Ying Yang, Xuebo Cao, Lin Huang, Quankun Li, Li Gu, Zheng Yan, Mengli Li, Ruobin Cheng, Zhufeng Lu, Ai-Jun Wang, Wenchao Yang
Electrochemical oxidization of crude ethylene glycol (EG) to fine chemicals driven by sustainable energy is an eco-friendly solution to the upcycling of end-of-life polyethylene terephthalate (PET) wastes. Here, pseudo Agx-PtyPdz core–shell electrocatalyst capable of hybrid oxidation of EG to formate (FA) is designed and synthesized. The trimetallic system consists of Ag nanowire and ultrathin PtPd alloy skin with defects, such as holes and grooves. The defects expose the Ag core to the surroundings and convert Ag0 to Ag2+ active species at appropriate potential (> 1.2 V vs RHE). Thus, hybrid EG oxidization reaction is realized on the Agx-PtyPdz electrocatalyst, where PtPd skin catalyzes EG oxidization through conventional Faradaic electrode process owing to inherent activities of Pt and Pd, while Ag2+ serves as auxiliar oxidant to oxidize EG/intermediates (non-Faradaic reaction). Such a hybrid oxidization strategy reinforces the removal of adsorbates on Agx-PtyPdz electrocatalyst and refresh the active sites timely. Eventually, ultrahigh specific activity (24.45 A mg−1PtPd) and long-term stability (> 3000 h at current density ≥ 400 mA cm−2) are delivered by the system. The finding of Ag2+-enhanced alcohol oxidization reactions introduces a new paradigm for designing high-performance electrocatalysts for energy and environmental applications.
在可持续能源的驱动下，将粗乙二醇（EG）电化学氧化为精细化学品，是对报废聚对苯二甲酸乙二醇酯（PET）废料进行再循环利用的一种生态友好型解决方案。本文设计并合成了能够将 EG 混合氧化为甲酸盐（FA）的假 Agx-PtyPdz 核壳电催化剂。该三金属体系由银纳米线和带有孔和凹槽等缺陷的超薄铂钯合金表皮组成。这些缺陷使银核暴露在周围环境中，并在适当的电位（1.2 V vs RHE）下将 Ag0 转化为 Ag2+ 活性物种。因此，在 Agx-PtyPdz 电催化剂上实现了 EG 混合氧化反应，其中 PtPd 表皮由于铂和钯的固有活性，通过传统的法拉第电极过程催化 EG 氧化，而 Ag2+ 作为辅助氧化剂氧化 EG/中间体（非法拉第反应）。这种混合氧化策略加强了 Agx-PtyPdz 电催化剂上吸附剂的清除，并及时刷新了活性位点。最终，该系统实现了超高比活度（24.45 A mg-1PtPd ）和长期稳定性（电流密度≥ 400 mA cm-2 时为 3000 h）。Ag2+ 增强醇氧化反应的发现为设计能源和环境应用领域的高性能电催化剂引入了新的范式。
{"title":"Hybrid Oxidization of Ethylene Glycol on Defective Ag-PtPd Electrocatalyst Beyond 3000 h Stability at an Industrial-Scale Current Density","authors":"Ying Yang, Xuebo Cao, Lin Huang, Quankun Li, Li Gu, Zheng Yan, Mengli Li, Ruobin Cheng, Zhufeng Lu, Ai-Jun Wang, Wenchao Yang","doi":"10.1002/adfm.202418588","DOIUrl":"https://doi.org/10.1002/adfm.202418588","url":null,"abstract":"Electrochemical oxidization of crude ethylene glycol (EG) to fine chemicals driven by sustainable energy is an eco-friendly solution to the upcycling of end-of-life polyethylene terephthalate (PET) wastes. Here, pseudo Ag<i><sub>x</sub></i>-Pt<i><sub>y</sub></i>Pd<i><sub>z</sub></i> core–shell electrocatalyst capable of hybrid oxidation of EG to formate (FA) is designed and synthesized. The trimetallic system consists of Ag nanowire and ultrathin PtPd alloy skin with defects, such as holes and grooves. The defects expose the Ag core to the surroundings and convert Ag<sup>0</sup> to Ag<sup>2+</sup> active species at appropriate potential (> 1.2 V vs RHE). Thus, hybrid EG oxidization reaction is realized on the Ag<i><sub>x</sub></i>-Pt<i><sub>y</sub></i>Pd<i><sub>z</sub></i> electrocatalyst, where PtPd skin catalyzes EG oxidization through conventional Faradaic electrode process owing to inherent activities of Pt and Pd, while Ag<sup>2+</sup> serves as auxiliar oxidant to oxidize EG/intermediates (non-Faradaic reaction). Such a hybrid oxidization strategy reinforces the removal of adsorbates on Ag<i><sub>x</sub></i>-Pt<i><sub>y</sub></i>Pd<i><sub>z</sub></i> electrocatalyst and refresh the active sites timely. Eventually, ultrahigh specific activity (24.45 A mg<sup>−1</sup><sub>PtPd</sub>) and long-term stability (> 3000 h at current density ≥ 400 mA cm<sup>−2</sup>) are delivered by the system. The finding of Ag<sup>2+</sup>-enhanced alcohol oxidization reactions introduces a new paradigm for designing high-performance electrocatalysts for energy and environmental applications.","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":"142678452","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}
