{"title":"Molecule-Induced Huge d-p Overlap Enhances Superexchange Interaction for Room-Temperature In-Plane Magnetism and Giant Magneto Band-Structure Effect in Ferromagnetic Clusterphene","authors":"Xiaofeng Liu, Yihang Bai, Weiduo Zhu, Zhao Liu, Zhao Chen, Pengfei Gao, Haidi Wang, Zhongjun Li, Bing Wang, Xingxing Li, Wei Hu, Jinlong Yang","doi":"10.1002/adfm.202414984","DOIUrl":"https://doi.org/10.1002/adfm.202414984","url":null,"abstract":"The discovery of 2D van der Waals XY ferromagnets is a vital task to access excellent topological spin textures, yet remains a longstanding challenge due to low critical temperatures (<i>T</i><sub>C</sub>) and weak in-plane magnetic anisotropy. Here, a novel 2D ferromagnetic clusterphene, (Cr<sub>3</sub>As<sub>2</sub>)<sub>2</sub>Cp<sub>3</sub> (Cp = cyclopentadienyl), by using Cr<sub>3</sub>As<sub>2</sub>Cp<sub>3</sub> cluster self-assembly with Cp as linker is proposed. Via first-principles calculations, it is demonstrated that an enhanced ferromagnetic superexchange interaction between the d orbital is achieved through a salient overlap onto the molecular frontier orbitals of the Cp ligand, producing a room-temperature <i>T</i><sub>C</sub>. The (Cr<sub>3</sub>As<sub>2</sub>)<sub>2</sub>Cp<sub>3</sub> clusterphene characterizes an ideal XY ferromagnet and a giant magneto band-structure (GMB) effect. Functional groups and element modifications are also introduced to effectively manipulate the magnetic anisotropy and the GMB effect. The results showcase that 2D magnetic cluster-assembled clusterphenes fuel a wide range of possibilities for exploring XY magnetism in reduced dimensions.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"33 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673712","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":"Organic Nitro Compounds for Batteries","authors":"Donghong Wang, Qiwang Shao, Xianjia Cao, Mengxuan Qin, Changyou Zhang, Lei Zhu, Shasha Wang, Qing Li, Dongming Liu, Chunyi Zhi","doi":"10.1002/adfm.202416000","DOIUrl":"https://doi.org/10.1002/adfm.202416000","url":null,"abstract":"High-performance energy storage technologies, with the representatives of rechargeable and redox flow batteries, are required due to the flying development of electrical gadgets and the increase in demand for sustainable energy supply. Nevertheless, most of these batteries are made of inorganic active materials with several critical deficiencies, preventing their further development. Organic nitro compounds (ONCs) are an appealing alternative in this context, providing the advantages of multi-electron redox processes and adjustable battery performance by structural modification. In this review, the utilization of ONCs as the electrode materials of batteries, interfacial layer materials for metal batteries, as well as redox shuttle additives is explored. The authors also go over material design issues, together with the corresponding electrochemical reaction mechanisms, and an overview of related viewpoints and future research directions to facilitate the advancement of this field is provided.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"57 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673683","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}
Zejing Wang, Shuai Wan, Chenjie Dai, Zhe Li, Zhongyang Li
{"title":"Direction-Decoupled Light-Emitting Metasurface via Guided-Photoluminescence Manipulation","authors":"Zejing Wang, Shuai Wan, Chenjie Dai, Zhe Li, Zhongyang Li","doi":"10.1002/adfm.202415823","DOIUrl":"https://doi.org/10.1002/adfm.202415823","url":null,"abstract":"On-demand manipulation of light emissions is crucial for a variety of practical applications, including bio-imaging and optical display, etc. Within this realm, the invention of metasurfaces provides powerful light–matter interaction capabilities for the control of multitudinous emission parameters. However, due to the omnidirectional, random, and incoherent nature of photoluminescence (PL) emission, the multiplexing modulation of PL remains a challenge and is rarely realized. Here, a direction-decoupled light-emitting metasurface (LEM) is originally demonstrated to display dual-channel independent incoherent-emission images based on guided-PL manipulation. Utilizing the wavevector differences of guided-PL between opposite pumping directions, the LEM is designed to enable selective unidirectional emission, thereby decoupling the directional freedom for PL multiplexing and realizing dual meta-display. Besides, the direction-multiplexed LEM can be integrated simultaneously with pumping-light holography for multi-dimensional meta-display. Such programmable unidirectional emission manipulation and direction-multiplexed PL meta-display approaches promise light-emitting techniques and can potentially find applications in multiplexing display, optical storage and encryption, etc.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"99 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673707","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}
