Jiahao Chang, Yaduo Jia, Song Sun, Xin Zhang, Huiyang Gou, Gongkai Wang
The rapid global accumulation of retired wind turbine blades (RWTBs) has emerged as a critical environmental challenge requiring urgent resolution. Conventional recycling methods, primarily limited to landfilling, construction fillers, and co‐processing in cement production, fail to achieve true resource circularity. To address this pressing issue, this study pioneers an innovative value‐added utilization strategy that successfully converts glass fibers from RWTBs into high‐performance silicon–carbon (Si─C) composite anodes for next‐generation lithium‐ion batteries (LIBs). By integrating an alloying reaction‐nitridation treatment with precisely optimized chemical vapor deposition (CVD), we constructed a hierarchically porous recycled micron‐sized silicon (rP‐Si) scaffold structure with uniform carbon coating. The resulting rP‐Si@C composite exhibits exceptional electrochemical performance, maintaining a specific capacity of 1256 mAh g −1 after 300 cycles at 1 A g −1 while demonstrating exceptional structural integrity against mechanical deformation. Systematic characterization via advanced analytical techniques confirms that the unique multi‐level architecture not only effectively accommodates significant volume changes during cycling but also significantly enhances lithium‐ion (Li + ) diffusion kinetics. This work establishes a feasible technological pathway for the sustainable transformation of RWTBs into advanced energy storage components, thereby constructing a complete closed‐loop ecosystem for renewable energy infrastructure.
全球风力涡轮机叶片退役数量的迅速增加已经成为一个迫切需要解决的严峻环境挑战。传统的回收方法主要局限于垃圾填埋、建筑填料和水泥生产中的协同处理,无法实现真正的资源循环。为了解决这一紧迫的问题,本研究开创了一种创新的增值利用策略,成功地将RWTBs中的玻璃纤维转化为下一代锂离子电池(lib)的高性能硅碳(Si─C)复合阳极。通过将合金化反应-氮化处理与精确优化的化学气相沉积(CVD)相结合,我们构建了具有均匀碳涂层的分层多孔再生微米级硅(rP - Si)支架结构。由此产生的rP‐Si@C复合材料具有优异的电化学性能,在1 ag−1下循环300次后保持1256 mAh g−1的比容量,同时具有优异的抗机械变形的结构完整性。通过先进的分析技术进行的系统表征证实,独特的多层结构不仅有效地适应了循环过程中显著的体积变化,而且显著增强了锂离子(Li +)扩散动力学。本研究为rwtb向先进储能组件的可持续转型建立了可行的技术途径,从而构建了一个完整的可再生能源基础设施闭环生态系统。
{"title":"Upcycling Wind Turbine Blade Waste into Hierarchically Porous Silicon–Carbon Anodes for High‐Performance Lithium‐Ion Batteries","authors":"Jiahao Chang, Yaduo Jia, Song Sun, Xin Zhang, Huiyang Gou, Gongkai Wang","doi":"10.1002/adfm.202531483","DOIUrl":"https://doi.org/10.1002/adfm.202531483","url":null,"abstract":"The rapid global accumulation of retired wind turbine blades (RWTBs) has emerged as a critical environmental challenge requiring urgent resolution. Conventional recycling methods, primarily limited to landfilling, construction fillers, and co‐processing in cement production, fail to achieve true resource circularity. To address this pressing issue, this study pioneers an innovative value‐added utilization strategy that successfully converts glass fibers from RWTBs into high‐performance silicon–carbon (Si─C) composite anodes for next‐generation lithium‐ion batteries (LIBs). By integrating an alloying reaction‐nitridation treatment with precisely optimized chemical vapor deposition (CVD), we constructed a hierarchically porous recycled micron‐sized silicon (rP‐Si) scaffold structure with uniform carbon coating. The resulting rP‐Si@C composite exhibits exceptional electrochemical performance, maintaining a specific capacity of 1256 mAh g <jats:sup>−1</jats:sup> after 300 cycles at 1 A g <jats:sup>−1</jats:sup> while demonstrating exceptional structural integrity against mechanical deformation. Systematic characterization via advanced analytical techniques confirms that the unique multi‐level architecture not only effectively accommodates significant volume changes during cycling but also significantly enhances lithium‐ion (Li <jats:sup>+</jats:sup> ) diffusion kinetics. This work establishes a feasible technological pathway for the sustainable transformation of RWTBs into advanced energy storage components, thereby constructing a complete closed‐loop ecosystem for renewable energy infrastructure.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"53 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145962317","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}
Xin‐Yu Li, Zhen‐Yu Miao, Yun‐Shan Jiang, Gang Sun, Fu‐Da Yu, Wang Ke, Liang Deng, Guo‐Xu Zhang, Lei Zhao, Zhen‐Bo Wang