Metal halide perovskites are widely employed in photodetectors (PDs) due to their exceptional photoelectric conversion ability. However, the high dark current induced by defect states during perovskite crystallization has not been well resolved, which enormously deteriorates the sensitivity of PD. Herein, a vacuum-assisted template-confined growth method is proposed to successfully fabricate high-quality single crystal perovskite microwire arrays with low defect states and superior photoelectric characteristics. Experimentally and theoretically, it is proved that the fabricated perovskite microwire arrays PDs exhibit superior performance with commendable responsivity of 0.49 A W−1 and detectivity surpassing 1.21 × 1013 Jones, which profits from ultralow dark current of ≈200 fA at a 5 V bias. Particularly, the perovskite microwire arrays PD behaves the characteristics of flexible robust stability and high-definition image recognition. This work provides a universal strategy for optimizing perovskite crystal quality and constructing high-performance optoelectronic devices in many scenarios.
金属卤化物包晶因其卓越的光电转换能力而被广泛应用于光电探测器（PD）中。然而，目前还没有很好地解决过氧化物晶体在结晶过程中由缺陷态引起的高暗电流问题，这极大地降低了光电探测器的灵敏度。本文提出了一种真空辅助模板约束生长方法，成功制备了具有低缺陷态和优异光电特性的高质量单晶包晶微线阵列。实验和理论证明，所制备的过氧化物微丝阵列 PD 具有优异的性能，在 5 V 偏置下，其响应率达到 0.49 A W-1，探测率超过 1.21 × 1013 Jones，暗电流≈200 fA。特别是，包晶微线阵列 PD 具有灵活、坚固、稳定和高清图像识别的特点。这项工作为优化包晶晶体质量和在多种应用场景下构建高性能光电器件提供了一种通用策略。
{"title":"Vacuum-Assisted Growth of Single Crystal Perovskite Arrays toward Ultralow Dark Current Photodetectors","authors":"Suicai Zhang, Yalong Ge, Xuan Qin, Xuekai Wang, Tian Tao, Leiming Yu, Xiaohui Song, Yurong Jiang, Congxin Xia","doi":"10.1002/adfm.202418968","DOIUrl":"https://doi.org/10.1002/adfm.202418968","url":null,"abstract":"Metal halide perovskites are widely employed in photodetectors (PDs) due to their exceptional photoelectric conversion ability. However, the high dark current induced by defect states during perovskite crystallization has not been well resolved, which enormously deteriorates the sensitivity of PD. Herein, a vacuum-assisted template-confined growth method is proposed to successfully fabricate high-quality single crystal perovskite microwire arrays with low defect states and superior photoelectric characteristics. Experimentally and theoretically, it is proved that the fabricated perovskite microwire arrays PDs exhibit superior performance with commendable responsivity of 0.49 A W<sup>−1</sup> and detectivity surpassing 1.21 × 10<sup>13</sup> Jones, which profits from ultralow dark current of ≈200 fA at a 5 V bias. Particularly, the perovskite microwire arrays PD behaves the characteristics of flexible robust stability and high-definition image recognition. This work provides a universal strategy for optimizing perovskite crystal quality and constructing high-performance optoelectronic devices in many scenarios.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"51 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678407","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}
