma.202502708","url":null,"abstract":"During past decades, the construction of morphotropic phase boundary (MPB) behavior in ceramic-based relaxor ferroelectrics has successfully led to a significant enhancement in the piezoelectric coefficient for actuators, transducers, and sensors application. However, MPB-like behavior is achieved only in the ferroelectric state in flexible ferroelectric polymers such as poly(vinylidene fluoride-trifluoroethylene) with the highest piezoelectric coefficients of ≈−63.5 pC/N, due to the lack of a rational design in polymer chain structure and composition. Here, the study reports the first MPB-like behavior observed in a relaxor ferroelectric polymer synthesized by fully hydrogenating poly(vinylidene fluoride-chlorotrifluoroethylene), which are primarily linked in a head-to-head/tail-to-tail manner, and trifluoroethylene units are randomly dispersed along the molecular chain. The unique polymer chain structure is found to be responsible for the formation of conformations disorder, thus strong relaxor behavior, and phase transition from an all<i>-trans</i> conformation to 3/1 helix, thus inducing phase boundary behavior. As a result, an outstanding longitudinal piezoelectric coefficient of −107 pC/N, more than five times higher than that of commercial poly(vinylidene fluoride) (−20 pC/N), is observed. This work opens up a new gate for next-generation high-performance flexible devices.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"47 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853810","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}
Xinzhe Xue, Zhen Liu, Swetha Chandrasekaran, Samuel Eisenberg, Curtis Althaus, Megan C. Freyman, Anica Pinongcos, Qiu Ren, Logan Valdovinos, Cathleen Hsieh, Bintao Hu, Bruce Dunn, Christine A. Orme, Xiao Wang, Marcus A. Worsley, Yat Li
Manganese dioxide (MnO2) deposition/dissolution (Mn2+/MnO2) chemistry, involving a two-electron-transfer process, holds promise for safe and eco-friendly large-scale energy storage. However, challenges like electrode/electrolyte interface environment fluctuations (H+ and H2O activity), irreversible Mn degradation, and limited understanding of degradation mechanisms hinder the reversibility of the Mn2+/MnO2 conversion. This study demonstrates a vanadyl/pervanadyl (VO2+/VO2+) redox-mediated interface designed for high-energy Mn2+/MnO2 batteries. Unlike flow systems, this work uncovers, for the first time, the mechanism of a static redox-mediated interface in regulating interfacial H+ and H2O activities. Significantly, the VO2+/VO2+ chemical redox mediation targets Mn3+ intermediates, suppressing their hydrolysis and enabling 100% Mn2+/MnO2 conversion. The redox-mediated interface enhances the Mn redox electron transfer process, achieving a stable ≈95% coulombic efficiency and ultrahigh capacity of 100 mAh cm−2 with an areal energy density of 111 mWh cm−2, outperforming flow systems. The electrode also exhibits an average specific capacity of 593 mAh g−1, approaching the theoretical limit of 616 mAh g−1, and a specific energy density of 721 Wh kg−1 at high MnO2 loadings (50–150 mg cm−2). The findings highlight the critical role of interfacial redox mediation in regulating H+ and H2O activities and underscore the significance of interface dynamics.