Li‐rich layered oxides (LLOs) are promising high‐capacity cathode materials for next generation Li‐ion batteries, but their practical application is hindered by voltage decay and capacity fading, which primarily originate from irreversible oxygen behaviors. Given that transition metal‐oxygen (TM─O) bonding is crucial for stabilizing anionic redox, this study reveals the critical role of elemental composition in determining the homogeneity of the TM‐O coordination environment within LLOs. This homogeneity directly influences the electrochemical behavior and structural stability of the material. Combining in situ X‐ray diffraction (XRD) and density‐functional theory (DFT) calculations on various model compounds, we demonstrate that while Co thermodynamically enhancing the Mn─O bonds, it forms highly covalent Co─O bonds that disrupt the uniformity of the TM─O bonding network. This inhomogeneity kinetically promotes irreversible ligand‐to‐metal charge transfer, exacerbates lattice strain along c ‐axis, and accelerates oxygen loss. In contrast, Ni promotes a homogeneous TM‐O coordination environment, facilitating reversible charge compensation and accommodating lattice strain through gentle ab ‐plane expansion. Consequently, the Ni‐rich cathodes achieve superior cycling stability and voltage retention. Our findings establish that a uniform TM─O bonding network is more crucial than the absolute bond strength for achieving reversible anionic redox, providing a new design principle for stable and high‐energy cathode materials.
{"title":"Achieving Reversible Anionic Redox via Homogeneous Transition Metal‐Oxygen Coordination in Li‐Rich Layered Oxides","authors":"Xin‐Yu Li, Zhen‐Yu Miao, Yun‐Shan Jiang, Gang Sun, Fu‐Da Yu, Wang Ke, Liang Deng, Guo‐Xu Zhang, Lei Zhao, Zhen‐Bo Wang","doi":"10.1002/adfm.202530355","DOIUrl":"https://doi.org/10.1002/adfm.202530355","url":null,"abstract":"Li‐rich layered oxides (LLOs) are promising high‐capacity cathode materials for next generation Li‐ion batteries, but their practical application is hindered by voltage decay and capacity fading, which primarily originate from irreversible oxygen behaviors. Given that transition metal‐oxygen (TM─O) bonding is crucial for stabilizing anionic redox, this study reveals the critical role of elemental composition in determining the homogeneity of the TM‐O coordination environment within LLOs. This homogeneity directly influences the electrochemical behavior and structural stability of the material. Combining in situ X‐ray diffraction (XRD) and density‐functional theory (DFT) calculations on various model compounds, we demonstrate that while Co thermodynamically enhancing the Mn─O bonds, it forms highly covalent Co─O bonds that disrupt the uniformity of the TM─O bonding network. This inhomogeneity kinetically promotes irreversible ligand‐to‐metal charge transfer, exacerbates lattice strain along <jats:italic>c</jats:italic> ‐axis, and accelerates oxygen loss. In contrast, Ni promotes a homogeneous TM‐O coordination environment, facilitating reversible charge compensation and accommodating lattice strain through gentle <jats:italic>ab</jats:italic> ‐plane expansion. Consequently, the Ni‐rich cathodes achieve superior cycling stability and voltage retention. Our findings establish that a uniform TM─O bonding network is more crucial than the absolute bond strength for achieving reversible anionic redox, providing a new design principle for stable and high‐energy cathode materials.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"29 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145955758","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}
2D ferromagnetic semiconductors are promising for spintronic and quantum applications by integrating electronic and magnetic functionalities at the atomic scale. However, most known ferromagnetic semiconductors suffer from Curie temperatures ( TC ) well below room temperature. Here, we report a 2D ferromagnetic semiconductor Fe 0.98 In 0.02 Te (FIT), exhibiting n‐type conduction and a record‐high TC of 860 K among known 2D magnetic materials to date. The intrinsic ferromagnetism and magnetic domain evolution were confirmed by X‐ray magnetic circular dichroism and magnetic force microscopy measurements. Density functional theory calculations indicate that In enhances ferromagnetic coupling and magnetic anisotropy energy in FIT through local electronic and structural modulation. Our findings pave the way for the applications of 2D ferromagnetic materials in spintronic device fabrication.