Low initial coulombic efficiency (ICE) and poor cycling performance are the pain points that hinder the commercialization of silicon monoxide (SiO) anode materials. Unfortunately, disproportionation commonly used to enhance cycling performance significantly reduces prelithiation efficiency, making it difficult to achieve both high-ICE and long-cycle-life SiO anodes. Herein, the intrinsic contradiction between disproportionation and prelithiation is successfully reconciled through the ingenious application of the carbon coating strategy, achieving a synergistic enhancement among the three processes (carbon coating, disproportionation, and prelithiation). The prepared SiO anode exhibits excellent electrochemical performance with an ICE as high as 113.74% and a reversible capacity of 713.68 mAh g−1 after 750 cycles. In-depth investigations reveal that carbon optimizes the distribution of Si and O within the disproportionated SiO, effectively thinning the SiO2 surface layer and releasing the shielded Si, thereby enhancing reversible capacity and prelithiation efficiency. TG-FTIR analysis further elucidates the underlying mechanism, demonstrating that the carbon effectively inhibits the outward migration and escape of O during disproportionation. In summary, this study uncovers the pivotal role of carbon coating in regulating the disproportionation behavior, promoting efficient prelithiation, and enhancing the capacity recovery of SiO.
初始库仑效率（ICE）低和循环性能差是阻碍一氧化硅（SiO）阳极材料商业化的痛点。遗憾的是，为提高循环性能而常用的歧化技术会显著降低预锂化效率，从而难以实现高ICE和长循环寿命的氧化硅阳极。在本文中，通过碳涂层策略的巧妙应用，成功地调和了歧化和预硫化之间的内在矛盾，实现了三种工艺（碳涂层、歧化和预硫化）的协同增强。所制备的氧化硅阳极具有优异的电化学性能，ICE 高达 113.74%，循环 750 次后的可逆容量为 713.68 mAh g-1。深入研究发现，碳优化了硅和氧在不成比例的氧化硅中的分布，有效地减薄了二氧化硅表层，释放了屏蔽硅，从而提高了可逆容量和预升辉效率。TG-FTIR 分析进一步阐明了其基本机制，表明碳在歧化过程中有效地抑制了 O 的向外迁移和逸出。总之，这项研究揭示了碳涂层在调节歧化行为、促进高效预硫化和提高氧化硅容量恢复方面的关键作用。
{"title":"Unveiling the Oxygen Migration Retarding Effort of Carbon Coating During Disproportionation Enabling High-ICE and Long-Cycle-Life SiO Anodes","authors":"Ruoyang Wang, Yuqing Wu, Qing Yang, Haoyu Li, Fang Wan, Ting Chen, Tingru Chen, Benhe Zhong, Zhenguo Wu, Xiaodong Guo","doi":"10.1002/adfm.202416392","DOIUrl":"https://doi.org/10.1002/adfm.202416392","url":null,"abstract":"Low initial coulombic efficiency (ICE) and poor cycling performance are the pain points that hinder the commercialization of silicon monoxide (SiO) anode materials. Unfortunately, disproportionation commonly used to enhance cycling performance significantly reduces prelithiation efficiency, making it difficult to achieve both high-ICE and long-cycle-life SiO anodes. Herein, the intrinsic contradiction between disproportionation and prelithiation is successfully reconciled through the ingenious application of the carbon coating strategy, achieving a synergistic enhancement among the three processes (carbon coating, disproportionation, and prelithiation). The prepared SiO anode exhibits excellent electrochemical performance with an ICE as high as 113.74% and a reversible capacity of 713.68 mAh g<sup>−1</sup> after 750 cycles. In-depth investigations reveal that carbon optimizes the distribution of Si and O within the disproportionated SiO, effectively thinning the SiO<sub>2</sub> surface layer and releasing the shielded Si, thereby enhancing reversible capacity and prelithiation efficiency. TG-FTIR analysis further elucidates the underlying mechanism, demonstrating that the carbon effectively inhibits the outward migration and escape of O during disproportionation. In summary, this study uncovers the pivotal role of carbon coating in regulating the disproportionation behavior, promoting efficient prelithiation, and enhancing the capacity recovery of SiO.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"230 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678411","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}