Jun Ren, Qian Xiang, Chunming Yang, Sufang Yang, Yun Liang, Jinlong Liu, Junhua Li, Dong Qian, Geoffrey I. N. Waterhouse
{"title":"Two Birds with One Stone: Self-Supporting Anodes and Cathodes for Quasi-Solid-State Asymmetric Supercapacitors via Reactions of 2-Thiobarbituric Acid with Fe and Co Foams","authors":"Jun Ren, Qian Xiang, Chunming Yang, Sufang Yang, Yun Liang, Jinlong Liu, Junhua Li, Dong Qian, Geoffrey I. N. Waterhouse","doi":"10.1002/adfm.202416506","DOIUrl":"https://doi.org/10.1002/adfm.202416506","url":null,"abstract":"Advanced electrode materials with simple manufacturing processes and wide voltage windows are needed for the commercialization of high energy density supercapacitors. Herein, a facile method is presented for fabricating self-supporting anodes and cathodes for quasi-solid-state asymmetric supercapacitors (QASCs) by hydrothermally reacting 2-thiobarbituric acid (TBA) with Fe foam (IF) and Co foam (CF), yielding FeTBA<sub>4</sub>/FeOOH/IF and Co<sub>9</sub>S<sub>8</sub>/CF electrodes, respectively. Due to the perfect match between the two electrodes, the redox-active TBA ligands in FeTBA<sub>4</sub>, the 2D ultrathin nanosheet structure of FeTBA<sub>4</sub>/FeOOH/IF, and multiple pairs of reversible redox reactions for suppressing water splitting, the configured Co<sub>9</sub>S<sub>8</sub>/CF//FeTBA<sub>4</sub>/FeOOH/IF QASC device delivers outstanding performance. The device possesses a wide operating voltage window of 1.6 V, leading to a high energy density of 82.64 Wh kg<sup>−1</sup> at 486.38 W kg<sup>−1</sup> and an equally impressive 35.36 Wh kg<sup>−1</sup> at 4595.92 W kg<sup>−1</sup>. Furthermore, a 98.5% capacitance retention is realized after 10000 charging–discharging cycles. Impressively, density functional theory (DFT) calculations reveal the unique pseudocapacitive reactions on the surface of Co<sub>9</sub>S<sub>8</sub>/CF and FeTBA<sub>4</sub>/FeOOH/IF electrodes. Importantly, this work guides the development of high-energy-density supercapacitors via the matching of electrodes and the use of redox-active complex electrodes.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"11 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673680","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}
Bin Zhu, Jiayu Wu, Desheng Liu, Yuke Yan, Xingxing Yang, Yixian Wang, Changcheng Bai, Danli Hu, Zhixing Zhang, Pan Jiang, Xiaolong Wang
{"title":"Sculpting Mechanical Properties of Hydrogels by Patterning Seamlessly Interlocked Stiff Skeleton","authors":"Bin Zhu, Jiayu Wu, Desheng Liu, Yuke Yan, Xingxing Yang, Yixian Wang, Changcheng Bai, Danli Hu, Zhixing Zhang, Pan Jiang, Xiaolong Wang","doi":"10.1002/adfm.202417477","DOIUrl":"https://doi.org/10.1002/adfm.202417477","url":null,"abstract":"Functional soft materials, especially hydrogels have been widely developed to achieve various soft structures and machines. However, synthetic hydrogels commonly show formula-dependent mechanical properties to fulfill the requirements of mechanical elasticity, stiffness, toughness, and tearing-resistance for adapting to complex application scenario. Inspired by heterostructures and materials found in nature such as leaves and insect wings, a sequential photopolymerization process combined with site-selective patterning exposure is reported to prepare programmable hydrogels with locally heterogeneous reinforcement skeletons, i.e., interpenetrating double networks. The heterogeneous interface between soft matrices and stiff skeletons is seamlessly interlocked through strong multiple hydrogen bonds induced by phase transition. By harnessing the size, shape, and distribution of the patterned stiff skeletons, a wide range of mechanical properties of hydrogels including modulus (0.32–5.92 MPa), toughness (0.15–18 kJ m<sup>−2</sup>), dissipated energy (1–100 kJ m<sup>−3</sup>), impact resistance, and mechanical anisotropy can be readily sculpted within one material system without needing design and optimization of the complex and elusive material formulation on demand. It is believed that this simple yet powerful method relying on heterogenous patterning would guide the development of functional hydrogel materials with programmable mechanical properties toward potential engineering applications, such as damping and flexible circuits.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"8 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673713","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}
Shucheng Guo, Xue Bai, Boqun Liang, Thomas Hoke, Ming Liu, Rafal E. Dunin-Borkowski, Xi Chen