二维铁磁半导体通过在原子尺度上集成电子和磁功能,在自旋电子和量子应用方面有很大的前景。然而,大多数已知的铁磁半导体的居里温度(T C)远低于室温。在这里,我们报道了一种二维铁磁半导体Fe 0.98 In 0.02 Te (FIT),在迄今已知的二维磁性材料中,它表现出n型导电和860 K的高温。通过X射线磁性圆二色性和磁力显微镜测量证实了材料的固有铁磁性和磁畴演化。密度泛函理论计算表明,In通过局部电子和结构调制增强了FIT中的铁磁耦合和磁各向异性能。我们的发现为二维铁磁材料在自旋电子器件制造中的应用铺平了道路。
{"title":"High Curie Temperature in 2D Fe 0.98 In 0.02 Te Ferromagnetic Semiconductor via Indium‐Induced Superexchange Enhancement","authors":"Dingyi Yang, Yongjie Xu, Jiawei Liu, Yong Wang, Miao Wang, Yu Zhang, Yang Liu, Yongmei Wang, Qikun Li, Yue Hao, Yizhang Wu","doi":"10.1002/adfm.202532088","DOIUrl":"https://doi.org/10.1002/adfm.202532088","url":null,"abstract":"2D ferromagnetic semiconductors are promising for spintronic and quantum applications by integrating electronic and magnetic functionalities at the atomic scale. However, most known ferromagnetic semiconductors suffer from Curie temperatures ( <jats:italic>T</jats:italic> <jats:sub>C</jats:sub> ) well below room temperature. Here, we report a 2D ferromagnetic semiconductor Fe <jats:sub>0.98</jats:sub> In <jats:sub>0.02</jats:sub> Te (FIT), exhibiting n‐type conduction and a record‐high <jats:italic>T</jats:italic> <jats:sub>C</jats:sub> of 860 K among known 2D magnetic materials to date. The intrinsic ferromagnetism and magnetic domain evolution were confirmed by X‐ray magnetic circular dichroism and magnetic force microscopy measurements. Density functional theory calculations indicate that In enhances ferromagnetic coupling and magnetic anisotropy energy in FIT through local electronic and structural modulation. Our findings pave the way for the applications of 2D ferromagnetic materials in spintronic device fabrication.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"9 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145955794","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}
Claudia Fernández‐González, Pamela Morales‐Fernández, Luke Alexander Turnbull, Claas Abert, Dieter Suess, Michael Foerster, Miguel Á. Niño, Pawel Nita, Anna Mandziak, Simone Finizio, Nuria Bagués, Eva Pereiro, Amalio Fernández‐Pacheco, Lucas Pérez, Sandra Ruiz‐Gómez, Claire Donnelly
{"title":"Realization of Complex‐Shaped Magnetic Nanotubes with 3D Printing and Electrodeposition (Adv. Funct. Mater. 4/2026)","authors":"Claudia Fernández‐González, Pamela Morales‐Fernández, Luke Alexander Turnbull, Claas Abert, Dieter Suess, Michael Foerster, Miguel Á. Niño, Pawel Nita, Anna Mandziak, Simone Finizio, Nuria Bagués, Eva Pereiro, Amalio Fernández‐Pacheco, Lucas Pérez, Sandra Ruiz‐Gómez, Claire Donnelly","doi":"10.1002/adfm.73580","DOIUrl":"https://doi.org/10.1002/adfm.73580","url":null,"abstract":"","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"4 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145955791","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}
Song Gao, Hao Li, Ning Li, Wenjing Yue, Hongsen Niu, Binghao Wang, Yang Li
Flexible tactile sensors are rapidly evolving toward high‐resolution, multimodal sensing and large‐area integrability, but traditional manufacturing processes face inherent limitations in complex 3D structure construction, material system compatibility, and fast and efficient manufacturing. Additive manufacturing (AM) technology, with its unique advantages such as on‐demand forming, high structural freedom, and multi‐material collaborative processing, is becoming a core driving force for breakthroughs in sensing performance and integration, moving the field toward cross‐process integration and accelerated innovation. However, AM processes and applications have not yet formed a complete system, and the development and intelligentization of AM‐based flexible tactile sensors have reached a bottleneck, urgently requiring a comprehensive and systematic review to achieve breakthrough progress. Therefore, this review systematically examines the mechanisms by which different AM processes affect the material properties, structural construction, and overall performance of devices, evaluates their applicability, process advantages, and limitations in micro‐nano structure manufacturing, and summarizes their latest advancements in intelligent systems and emerging application scenarios. Finally, it provides an in‐depth outlook on the future development challenges and potential opportunities of AM‐based flexible tactile sensors.