Anne S. Meeussen, Giovanni Bordiga, Audrey X. Chang, Ben Spoettling, Kaitlyn P. Becker, L. Mahadevan, Katia Bertoldi
Mechanical metamaterials—structures with unusual properties that emerge from their internal architecture—that are designed to undergo large deformations typically exploit large internal rotations, and therefore, necessitate the incorporation of flexible hinges. Kirigami structures, made by introducing ordered cuts in a planar material, are one such example. In the mechanism limit, these structures consist of rigid bodies connected by ideal hinges that deform at zero energy cost. However, fabrication in this limit has remained elusive. Here, we demonstrate that the integration of textile hinges provides a scalable platform for creating large kirigami metamaterials with mechanism-like behaviors. Further, leveraging recently introduced kinematic optimization tools, we show that textile hinges enable extreme shape-morphing responses, paving the way for the next generation of mechanism-based metamaterials.
{"title":"Textile Hinges Enable Extreme Properties of Kirigami Metamaterials","authors":"Anne S. Meeussen, Giovanni Bordiga, Audrey X. Chang, Ben Spoettling, Kaitlyn P. Becker, L. Mahadevan, Katia Bertoldi","doi":"10.1002/adfm.202415986","DOIUrl":"https://doi.org/10.1002/adfm.202415986","url":null,"abstract":"Mechanical metamaterials—structures with unusual properties that emerge from their internal architecture—that are designed to undergo large deformations typically exploit large internal rotations, and therefore, necessitate the incorporation of flexible hinges. Kirigami structures, made by introducing ordered cuts in a planar material, are one such example. In the mechanism limit, these structures consist of rigid bodies connected by ideal hinges that deform at zero energy cost. However, fabrication in this limit has remained elusive. Here, we demonstrate that the integration of textile hinges provides a scalable platform for creating large kirigami metamaterials with mechanism-like behaviors. Further, leveraging recently introduced kinematic optimization tools, we show that textile hinges enable extreme shape-morphing responses, paving the way for the next generation of mechanism-based metamaterials.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"74 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678861","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}
Pu-An Lin, Wenfeng Zhang, Yang Yang, Lang Yu, Yuan Yin, Ruihao Chen, Bing Cai, Jie Sun, Xiaojia Zheng, Yuelong Huang, Wen-Hua Zhang
Perovskite solar cells are among the most promising candidates for the next generation of photovoltaic technology. However, the heterogeneous nature of mixed halide perovskites as ionic crystals raises challenges to their photovoltaic performance and long-term stability. Herein, a functional molecule, named 2-amino-4-trifluoromethylpyridine (2A4TP), is introduced as an inhibitor of impurity phases in perovskite wet films, enabling the formation of optically active pure phase (α-phase) perovskites at room temperature. Meanwhile, reducing aggregation barrier for perovskite colloidal particles contribute to accelerate perovskite nucleation rate. Ultimately, the resulting uniform perovskite films afford to the optimized perovskite solar cells (0.09 cm2) exhibited a champion efficiency of 24.59% along with superior thermal and operational stability. Finally, 30x30 cm2 modules fabricated in this way delivers an impressive efficiency of 16.12% (with an aperture area of 655.2 cm2), demonstrating the large-area compatibility of the strategy.