{"title":"Achieving Large and Anisotropic Spin-Mediated Thermal Transport in Textured Quantum Magnets","authors":"Shucheng Guo, Xue Bai, Boqun Liang, Thomas Hoke, Ming Liu, Rafal E. Dunin-Borkowski, Xi Chen","doi":"10.1002/adfm.202417505","DOIUrl":"https://doi.org/10.1002/adfm.202417505","url":null,"abstract":"Spin excitations, including magnons and spinons, can carry thermal energy and spin information. Studying spin-mediated thermal transport is crucial for spin caloritronics, enabling efficient heat dissipation in microelectronics and advanced thermoelectric applications. However, designing quantum materials with controllable spin transport is challenging. Here, highly textured spin-chain compound Ca<sub>2</sub>CuO<sub>3</sub> is synthesized using a solvent-cast cold pressing technique, aligning 2D nanostructures with spin chains perpendicular to the pressing direction. The sample exhibits high thermal conductivity anisotropy and an excellent room-temperature thermal conductivity of 12 ± 0.7 W m<sup>−1</sup> K<sup>−1</sup>, surpassing all polycrystalline quantum magnets. Such a high value is attributed to the significant spin-mediated thermal conductivity of 10 ± 1 W m<sup>−1</sup> K<sup>−1</sup>, the highest reported among all polycrystalline quantum materials. Analysis through a 1D kinetic model suggests that near room-temperature, spinon thermal transport is dominated by coupling with high-frequency phonons, while extrinsic spinon-defect scattering is negligible. Additionally, this method is used to prepare textured La<sub>2</sub>CuO<sub>4</sub>, exhibiting highly anisotropic magnon thermal transport and demonstrating its broad applicability. A distinct role of defect scattering in spin-mediated thermal transport is observed in two spin systems. These findings open new avenues for designing quantum materials with controlled spin transport for thermal management and energy conversion.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"157 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673674","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}
Dedong He, Yimin Zhang, Tan Li, Dingkai Chen, Hao Wang, Lei Zhang, Jiangping Liu, Xiaohua Cao, Jichang Lu, Yongming Luo
{"title":"Designing Ultra-Stable and Surface-Exposed Ni Nanoparticles with Dually Confined Microenvironment for High-Temperature Methane Dry Reforming","authors":"Dedong He, Yimin Zhang, Tan Li, Dingkai Chen, Hao Wang, Lei Zhang, Jiangping Liu, Xiaohua Cao, Jichang Lu, Yongming Luo","doi":"10.1002/adfm.202412895","DOIUrl":"https://doi.org/10.1002/adfm.202412895","url":null,"abstract":"Conversion of CO<sub>2</sub> and CH<sub>4</sub> into syngas offers a promising route to reduce emissions of greenhouse gases, which facilitates large-scale carbon fixation and boosts carbon-neutral goal. The main obstacle for CO<sub>2</sub>/CH<sub>4</sub> reforming is the lack of durable catalysts showing both high metal-exposure and high-temperature structure stability, since the reported Ni-based catalysts have difficulty in avoiding deactivation by sintering metal at high temperature. Herein, ultra-small Ni nanoparticles, which display multiple characteristics of high surface-exposure and stabilized structure, are constructed from the evolution of atomically dispersed low-valent nickel under a dually confined microenvironment. Consequently, the developed strategy can not only break the stable-exposure trade-off in heterogeneous catalysis but also provide new opportunity for the engineering of high-performance and sintering-resistant reforming catalysts as well as other durable heterogeneous catalysts.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"1 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673709","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}
Lu Gao, Xia Liu, Lei Li, Nanping Deng, Weimin Kang, Bowen Cheng
{"title":"Commonalities and Characteristics Analysis of Fluorine and Iodine used in Lithium-Based Batteries","authors":"Lu Gao, Xia Liu, Lei Li, Nanping Deng, Weimin Kang, Bowen Cheng","doi":"10.1002/adfm.202413888","DOIUrl":"https://doi.org/10.1002/adfm.202413888","url":null,"abstract":"Among optimization strategies for solving the poor ion transport ability and electrolyte/electrode interface compatibility problems of lithium (Li)-based batteries, halogen elements, such as fluorine (F) and iodine (I), have gradually occupied an important position because of their superb electronegativity, oxidizability, ionic radius, and other properties. The study commences by outlining the shared mechanism by which F and I enhance solid-state lithium metal batteries' electrochemical performance. In particular, F and I can considerably improve ion transport capacity through chemical means such as intermolecular interactions and halogenation reactions. Furthermore, the utilization of F and I significantly enhances the stability of the electrolyte/electrode interface via physical strategies, encompassing doping techniques, the application of surface coatings, and the fabrication of synthetic intermediate layers. Subsequently, the characteristics of F and I used in Li-based batteries are elaborated in detail, focusing on the fact that F can provide additional energy density as an anode material but by different mechanisms. Additionally, I can considerably activate dead lithium at the negative electrode, and F can act as a new carrier. Finally, a rational concept of the synergistic effect of F and I is proposed and the feasibility of F–I bihalide solid electrolytes is explored.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"57 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673710","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}