{"title":"Additive‐Manufacturing‐Based Flexible Tactile Sensors","authors":"Song Gao, Hao Li, Ning Li, Wenjing Yue, Hongsen Niu, Binghao Wang, Yang Li","doi":"10.1002/adfm.202532112","DOIUrl":"https://doi.org/10.1002/adfm.202532112","url":null,"abstract":"Flexible tactile sensors are rapidly evolving toward high‐resolution, multimodal sensing and large‐area integrability, but traditional manufacturing processes face inherent limitations in complex 3D structure construction, material system compatibility, and fast and efficient manufacturing. Additive manufacturing (AM) technology, with its unique advantages such as on‐demand forming, high structural freedom, and multi‐material collaborative processing, is becoming a core driving force for breakthroughs in sensing performance and integration, moving the field toward cross‐process integration and accelerated innovation. However, AM processes and applications have not yet formed a complete system, and the development and intelligentization of AM‐based flexible tactile sensors have reached a bottleneck, urgently requiring a comprehensive and systematic review to achieve breakthrough progress. Therefore, this review systematically examines the mechanisms by which different AM processes affect the material properties, structural construction, and overall performance of devices, evaluates their applicability, process advantages, and limitations in micro‐nano structure manufacturing, and summarizes their latest advancements in intelligent systems and emerging application scenarios. Finally, it provides an in‐depth outlook on the future development challenges and potential opportunities of AM‐based flexible tactile sensors.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"92 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145955792","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}
Gahye Shin, Subhash Chandra Shit, Min Seok Koo, Dong Jin Ham, Hyuk Jae Kwon, Hyunwoong Park, Wooyul Kim
Indoor exposure to volatile organic compounds (VOCs) such as acetaldehyde and toluene poses major health risks, but photocatalytic oxidation over TiO 2 is strongly modulated by humidity and pollutant complexity. Here, we reveal contrasting humidity responses of acetaldehyde and toluene on TiO 2 : acetaldehyde degradation improves under dry conditions, whereas toluene removal requires humid environments to avoid severe deactivation. These divergent behaviors are amplified under mixed‐VOCs feeds, where toluene deactivation suppresses overall mineralization efficiency. Remarkably, plasmonic Au/TiO 2 catalysts exhibit humidity resilient and durable performance, maintaining >70% removal efficiency for both VOCs across RH 25%–80%. Spectroscopic characterizations (XPS, Raman, soft and hard XAS) demonstrate that Au nanoparticles establish strong electronic interactions with TiO 2 facilitating interfacial charge transfer and enhanced ROS generation, while in situ EPR distinguishes the specific formation pathways of • OH, O 2•− , and h + , demonstrating that plasmonic excitation sustains ROS activity even under conditions where TiO 2 alone becomes inactive. Critically, wavelength‐resolved operando FT‐IR directly shows plasmon excitation selectively accelerates ring‐opening step providing clear evidence of plasmon‐driven regeneration processes. Collectively, these results provide direct mechanistic evidence that plasmonic excitation at the Au/TiO 2 interface sustains VOCs mineralization offering a generalizable strategy to design deactivation resilient photocatalysts for indoor air remediation.