{"title":"A Facile Strategy to Suppressing Impurity Phase in Perovskite Wet Films for Efficient and Stable Photovoltaics","authors":"Pu-An Lin, Wenfeng Zhang, Yang Yang, Lang Yu, Yuan Yin, Ruihao Chen, Bing Cai, Jie Sun, Xiaojia Zheng, Yuelong Huang, Wen-Hua Zhang","doi":"10.1002/adfm.202416582","DOIUrl":"https://doi.org/10.1002/adfm.202416582","url":null,"abstract":"Perovskite solar cells are among the most promising candidates for the next generation of photovoltaic technology. However, the heterogeneous nature of mixed halide perovskites as ionic crystals raises challenges to their photovoltaic performance and long-term stability. Herein, a functional molecule, named 2-amino-4-trifluoromethylpyridine (2A4TP), is introduced as an inhibitor of impurity phases in perovskite wet films, enabling the formation of optically active pure phase (α-phase) perovskites at room temperature. Meanwhile, reducing aggregation barrier for perovskite colloidal particles contribute to accelerate perovskite nucleation rate. Ultimately, the resulting uniform perovskite films afford to the optimized perovskite solar cells (0.09 cm<sup>2</sup>) exhibited a champion efficiency of 24.59% along with superior thermal and operational stability. Finally, 30x30 cm<sup>2</sup> modules fabricated in this way delivers an impressive efficiency of 16.12% (with an aperture area of 655.2 cm<sup>2</sup>), demonstrating the large-area compatibility of the strategy.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"19 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679133","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}
Rational design and optimization of the electrochemiluminescence (ECL) system undoubtedly underpins critical future advances in the field of sensing. Herein, an efficient ECL system is prepared by the integration of pyrene self-assembled hydrogen-bonded organic frameworks (PSA-HOF) and defective hydrated tungsten oxide nanosheets (dWO3H2), displaying a self-cycling photocatalytic activation mechanism to boost ECL performances. PSA-HOF was exploited as the ECL luminophor to produce a light source with sufficient intensity due to the unique structure and aggregation-induced emission-enhanced emission. Meanwhile, dWO3H2O exhibited dual functionality: 1) serving as highly efficient adsorbents for capturing peroxydisulfate (PDS), 2) acting as photoactive materials, which can be activated by the light emitted from PSA-HOF. Notably, the presence of oxygen vacancies within dWO3H2O can not only lowered adsorption energy and increase exposure of active sites, but also enhance the photocatalytic performance, thus activating PDS through a radical-mediated mechanism, which can further stimulate the photocatalytic materials in turn to achieve self-circulation within the system. As a proof of concept, an ECL biosensor for detecting microcystin-RR (MC-RR) is successfully established, which displays a wide detection range and a low detection limit. This work offers a new perspective on the development of ECL technology with high efficiency and stability.
{"title":"Self-Photocatalysis Boosted Electrochemiluminescence System of Pyrene Based Hydrogen-Bonded Organic Framework: Oxygen-Vacancy Mediated Adsorption and Peroxydisulfate Radical Activation","authors":"Ying Wang, Ding Jiang, Yuqing Bian, Xiaojiao Du, Xueling Shan, Wenchang Wang, Hiroshi Shiigi, Haijiao Xie, Zhidong Chen","doi":"10.1002/adfm.202417733","DOIUrl":"https://doi.org/10.1002/adfm.202417733","url":null,"abstract":"Rational design and optimization of the electrochemiluminescence (ECL) system undoubtedly underpins critical future advances in the field of sensing. Herein, an efficient ECL system is prepared by the integration of pyrene self-assembled hydrogen-bonded organic frameworks (PSA-HOF) and defective hydrated tungsten oxide nanosheets (dWO<sub>3</sub>H<sub>2</sub>), displaying a self-cycling photocatalytic activation mechanism to boost ECL performances. PSA-HOF was exploited as the ECL luminophor to produce a light source with sufficient intensity due to the unique structure and aggregation-induced emission-enhanced emission. Meanwhile, dWO<sub>3</sub>H<sub>2</sub>O exhibited dual functionality: 1) serving as highly efficient adsorbents for capturing peroxydisulfate (PDS), 2) acting as photoactive materials, which can be activated by the light emitted from PSA-HOF. Notably, the presence of oxygen vacancies within dWO<sub>3</sub>H<sub>2</sub>O can not only lowered adsorption energy and increase exposure of active sites, but also enhance the photocatalytic performance, thus activating PDS through a radical-mediated mechanism, which can further stimulate the photocatalytic materials in turn to achieve self-circulation within the system. As a proof of concept, an ECL biosensor for detecting microcystin-RR (MC-RR) is successfully established, which displays a wide detection range and a low detection limit. This work offers a new perspective on the development of ECL technology with high efficiency and stability.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"71 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679140","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
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 Ca2CuO3 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−1 K−1, surpassing all polycrystalline quantum magnets. Such a high value is attributed to the significant spin-mediated thermal conductivity of 10 ± 1 W m−1 K−1, 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 La2CuO4, 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.
