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 NaKH12 hosts Tc values up to 245 K at moderate pressure of 60 GPa. Both the excellent stability and superconductivity of NaKH12 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 H2 units. These localized electrons weaken the H─H covalent bonds and improve the charge connectivity between the H2 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.
{"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}
Pengfei Xie, Xiao Rong, Xuelian Qin, Min Li, Yan Zuo, Bingjie Liu, Sujiao Cao, Jie Yang, Li Qiu
Ultrasound (US) becomes an appealing modality for stimulating or amplifying immune responses during cancer therapy, which is also termed sono-immunotherapy. However, the clinical prospect has not been fully realized due to the scarcity of efficient sonosensitizers. Herein, for the first time a novel Os-doped Au-tri(pyridin-4-yl) amine coordination structure (Os@Au-TPA)-based sonosensitizer is originally designed and synthesized for sono-immunotherapy of breast-metastasized tumors. Impressively, Os@Au-TPA shows much higher US-mediated 1O2-producing activity than Au-TPA as well as the other traditional sonosensitizers, for example, ≈41.6 folds to ce6, 19.5 times to Protoporphyrin IX (PpIX), 12.0 to Indocyanine Green (ICG), and 11.1 to Iron phthalocyanine (Pc(Fe)). The Os@Au-TPA can not only generate abundant ROS upon US irradiation to implement sonodynamic therapy (SDT), stimulating cell apoptosis and further immunogenic cell death, but can also generate O2 to alleviate hypoxia to promote the polarization of M2 to M1 macrophages to enhance tumor immunogenicity. As a result, when combined with PD-L1 antibody, it remodels the immunosuppressive tumor microenvironment, achieves concurrent sonodynamic-triggered immune activation, and eradicates both the original and distant-metastasized tumors efficiently. This work not only provides a new strategy to construct potent sonosensitizers from pyridine-metal coordination structures but also proves that sonosensitizers with high performance are crucial in boosting cancer sono-immunotherapy.
{"title":"A Highly Potent Os@Au-TPA Coordination Structure-Based Sonosensitizer for Tumor Sono-Immunotherapies","authors":"Pengfei Xie, Xiao Rong, Xuelian Qin, Min Li, Yan Zuo, Bingjie Liu, Sujiao Cao, Jie Yang, Li Qiu","doi":"10.1002/adfm.202412564","DOIUrl":"https://doi.org/10.1002/adfm.202412564","url":null,"abstract":"Ultrasound (US) becomes an appealing modality for stimulating or amplifying immune responses during cancer therapy, which is also termed sono-immunotherapy. However, the clinical prospect has not been fully realized due to the scarcity of efficient sonosensitizers. Herein, for the first time a novel Os-doped Au-tri(pyridin-4-yl) amine coordination structure (Os@Au-TPA)-based sonosensitizer is originally designed and synthesized for sono-immunotherapy of breast-metastasized tumors. Impressively, Os@Au-TPA shows much higher US-mediated <sup>1</sup>O<sub>2</sub>-producing activity than Au-TPA as well as the other traditional sonosensitizers, for example, ≈41.6 folds to ce6, 19.5 times to Protoporphyrin IX (PpIX), 12.0 to Indocyanine Green (ICG), and 11.1 to Iron phthalocyanine (Pc(Fe)). The Os@Au-TPA can not only generate abundant ROS upon US irradiation to implement sonodynamic therapy (SDT), stimulating cell apoptosis and further immunogenic cell death, but can also generate O<sub>2</sub> to alleviate hypoxia to promote the polarization of M2 to M1 macrophages to enhance tumor immunogenicity. As a result, when combined with PD-L1 antibody, it remodels the immunosuppressive tumor microenvironment, achieves concurrent sonodynamic-triggered immune activation, and eradicates both the original and distant-metastasized tumors efficiently. This work not only provides a new strategy to construct potent sonosensitizers from pyridine-metal coordination structures but also proves that sonosensitizers with high performance are crucial in boosting cancer sono-immunotherapy.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"99 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665387","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}
Chunyu Liu, Denghui Liu, Deli Li, Tong Wang, Di Liu, Xilin Mu, Jiasen Zhang, Tingting Feng, Kaibo Fang, Shi-Jian Su, Yubo Zhou, Siyao Wu, Wei Li, Ziyi Ge
The development of blue electroluminescent (EL) materials remains a significant challenge in organic light-emitting diode (OLED) technology. In this study, a novel design strategy is proposed for blue hot exciton (HE) materials, which involves utilizing a “cross” shaped molecular structure characterized by substantial steric hindrance and a highly twisted conformation. The unique cross-shaped molecular architecture with distinct “arms” enables flexible control over the excited state properties of the molecule, thereby facilitating precise modulation of high-lying triplet and low-lying singlet excited state energy levels. Furthermore, the 3D spatial configuration of the molecule effectively reduces close molecular packing, thereby minimizing the risk of material concentration quenching. The proof-of-concept HE emitters CN-PI and TP-PI exhibit non-π-π stacking configurations in single crystals, achieving high photoluminescence quantum yield (PLQY) values up to 51.3% and 46.5% in non-doped thin films, respectively, along with rapid radiation decay rates and reasonable distribution of Tm (m ≤ 5) and S1 states. Non-doped OLEDs incorporating these emitters demonstrate exceptional external quantum efficiencies (EQE), reaching 7.3% and 6.4%, respectively, while exhibiting minimal efficiency roll-off at high luminance. This research introduces a promising approach for developing high-performance blue HE emitters.