室内暴露于挥发性有机化合物(VOCs)如乙醛和甲苯会造成主要的健康风险,但二氧化钛的光催化氧化受到湿度和污染物复杂性的强烈调节。在这里,我们揭示了乙醛和甲苯对tio2的不同湿度响应:干燥条件下乙醛降解改善,而甲苯去除需要潮湿环境以避免严重失活。这些不同的行为在混合VOCs饲料中被放大,其中甲苯失活抑制了整体矿化效率。值得注意的是,等离子体Au/ tio2催化剂具有抗湿性和耐用性,在相对湿度为25%-80%的情况下,对这两种挥发性有机化合物的去除效率均达到70%。光谱表征(XPS,拉曼,软XAS和硬XAS)表明,Au纳米颗粒与tio2建立了强电子相互作用,促进了界面电荷转移和增强ROS的产生,而原位EPR区分了•OH, O 2•−和h +的特定形成途径,表明等离子体激发即使在单独的tio2变得不活跃的情况下也能维持ROS活性。关键的是,波长分辨的operando FT - IR直接显示等离子激元激发选择性地加速开环步骤,为等离子激元驱动的再生过程提供了明确的证据。总的来说,这些结果提供了直接的机制证据,表明Au/ tio2界面的等离子体激发维持了VOCs的矿化,为设计用于室内空气修复的失活弹性光催化剂提供了一种通用策略。
{"title":"Plasmonic Enhancement Enables Deactivation Resilient TiO 2 for Sustainable VOCs Remediation under Practical Conditions","authors":"Gahye Shin, Subhash Chandra Shit, Min Seok Koo, Dong Jin Ham, Hyuk Jae Kwon, Hyunwoong Park, Wooyul Kim","doi":"10.1002/adfm.202526193","DOIUrl":"https://doi.org/10.1002/adfm.202526193","url":null,"abstract":"Indoor exposure to volatile organic compounds (VOCs) such as acetaldehyde and toluene poses major health risks, but photocatalytic oxidation over TiO <jats:sub>2</jats:sub> is strongly modulated by humidity and pollutant complexity. Here, we reveal contrasting humidity responses of acetaldehyde and toluene on TiO <jats:sub>2</jats:sub> : acetaldehyde degradation improves under dry conditions, whereas toluene removal requires humid environments to avoid severe deactivation. These divergent behaviors are amplified under mixed‐VOCs feeds, where toluene deactivation suppresses overall mineralization efficiency. Remarkably, plasmonic Au/TiO <jats:sub>2</jats:sub> catalysts exhibit humidity resilient and durable performance, maintaining >70% removal efficiency for both VOCs across RH 25%–80%. Spectroscopic characterizations (XPS, Raman, soft and hard XAS) demonstrate that Au nanoparticles establish strong electronic interactions with TiO <jats:sub>2</jats:sub> facilitating interfacial charge transfer and enhanced ROS generation, while in situ EPR distinguishes the specific formation pathways of <jats:sup>•</jats:sup> OH, O <jats:sub>2</jats:sub> <jats:sup>•−</jats:sup> , and h <jats:sup>+</jats:sup> , demonstrating that plasmonic excitation sustains ROS activity even under conditions where TiO <jats:sub>2</jats:sub> alone becomes inactive. Critically, wavelength‐resolved operando FT‐IR directly shows plasmon excitation selectively accelerates ring‐opening step providing clear evidence of plasmon‐driven regeneration processes. Collectively, these results provide direct mechanistic evidence that plasmonic excitation at the Au/TiO <jats:sub>2</jats:sub> interface sustains VOCs mineralization offering a generalizable strategy to design deactivation resilient photocatalysts for indoor air remediation.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"29 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145955796","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}
Selective catalytic oxidation of NH3 is limited by a fundamental activity‐selectivity trade‐off: catalysts that accelerate low‐temperature turnover often promote NH 3 over‐oxidation to NO x and N 2 O at higher temperature. Here, we address this limitation with a bifunctional platinum‐copper catalyst that combines distinct intermetallic and oxide sites supported on γ‐Al 2 O 3 . The catalyst exhibits > 90% NH 3 conversion at 140°C and sustains > 80% N 2 selectivity up to 300°C. Atomic‐resolution microscopy and X‐ray absorption spectroscopy identify L1 0 ‐ordered PtCu intermetallic nanoparticles with Pt‐enriched surfaces, coexisting with CuO x clusters that host isolated Pt single atoms (Pt 1 CuO x ). DRIFTS analysis determines an internal selective catalytic reduction sequence that converts in situ formed NO x to N 2 on the Pt 1 CuO x . Meanwhile, the enhanced low‐temperature activity of the PtCu intermetallic nanoparticles was explained through DFT calculations and microkinetic modeling: electron‐enrichment of Pt by alloying with Cu lowers the upper d‐band edge (ε u ), which weakens *N adsorption and reduces the barrier of the rate‐determining step of N–N coupling. This work proposes a dual‐site design concept of intermetallic‐oxide hybrid catalysts, harnessing ε u engineering of intermetallic sites for activity control, with tandem conversion of in situ formed by‐products on oxide sites for N 2 selectivity control.