二氧化锰（MnO2）沉积/溶解（Mn2+/MnO2）化学过程涉及双电子转移过程，有望实现安全和环保的大规模储能。然而，诸如电极/电解质界面环境波动（H+和H2O活性），不可逆的Mn降解以及对降解机制的有限理解等挑战阻碍了Mn2+/MnO2转化的可逆性。本研究展示了一种设计用于高能Mn2+/MnO2电池的钒基/过钒基（VO2+/VO2+）氧化还原介导界面。与流动系统不同，这项工作首次揭示了静态氧化还原介导的界面调节界面H+和H2O活性的机制。值得注意的是，VO2+/VO2+化学氧化还原介质以Mn3+中间体为目标，抑制它们的水解，实现100%的Mn2+/MnO2转化。氧化还原介导的界面增强了Mn氧化还原电子传递过程，实现了稳定的约95%的库仑效率和100 mAh cm - 2的超高容量，面能密度为111 mWh cm - 2，优于流动体系。该电极的平均比容量为593 mAh g−1，接近616 mAh g−1的理论极限，在高MnO2负载（50-150 mg cm−2）下的比能量密度为721 Wh kg−1。这些发现强调了界面氧化还原调解在调节H+和H2O活性中的关键作用，并强调了界面动力学的重要性。
{"title":"Interface-Controlled Redox Chemistry in Aqueous Mn2⁺/MnO₂ Batteries","authors":"Xinzhe Xue, Zhen Liu, Swetha Chandrasekaran, Samuel Eisenberg, Curtis Althaus, Megan C. Freyman, Anica Pinongcos, Qiu Ren, Logan Valdovinos, Cathleen Hsieh, Bintao Hu, Bruce Dunn, Christine A. Orme, Xiao Wang, Marcus A. Worsley, Yat Li","doi":"10.1002/adma.202419505","DOIUrl":"https://doi.org/10.1002/adma.202419505","url":null,"abstract":"Manganese dioxide (MnO<sub>2</sub>) deposition/dissolution (Mn<sup>2+</sup>/MnO<sub>2</sub>) chemistry, involving a two-electron-transfer process, holds promise for safe and eco-friendly large-scale energy storage. However, challenges like electrode/electrolyte interface environment fluctuations (H<sup>+</sup> and H<sub>2</sub>O activity), irreversible Mn degradation, and limited understanding of degradation mechanisms hinder the reversibility of the Mn<sup>2+</sup>/MnO<sub>2</sub> conversion. This study demonstrates a vanadyl/pervanadyl (VO<sup>2+</sup>/VO<sub>2</sub><sup>+</sup>) redox-mediated interface designed for high-energy Mn<sup>2+</sup>/MnO<sub>2</sub> batteries. Unlike flow systems, this work uncovers, for the first time, the mechanism of a static redox-mediated interface in regulating interfacial H<sup>+</sup> and H<sub>2</sub>O activities. Significantly, the VO<sup>2+</sup>/VO<sub>2</sub><sup>+</sup> chemical redox mediation targets Mn<sup>3+</sup> intermediates, suppressing their hydrolysis and enabling 100% Mn<sup>2+</sup>/MnO<sub>2</sub> conversion. The redox-mediated interface enhances the Mn redox electron transfer process, achieving a stable ≈95% coulombic efficiency and ultrahigh capacity of 100 mAh cm<sup>−</sup><sup>2</sup> with an areal energy density of 111 mWh cm<sup>−</sup><sup>2</sup>, outperforming flow systems. The electrode also exhibits an average specific capacity of 593 mAh g<sup>−1</sup>, approaching the theoretical limit of 616 mAh g<sup>−1</sup>, and a specific energy density of 721 Wh kg<sup>−1</sup> at high MnO<sub>2</sub> loadings (50–150 mg cm<sup>−2</sup>). The findings highlight the critical role of interfacial redox mediation in regulating H<sup>+</sup> and H<sub>2</sub>O activities and underscore the significance of interface dynamics.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"24 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143857400","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}
Lithium iron phosphate (LiFePO4) batteries are increasingly adopted in grid-scale energy storage due to their superior performance and cost metrics. However, as the desired energy and power are further densified, the lifespan of LiFePO4 batteries is significantly limited, mainly because the lithium plating severely occurs on the graphite anode. Here, first the lithium plating characteristics of both energy-type and power-type graphite electrodes in single-layer design are deciphered. Based on these findings, a suitable two-layer design with energy-type graphite on the top layer and power-type one on the bottom layer, is disclosed. Such configuration effectively inhibits lithium plating throughout the graphite electrode, drastically increasing the lifespan in an energy- and power-densified LiFePO4 battery. The assembled pouch cell with an energy density of 161.5 Wh kg−1, delivers a capacity retention rate of 90.8% after 2000 cycles at 2 C. This work provides valuable insights into the failure mechanism of graphite electrodes, but also innovative strategies of electrode engineering for extending batteries’ performance horizon.