自旋激发（包括磁子和自旋子）可以携带热能和自旋信息。研究自旋介导的热传输对自旋热电子学至关重要，它能在微电子学和先进热电应用中实现高效散热。然而，设计具有可控自旋传输的量子材料是一项挑战。本文采用溶剂浇铸冷压技术合成了高纹理自旋链化合物 Ca2CuO3，使二维纳米结构的自旋链垂直于压制方向。该样品具有很高的热导各向异性，室温热导率高达 12 ± 0.7 W m-1 K-1，超过了所有多晶量子磁体。之所以能达到如此高的热导率，是因为自旋介导的热导率高达 10 ± 1 W m-1 K-1，是所有多晶量子材料中最高的。通过一维动力学模型进行的分析表明，在接近室温时，自旋子的热传输主要是通过与高频声子的耦合来实现的，而外在的自旋子-缺陷散射可以忽略不计。此外，该方法还用于制备纹理化的 La2CuO4，表现出高度各向异性的磁子热传输，证明了其广泛的适用性。在两个自旋体系中观察到了缺陷散射在自旋介导的热传输中的独特作用。这些发现为设计具有热管理和能量转换可控自旋传输的量子材料开辟了新途径。
{"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
Conversion of CO2 and CH4 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 CO2/CH4 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.
将 CO2 和 CH4 转化为合成气为减少温室气体排放提供了一条前景广阔的途径，这有利于大规模碳固定并促进碳中和目标的实现。CO2/CH4 重整的主要障碍是缺乏具有高金属暴露和高温结构稳定性的耐用催化剂，因为已报道的镍基催化剂难以避免高温下金属烧结而失活。在本文中，超小型镍纳米颗粒是由原子分散的低价镍在双重限制的微环境下演化构建而成，具有高表面暴露和结构稳定的多重特性。因此，所开发的策略不仅能打破异相催化中稳定-暴露权衡的难题，还能为高性能、抗烧结重整催化剂以及其他耐用异相催化剂的工程化提供新的机遇。
{"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
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.
在解决锂（Li）基电池离子传输能力差和电解质/电极界面兼容性问题的优化策略中，卤素元素，如氟（F）和碘（I），因其超强的电负性、氧化性、离子半径等特性，逐渐占据了重要地位。本研究首先概述了 F 和 I 增强固态锂金属电池电化学性能的共同机制。特别是，F 和 I 可通过分子间相互作用和卤化反应等化学手段显著提高离子传输能力。此外，通过物理策略，包括掺杂技术、表面涂层的应用和合成中间层的制造，F 和 I 的使用可显著提高电解质/电极界面的稳定性。随后，详细阐述了锂基电池中使用的 F 和 I 的特性，重点是 F 作为阳极材料可以通过不同的机制提供额外的能量密度。此外，I 可以显著激活负极上的死锂，而 F 则可以充当新的载体。最后，提出了 F 和 I 协同效应的合理概念，并探讨了 F-I 双卤化物固体电解质的可行性。
{"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
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.
{"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}
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