{"title":"Resolving the Activity–Selectivity Trade‐Off in NH 3 Oxidation with an Intermetallic‐Oxide Dual‐Site Catalyst","authors":"Jiaxing Li, William Orbell, Xinbo Li, Yifan Li, Yunpeng Long, Yarong Bai, Lin Chen, Chuan Gao, Liang Zhang, Junhua Li, Yue Peng","doi":"10.1002/adfm.202530020","DOIUrl":"https://doi.org/10.1002/adfm.202530020","url":null,"abstract":"Selective catalytic oxidation of NH3 is limited by a fundamental activity‐selectivity trade‐off: catalysts that accelerate low‐temperature turnover often promote NH <jats:sub>3</jats:sub> over‐oxidation to NO <jats:sub>x</jats:sub> and N <jats:sub>2</jats:sub> O at higher temperature. Here, we address this limitation with a bifunctional platinum‐copper catalyst that combines distinct intermetallic and oxide sites supported on γ‐Al <jats:sub>2</jats:sub> O <jats:sub>3</jats:sub> . The catalyst exhibits > 90% NH <jats:sub>3</jats:sub> conversion at 140°C and sustains > 80% N <jats:sub>2</jats:sub> selectivity up to 300°C. Atomic‐resolution microscopy and X‐ray absorption spectroscopy identify L1 <jats:sub>0</jats:sub> ‐ordered PtCu intermetallic nanoparticles with Pt‐enriched surfaces, coexisting with CuO <jats:sub>x</jats:sub> clusters that host isolated Pt single atoms (Pt <jats:sub>1</jats:sub> CuO <jats:sub>x</jats:sub> ). DRIFTS analysis determines an internal selective catalytic reduction sequence that converts in situ formed NO <jats:sub>x</jats:sub> to N <jats:sub>2</jats:sub> on the Pt <jats:sub>1</jats:sub> CuO <jats:sub>x</jats:sub> . Meanwhile, the enhanced low‐temperature activity of the PtCu intermetallic nanoparticles was explained through DFT calculations and microkinetic modeling: electron‐enrichment of Pt by alloying with Cu lowers the upper d‐band edge (ε <jats:sub>u</jats:sub> ), which weakens *N adsorption and reduces the barrier of the rate‐determining step of N–N coupling. This work proposes a dual‐site design concept of intermetallic‐oxide hybrid catalysts, harnessing ε <jats:sub>u</jats:sub> engineering of intermetallic sites for activity control, with tandem conversion of in situ formed by‐products on oxide sites for N <jats:sub>2</jats:sub> selectivity control.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"47 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145955790","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}
Zero‐valent iron (ZVI) has been extensively utilized for heavy metal sequestration. However, its limited spatiotemporal selectivity—defined as the ability to selectively remove coexisting metals at distinct locations and times—often leads to unbalanced reactivity and rapid passivation. Herein, we develop ZVI cointercalated with sulfur and aluminum (SA‐ZVI) to achieve the simultaneous and selective removal of Cr(VI) and complexed Cu(II). The rate constant ratio (R = kCu / kCr ) increases from 0.56 for ZVI to 1.33 for SA‐ZVI, demonstrating enhanced Cu(II) selectivity under Cr(VI) stress. Cross‐sectional FIB‐SEM imaging reveals spatially decoupled reactivity, with Cr predominantly enriched at the surface and Cu deposited in the core. Further correlation analysis shows that Cu immobilization is closely linked to sulfur‐enriched FeS x domains, while Cr removal correlates with Al‐modified adsorption sites. Depth‐resolved XPS analysis suggests that sulfur forms conductive FeS x domains, facilitating Cu(II) reduction, while aluminum promotes selective adsorption of Cr(VI) and mitigates Fe–Cr passivation. Finally, the Kirkendall effect and galvanic replacement induce Fe diffusion and inward Cu growth, leading to enhanced Cu enrichment within SA‐ZVI. This cointercalation‐driven interface engineering effectively balances reactivity with selectivity and provides a mechanistic framework for designing multifunctional iron‐based materials with programmable spatiotemporal selectivity for wastewater treatment and resource recovery.