{"title":"Two-Layer Graphite Anode for Energy and Power Densified LiFePO4 Battery","authors":"Renjie He, Wei Zhong, Yuanke Wu, Wei Liu, Chuyue Cai, Shijie Cheng, Ling Huang, Jia Xie","doi":"10.1002/adma.202501185","DOIUrl":"https://doi.org/10.1002/adma.202501185","url":null,"abstract":"Lithium iron phosphate (LiFePO<sub>4</sub>) batteries are increasingly adopted in grid-scale energy storage due to their superior performance and cost metrics. However, as the desired energy and power are further densified, the lifespan of LiFePO<sub>4</sub> batteries is significantly limited, mainly because the lithium plating severely occurs on the graphite anode. Here, first the lithium plating characteristics of both energy-type and power-type graphite electrodes in single-layer design are deciphered. Based on these findings, a suitable two-layer design with energy-type graphite on the top layer and power-type one on the bottom layer, is disclosed. Such configuration effectively inhibits lithium plating throughout the graphite electrode, drastically increasing the lifespan in an energy- and power-densified LiFePO<sub>4</sub> battery. The assembled pouch cell with an energy density of 161.5 Wh kg<sup>−1</sup>, delivers a capacity retention rate of 90.8% after 2000 cycles at 2 C. This work provides valuable insights into the failure mechanism of graphite electrodes, but also innovative strategies of electrode engineering for extending batteries’ performance horizon.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"7 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143857511","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}
Haotian Guan, Jiang Liu, Xuan Sun, Yangfan Lu, Hongyuan Wang, Qun Luo, Qian Li, Fusheng Pan
Enhancing hydrogenation and dehydrogenation (de/hydrogenation) kinetics without compromising cycle stability is a major challenge for Mg-based hydrogen storage materials (Mg/MgH2). The de/hydrogenation reactions of Mg/MgH2 are one of the gas–solid reactions involving hydrogen adsorption, dissociation, diffusion, and nucleation, which often results in the catalysts being unable to simultaneously accelerate these distinct kinetic processes. Here, the Mg2Ni@Ti─MgO catalyst with dual active sites is reported to be designed to address this issue. The stabilization of Ti2+ and Ti3+ valence states in the MgO lattice simultaneously accelerates hydrogen adsorption and dissociation. Additionally, Mg2Ni serves as a hydrogen diffusion and nucleation center, synergistically enhancing de/hydrogenation reactions. Consequently, it enables MgH2 to release 5.28 wt.% H2 in 2 min at 280 °C, and achieves 1.96 wt.% H2 of hydrogen release in 60 min at 180 °C. The Mg2Ni@Ti─MgO catalyst exhibits remarkable chemical stability at the interfacial structure, minimizing structural and chemical degradation impact, and realizing excellent de/hydrogenation performance over 1000 cycles. These results provide a new methodology for optimizing multiple kinetic steps, attaining highly efficient and stable de/hydrogenation reactions.
{"title":"Titanium‒Nickel Dual Active Sites Enabled Reversible Hydrogen Storage of Magnesium at 180 °C with Exceptional Cycle Stability","authors":"Haotian Guan, Jiang Liu, Xuan Sun, Yangfan Lu, Hongyuan Wang, Qun Luo, Qian Li, Fusheng Pan","doi":"10.1002/adma.202500178","DOIUrl":"https://doi.org/10.1002/adma.202500178","url":null,"abstract":"Enhancing hydrogenation and dehydrogenation (de/hydrogenation) kinetics without compromising cycle stability is a major challenge for Mg-based hydrogen storage materials (Mg/MgH<sub>2</sub>). The de/hydrogenation reactions of Mg/MgH<sub>2</sub> are one of the gas–solid reactions involving hydrogen adsorption, dissociation, diffusion, and nucleation, which often results in the catalysts being unable to simultaneously accelerate these distinct kinetic processes. Here, the Mg<sub>2</sub>Ni@Ti─MgO catalyst with dual active sites is reported to be designed to address this issue. The stabilization of Ti<sup>2+</sup> and Ti<sup>3+</sup> valence states in the MgO lattice simultaneously accelerates hydrogen adsorption and dissociation. Additionally, Mg<sub>2</sub>Ni serves as a hydrogen diffusion and nucleation center, synergistically enhancing de/hydrogenation reactions. Consequently, it enables MgH<sub>2</sub> to release 5.28 wt.% H<sub>2</sub> in 2 min at 280 °C, and achieves 1.96 wt.% H<sub>2</sub> of hydrogen release in 60 min at 180 °C. The Mg<sub>2</sub>Ni@Ti─MgO catalyst exhibits remarkable chemical stability at the interfacial structure, minimizing structural and chemical degradation impact, and realizing excellent de/hydrogenation performance over 1000 cycles. These results provide a new methodology for optimizing multiple kinetic steps, attaining highly efficient and stable de/hydrogenation reactions.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"16 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853802","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}
Engineering electrocatalysts at a single-atomic site can enable unprecedented atomic utilization and catalytic activity, yet it remains challenging in multimetallic active centers to simultaneously achieve high catalytic selectivity and stability. Herein, the atomic design and control of golden single-atom alloys (PdAu1 and PtAu1 SAAs) based on fully ordered PdBi and PtBi matrixes is presented, serving as highly selective, active, and stable cathode and anode electrocatalysts, respectively, to trigger direct methanol fuel cell (DMFC). The octahedral PdAu1 SAA exhibits ultrahigh mass-activity of 5.37 A mgPd + Au−1 without noticeable decay for 12 0000 cycles toward oxygen reduction. While PdAu1 SAA is inactive for methanol oxidation, PtAu1 SAA exhibits an ultrahigh mass-activity of 28.59 A mgPt + Au−1. The selective electrocatalysts drive a practical DMFC with a high-power density of 155.0 mW cm−2. Density functional theory calculations reveal the desired regulation of selectivity via reducing the energy barrier for potential-determining steps (PDS) of *OH to H2O and *HCOO to CO2. This work provides a general strategy to engineer multimetallic alloys at the atomic level, advancing the development of high-performance electrocatalysts.