Yanbai Chen, Xufeng Wan, Yan Yue, Shuai He, Jian Cao, Wenxuan He, Tailee Toctocan Tai, Duan Wang, Zongke Zhou, Yi Deng
{"title":"Low-Intensity Ultrasound-Activated Cavitation Effect Triggers Piezoelectric Catalysis Coordinating Respiratory Chain Interference Tactics Against Bacterial Infection","authors":"Yanbai Chen, Xufeng Wan, Yan Yue, Shuai He, Jian Cao, Wenxuan He, Tailee Toctocan Tai, Duan Wang, Zongke Zhou, Yi Deng","doi":"10.1002/adfm.202419426","DOIUrl":"https://doi.org/10.1002/adfm.202419426","url":null,"abstract":"Piezocatalytic therapy has aroused considerable attention in the treatment of bacterial infection due to its noninvasive and deep tissue penetration capabilities. The catalytic efficiency, however, is significantly constrained by the insufficient piezoresponse of sonosensitizers at low-intensity ultrasound (LIU) accompanied poor separation efficiency of charges, resulting in unsatisfactory sterilization. To address the dilemma, a piezocatalytic bio-heterojunction (P-bioHJ) consisting of BiOI and few-layered Mxene is constructed for rapid antibacterial. The engineered P-bioHJ not merely possesses a relatively narrow-bandgap for responding to the sonoluminescence emitted by the sonocavitation effect, but rather induces the interfacial polarization and the generation of oxygen vacancies to facilitate the effective separation of carriers, leading to a burst of radicals for rapid sterilization. Transcriptomic analysis reveals that P-bioHJ instigates sterilization by interfering with bacterial electron transport chain, disrupting both metabolism and energy synthesis. In vitro experiments indicate excellent cytocompatibility of P-bioHJ. Furthermore, in vivo assays demonstrate that P-bioHJ exhibits outstanding antimicrobial properties in a cutaneous infection model with LIU, and promotes angiogenesis and osteogenesis in an infectious bone defect model by decorating with naringin. As envisaged, this work offers valuable insight to augment piezocatalytic therapy by harnessing sonocavitation effect, advancing the remediation of infected tissue regeneration.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"18 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670716","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":"Unlocking the Origin of High-Temperature Superconductivity in Molecular Hydrides at Moderate Pressures","authors":"Wendi Zhao, Austin Ellis, Defang Duan, Hongwei Wang, Qiwen Jiang, Mingyang Du, Tian Cui, Maosheng Miao","doi":"10.1002/adfm.202415910","DOIUrl":"https://doi.org/10.1002/adfm.202415910","url":null,"abstract":"The current pressing challenge in the field of superconducting hydride research is to lower the stable pressure of such materials for practical applications. Molecular hydrides are usually stable under moderate pressure, but the underlying metallization mechanism remains elusive. Here, the important role of chemical interactions in governing the structures and properties of molecular hydrides is demonstrated. A new mechanism is proposed for obtaining high-temperature and even room-temperature superconductivity in molecular hydrides and report that the ternary hydride NaKH<sub>12</sub> hosts <i>T</i><sub>c</sub> values up to 245 K at moderate pressure of 60 GPa. Both the excellent stability and superconductivity of NaKH<sub>12</sub> originate from the fact that the localized electrons in the interstitial region of the metal lattice occupying the crystal orbitals well matched with the hydrogen lattice and forming chemical templates to assist the assembly of H<sub>2</sub> units. These localized electrons weaken the H─H covalent bonds and improve the charge connectivity between the H<sub>2</sub> units, ensuring the strong coupling between electrons and hydrogen-dominated optical phonons. The theory provides a key perspective for understanding the superconductivity of molecular hydrides with various structural motifs, opening the door to obtaining high-temperature superconductors from molecular hydrides at moderate pressures.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"31 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665345","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}