零价铁(Zero - valent iron, ZVI)已被广泛应用于重金属的固存。然而,其有限的时空选择性(定义为在不同位置和时间选择性去除共存金属的能力)往往导致反应性不平衡和快速钝化。在此,我们开发了与硫和铝共插层的ZVI (SA‐ZVI),以实现同时和选择性去除Cr(VI)和络合Cu(II)。速率常数比(R = k Cu / k Cr)从ZVI的0.56增加到SA‐ZVI的1.33,表明在Cr(VI)胁迫下Cu(II)选择性增强。截面FIB - SEM成像显示空间去耦反应性,Cr主要富集在表面,Cu沉积在岩心。进一步的相关分析表明,Cu的固定化与富硫FeS x结构域密切相关,而Cr的去除与Al修饰的吸附位点相关。深度分辨XPS分析表明,硫形成导电的FeS x结构域,促进Cu(II)的还原,而铝促进Cr(VI)的选择性吸附并减轻Fe-Cr的钝化。最后,Kirkendall效应和电替换诱导Fe扩散和Cu向内生长,导致SA‐ZVI内Cu富集增强。这种共插层驱动的界面工程有效地平衡了反应性和选择性,并为设计具有可编程时空选择性的多功能铁基材料提供了一个机制框架,用于废水处理和资源回收。
{"title":"Cointercalation of Zero‐Valent Iron for Improving Spatiotemporal Selectivity toward Heavy Metals in Wastewater","authors":"Hua Liu, Zhen Li, Yuankui Sun, Ziwei Bao, Minyao Zhou, Jinxiang Li, Xiaohong Guan","doi":"10.1002/adfm.202528568","DOIUrl":"https://doi.org/10.1002/adfm.202528568","url":null,"abstract":"Zero‐valent iron (ZVI) has been extensively utilized for heavy metal sequestration. However, its limited spatiotemporal selectivity—defined as the ability to selectively remove coexisting metals at distinct locations and times—often leads to unbalanced reactivity and rapid passivation. Herein, we develop ZVI cointercalated with sulfur and aluminum (SA‐ZVI) to achieve the simultaneous and selective removal of Cr(VI) and complexed Cu(II). The rate constant ratio (R = <jats:italic>k</jats:italic> <jats:sub>Cu</jats:sub> / <jats:italic>k</jats:italic> <jats:sub>Cr</jats:sub> ) increases from 0.56 for ZVI to 1.33 for SA‐ZVI, demonstrating enhanced Cu(II) selectivity under Cr(VI) stress. Cross‐sectional FIB‐SEM imaging reveals spatially decoupled reactivity, with Cr predominantly enriched at the surface and Cu deposited in the core. Further correlation analysis shows that Cu immobilization is closely linked to sulfur‐enriched FeS <jats:sub>x</jats:sub> domains, while Cr removal correlates with Al‐modified adsorption sites. Depth‐resolved XPS analysis suggests that sulfur forms conductive FeS <jats:sub>x</jats:sub> domains, facilitating Cu(II) reduction, while aluminum promotes selective adsorption of Cr(VI) and mitigates Fe–Cr passivation. Finally, the Kirkendall effect and galvanic replacement induce Fe diffusion and inward Cu growth, leading to enhanced Cu enrichment within SA‐ZVI. This cointercalation‐driven interface engineering effectively balances reactivity with selectivity and provides a mechanistic framework for designing multifunctional iron‐based materials with programmable spatiotemporal selectivity for wastewater treatment and resource recovery.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"248 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145955759","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}
Vertical organic field-effect transistors (VOFETs) have garnered significant attention due to their inherently short-channel design, which facilitates high-frequency operation, low power consumption, and the capability to drive high current densities. However, the incompatibility between traditional source electrodes and solution-processed organic semiconductors severely limits large-scale integration and performance enhancement of VOFETs. In this study, we report a controllable solvent interface self-assembly strategy for fabricating ultra-thin, low-roughness