在单原子位点上设计电催化剂可以实现前所未有的原子利用率和催化活性，但在多金属活性中心中同时实现高催化选择性和稳定性仍然是一项挑战。本文介绍了基于完全有序的 PdBi 和 PtBi 基体的黄金单原子合金（PdAu1 和 PtAu1 SAA）的原子设计和控制，它们可分别用作高选择性、高活性和高稳定性的阴极和阳极电催化剂，以触发直接甲醇燃料电池（DMFC）。八面体 PdAu1 SAA 表现出 5.37 A mgPd + Au-1 的超高质量活性，在 12 0000 个氧还原循环中没有明显衰减。PdAu1 SAA 对甲醇氧化不活跃，而 PtAu1 SAA 则表现出 28.59 A mgPt + Au-1 的超高质量活性。这种选择性电催化剂能驱动实用的 DMFC，其功率密度高达 155.0 mW cm-2。密度泛函理论计算显示，通过降低 *OH 到 H2O 和 *HCOO 到 CO2 的电位决定步骤 (PDS) 的能量障碍，可对选择性进行理想的调节。这项工作为在原子水平上设计多金属合金提供了一种通用策略，从而推动了高性能电催化剂的开发。
{"title":"Golden Single-Atom Alloys Selectively Boosting Oxygen Reduction and Methanol Oxidation","authors":"Shuiping Luo, Lei Xie, Xinyi Cai, Wen Chen, Jiayi Wu, Yutian Ding, Yongsheng Zhou, Zewei Quan, Renfei Feng, Xian-Zhu Fu, Jing-Li Luo","doi":"10.1002/adma.202500848","DOIUrl":"https://doi.org/10.1002/adma.202500848","url":null,"abstract":"Engineering electrocatalysts at a single-atomic site can enable unprecedented atomic utilization and catalytic activity, yet it remains challenging in multimetallic active centers to simultaneously achieve high catalytic selectivity and stability. Herein, the atomic design and control of golden single-atom alloys (PdAu<sub>1</sub> and PtAu<sub>1</sub> SAAs) based on fully ordered PdBi and PtBi matrixes is presented, serving as highly selective, active, and stable cathode and anode electrocatalysts, respectively, to trigger direct methanol fuel cell (DMFC). The octahedral PdAu<sub>1</sub> SAA exhibits ultrahigh mass-activity of 5.37 A mg<sub>Pd + Au</sub><sup>−1</sup> without noticeable decay for 12 0000 cycles toward oxygen reduction. While PdAu<sub>1</sub> SAA is inactive for methanol oxidation, PtAu<sub>1</sub> SAA exhibits an ultrahigh mass-activity of 28.59 A mg<sub>Pt + Au</sub><sup>−1</sup>. The selective electrocatalysts drive a practical DMFC with a high-power density of 155.0 mW cm<sup>−2</sup>. Density functional theory calculations reveal the desired regulation of selectivity via reducing the energy barrier for potential-determining steps (PDS) of <sup>*</sup>OH to H<sub>2</sub>O and <sup>*</sup>HCOO to CO<sub>2</sub>. This work provides a general strategy to engineer multimetallic alloys at the atomic level, advancing the development of high-performance electrocatalysts.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"108 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853803","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}
Tissue adhesives are promising materials for expeditious hemorrhage control, while it remains a grand challenge to engineer a superior formulation with instantaneous adhesion, on‐demand debonding, and the integration of multiple desirable properties such as antibacterial and hemostatic capabilities. Herein, a multifunctional supramolecular tissue adhesive based on guanidinium‐modified polydimethylsiloxane (PDMS) is introduced, driven by a reversible microphase separation mechanism. By optimizing the content of guanidinium ions, precise control over cohesive strength, adhesion, and wettability is achieved, resulting in strong instantaneous adhesion under both dry and wet conditions. Notably, the supramolecular nature of the adhesive allows for convenient on‐demand removal using medical‐grade alcohol, offering a critical advantage for easy debonding. Additionally, the adhesive exhibits remarkable antimicrobial properties while maintaining excellent biocompatibility and hemocompatibility. Its underwater injectability supports minimally invasive surgical procedures. Furthermore, the adhesive's ability to incorporate solid particles enhances its versatility, particularly for the development of drug‐embedded bioadhesives. This work addresses key challenges in tissue adhesive design via a microphase separation‐driven working principle, thereby opening promising new avenues for the development of advanced bioadhesives with tailored properties and enhanced surgical and wound care outcomes.