graphene source electrodes. Based on the source electrodes and precise control of the molecular packing of the polymer semiconductor (PffBT4T-2OD), the resulting polymer-based VOFETs demonstrate competitive performance metrics, including a high on/off ratio of 3.4 × 106 and a current density of 63.2 mA cm−2, along with exceptional operational stability. Furthermore, devices with operating voltages as low as −1.5 V and channel lengths down-scaled to 37 nm have been realized. Importantly, large-area VOFET arrays with a device density of 3906 devices per cm2 have been successfully fabricated, laying the groundwork for high-density, low-power organic integrated circuits. This advancement provides a scalable manufacturing solution for flexible electronics and organic electronic system-on-chip applications.
垂直有机场效应晶体管(vofet)由于其固有的短通道设计而获得了极大的关注,这有利于高频工作,低功耗和驱动高电流密度的能力。然而,传统源电极与溶液处理有机半导体之间的不兼容性严重限制了vofet的大规模集成和性能提升。在这项研究中,我们报告了一种可控制的溶剂界面自组装策略,用于制造超薄、低粗糙度的石墨烯源电极。基于源电极和对聚合物半导体(PffBT4T-2OD)分子封装的精确控制,所得到的基于聚合物的vofet表现出具有竞争力的性能指标,包括3.4 × 106的高开/关比和63.2 mA cm−2的电流密度,以及出色的工作稳定性。此外,工作电压低至- 1.5 V,通道长度缩小至37 nm的器件已经实现。重要的是,器件密度为每平方厘米3906个器件的大面积VOFET阵列已经成功制造,为高密度、低功耗有机集成电路奠定了基础。这一进步为柔性电子和有机电子片上系统应用提供了可扩展的制造解决方案。
{"title":"Large-Area Self-Assembled Graphene Source Electrodes for High-Performance Vertical Organic Field-Effect Transistors and their Arrays","authors":"Fangcong Zhang, Shunhong Dong, Suyun Tian, Hangyuan Cui, Lingxiang Zhang, Changjin Wan, Huiting Fu, Qingdong Zheng","doi":"10.1002/adfm.202530029","DOIUrl":"https://doi.org/10.1002/adfm.202530029","url":null,"abstract":"Vertical organic field-effect transistors (VOFETs) have garnered significant attention due to their inherently short-channel design, which facilitates high-frequency operation, low power consumption, and the capability to drive high current densities. However, the incompatibility between traditional source electrodes and solution-processed organic semiconductors severely limits large-scale integration and performance enhancement of VOFETs. In this study, we report a controllable solvent interface self-assembly strategy for fabricating ultra-thin, low-roughness graphene source electrodes. Based on the source electrodes and precise control of the molecular packing of the polymer semiconductor (PffBT4T-2OD), the resulting polymer-based VOFETs demonstrate competitive performance metrics, including a high on/off ratio of 3.4 × 10<sup>6</sup> and a current density of 63.2 mA cm<sup>−2</sup>, along with exceptional operational stability. Furthermore, devices with operating voltages as low as −1.5 V and channel lengths down-scaled to 37 nm have been realized. Importantly, large-area VOFET arrays with a device density of 3906 devices per cm<sup>2</sup> have been successfully fabricated, laying the groundwork for high-density, low-power organic integrated circuits. This advancement provides a scalable manufacturing solution for flexible electronics and organic electronic system-on-chip applications.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"4 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2026-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145956236","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}