{"title":"A Microphase Separation‐Driven Supramolecular Tissue Adhesive with Instantaneous Dry/Wet Adhesion, Alcohol‐Triggered Debonding, and Antibacterial Hemostasis","authors":"Bowen Pang, Weichang Li, Jiaqin Li, Shangwu Yang, Taolin Sun, Qianqian Yu, Kan Yue, Wei Zhang","doi":"10.1002/adma.202501810","DOIUrl":"https://doi.org/10.1002/adma.202501810","url":null,"abstract":"Tissue adhesives are promising materials for expeditious hemorrhage control, while it remains a grand challenge to engineer a superior formulation with instantaneous adhesion, on‐demand debonding, and the integration of multiple desirable properties such as antibacterial and hemostatic capabilities. Herein, a multifunctional supramolecular tissue adhesive based on guanidinium‐modified polydimethylsiloxane (PDMS) is introduced, driven by a reversible microphase separation mechanism. By optimizing the content of guanidinium ions, precise control over cohesive strength, adhesion, and wettability is achieved, resulting in strong instantaneous adhesion under both dry and wet conditions. Notably, the supramolecular nature of the adhesive allows for convenient on‐demand removal using medical‐grade alcohol, offering a critical advantage for easy debonding. Additionally, the adhesive exhibits remarkable antimicrobial properties while maintaining excellent biocompatibility and hemocompatibility. Its underwater injectability supports minimally invasive surgical procedures. Furthermore, the adhesive's ability to incorporate solid particles enhances its versatility, particularly for the development of drug‐embedded bioadhesives. This work addresses key challenges in tissue adhesive design via a microphase separation‐driven working principle, thereby opening promising new avenues for the development of advanced bioadhesives with tailored properties and enhanced surgical and wound care outcomes.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"17 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853342","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}
Xiangyu Sheng, Zhijian Du, Zhiyi Gao, Jianxiong Xu, La Li, Guozhen Shen
The bidirectional modulation of cerebral neurons in the brain possesses enhancement and inhibition of neural activity, which is of great interest in the treatment of motor nerve disorders and emotional disorders, and cognitive defects. However, existing approaches usually rely on electrical/electrochemical stimulations, which show low security by implanting metal probes and unidirectional currents with single modulation. Herein, an implantable in‐hydrogel wireless supercapacitor‐activated neuron system consisting of the coil, diode bridge circuit, in‐hydrogel supercapacitor, and stimulation electrodes is fabricated, which provides a bidirectional and adjustable ion diffusion current to safely and effectively excite and inhibit brain neurons. The designed in‐hydrogel supercapacitor exhibits a high storage charge ability of ≈90 times larger than the devices without hydrogel encapsulation, owing to the in situ radical addition mechanism. Moreover, the in‐hydrogel electrodes are implanted into the thalamus, amygdala, and prefrontal lobes of the brain to evoke the corresponding changes in potential intensity and frequency through the external chargeable coil and diode bridge circuit, which verifies the potential of the multimodule supercapacitor in amelioration and treatment Parkinson's, severe depression, and Alzheimer's disease.
{"title":"An Implantable In‐Hydrogel Wireless Supercapacitor‐Activated Neuron System Enables Bidirectional Modulation","authors":"Xiangyu Sheng, Zhijian Du, Zhiyi Gao, Jianxiong Xu, La Li, Guozhen Shen","doi":"10.1002/adma.202504558","DOIUrl":"https://doi.org/10.1002/adma.202504558","url":null,"abstract":"The bidirectional modulation of cerebral neurons in the brain possesses enhancement and inhibition of neural activity, which is of great interest in the treatment of motor nerve disorders and emotional disorders, and cognitive defects. However, existing approaches usually rely on electrical/electrochemical stimulations, which show low security by implanting metal probes and unidirectional currents with single modulation. Herein, an implantable in‐hydrogel wireless supercapacitor‐activated neuron system consisting of the coil, diode bridge circuit, in‐hydrogel supercapacitor, and stimulation electrodes is fabricated, which provides a bidirectional and adjustable ion diffusion current to safely and effectively excite and inhibit brain neurons. The designed in‐hydrogel supercapacitor exhibits a high storage charge ability of ≈90 times larger than the devices without hydrogel encapsulation, owing to the in situ radical addition mechanism. Moreover, the in‐hydrogel electrodes are implanted into the thalamus, amygdala, and prefrontal lobes of the brain to evoke the corresponding changes in potential intensity and frequency through the external chargeable coil and diode bridge circuit, which verifies the potential of the multimodule supercapacitor in amelioration and treatment Parkinson's, severe depression, and Alzheimer's disease.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"108 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853604","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}
Acquired drug resistance and the immunosuppressive tumor microenvironment significantly limit the efficacy of chemotherapy and immunotherapy in advanced prostate cancer. Blocking the PI3K/mTOR signaling pathway has been recently proved as a new strategy to improve sensitivity to chemotherapy and immunotherapy. Herein, glutathione (GSH)-sensitive nanoparticles (PSMA-NP/BEZ) are developed that can target prostate-specific membrane antigen (PSMA), loaded with PI3K/mTOR dual inhibitor prodrug BEZ235. BEZ235 can be released from PSMA-NP/BEZ in response to elevated GSH levels in prostate cancer tissues, inhibiting the PI3K/AKT/mTOR pathway and impairing downstream cellular functions such as cell proliferation, DNA repair, and protein synthesis. When combined with paclitaxel, PSMA-NP/BEZ could reduce drug efflux by downregulating P-glycoprotein expression in cancer cells, thus enhancing the sensitivity to chemotherapy. Furthermore, PSMA-NP/BEZ could impair the immunosuppressive functions of myeloid-derived suppressor cells and reshape the “cold” immune microenvironment in prostate cancer, enhancing immunotherapeutic efficacy and including long-term immune memory against tumor recurrence. PSMA-NP/BEZ serves a safe and promising strategy to improve the efficacy of chemotherapy and immunotherapy in advanced prostate cancer.
{"title":"PSMA-Targeted Nanoparticles with PI3K/mTOR Dual Inhibitor Downregulate P-Glycoprotein and Inactivate Myeloid-Derived Suppressor Cells for Enhanced Chemotherapy and Immunotherapy in Prostate Cancer","authors":"Lu Yin, Feiya Yang, Wenkuan Wang, Lingpu Zhang, Zheng Cao, Haoyuan Shi, Kehao Pan, Liyuan Wu, Haihua Xiao, Nianzeng Xing","doi":"10.1002/adma.202415322","DOIUrl":"https://doi.org/10.1002/adma.202415322","url":null,"abstract":"Acquired drug resistance and the immunosuppressive tumor microenvironment significantly limit the efficacy of chemotherapy and immunotherapy in advanced prostate cancer. Blocking the PI3K/mTOR signaling pathway has been recently proved as a new strategy to improve sensitivity to chemotherapy and immunotherapy. Herein, glutathione (GSH)-sensitive nanoparticles (PSMA-NP/BEZ) are developed that can target prostate-specific membrane antigen (PSMA), loaded with PI3K/mTOR dual inhibitor prodrug BEZ235. BEZ235 can be released from PSMA-NP/BEZ in response to elevated GSH levels in prostate cancer tissues, inhibiting the PI3K/AKT/mTOR pathway and impairing downstream cellular functions such as cell proliferation, DNA repair, and protein synthesis. When combined with paclitaxel, PSMA-NP/BEZ could reduce drug efflux by downregulating P-glycoprotein expression in cancer cells, thus enhancing the sensitivity to chemotherapy. Furthermore, PSMA-NP/BEZ could impair the immunosuppressive functions of myeloid-derived suppressor cells and reshape the “cold” immune microenvironment in prostate cancer, enhancing immunotherapeutic efficacy and including long-term immune memory against tumor recurrence. PSMA-NP/BEZ serves a safe and promising strategy to improve the efficacy of chemotherapy and immunotherapy in advanced prostate cancer.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"66 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853804","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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