{"title":"Highly Efficient Blue Organic Light-Emitting Devices Based on “Cross”-Shaped Hot Exciton Emitters","authors":"Chunyu Liu, Denghui Liu, Deli Li, Tong Wang, Di Liu, Xilin Mu, Jiasen Zhang, Tingting Feng, Kaibo Fang, Shi-Jian Su, Yubo Zhou, Siyao Wu, Wei Li, Ziyi Ge","doi":"10.1002/adfm.202415633","DOIUrl":"https://doi.org/10.1002/adfm.202415633","url":null,"abstract":"The development of blue electroluminescent (EL) materials remains a significant challenge in organic light-emitting diode (OLED) technology. In this study, a novel design strategy is proposed for blue hot exciton (HE) materials, which involves utilizing a “cross” shaped molecular structure characterized by substantial steric hindrance and a highly twisted conformation. The unique cross-shaped molecular architecture with distinct “arms” enables flexible control over the excited state properties of the molecule, thereby facilitating precise modulation of high-lying triplet and low-lying singlet excited state energy levels. Furthermore, the 3D spatial configuration of the molecule effectively reduces close molecular packing, thereby minimizing the risk of material concentration quenching. The proof-of-concept HE emitters CN-PI and TP-PI exhibit non-π-π stacking configurations in single crystals, achieving high photoluminescence quantum yield (PLQY) values up to 51.3% and 46.5% in non-doped thin films, respectively, along with rapid radiation decay rates and reasonable distribution of T<sub>m</sub> (m ≤ 5) and S<sub>1</sub> states. Non-doped OLEDs incorporating these emitters demonstrate exceptional external quantum efficiencies (EQE), reaching 7.3% and 6.4%, respectively, while exhibiting minimal efficiency roll-off at high luminance. This research introduces a promising approach for developing high-performance blue HE emitters.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"248 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665343","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}
Huizhen Fan, Ka Ioi Wong, Yingying Ma, Ming Li, Hanqing Li, Li Wei, Shen Wang, Min Yao, Min Lu
Metal ion-based inhibition of urease activity is a promising strategy for treating Helicobacter pylori (H. pylori) infections. However, the challenges of safe delivery and reducing cytotoxicity persist. In this study, an innovative nanocarrier capable of acid-responsive release of Ag+ and antibiotics is developed, with complete degradation after treatment. Mesoporous organosilica nanoparticle (MON) is encapsulated with hyaluronic acid (HA) to prevent drug leakage and further coated with bacterial outer membrane vesicle (OMV) from Escherichia coli Nissle 1917, creating a nanocarrier with cell-protective capabilities. Ag+ and antibiotic clarithromycin (CLR) are incorporated into the nanocarrier to form CLR-Ag+@MON@HA@OMV (CAMO), designed for the targeted treatment of gastric H. pylori infection. The HA encapsulation ensures acid-responsive release of CLR and Ag+ in the stomach, preventing premature release at non-inflammatory sites. There is a potential for Ag⁺ in CAMO to replace Ni2⁺ at the active site of urease, enhancing the bactericidal effect of CLR through urease inhibition. Furthermore, the OMV provides additional cytoprotection, mitigating cell damage and inflammation response induced by the H. pylori infection. This study introduces a safe and effective nanocarrier that eradicates H. pylori and alleviates gastric inflammation.
{"title":"Biodegradable Acid-Responsive Nanocarrier for Enhanced Antibiotic Therapy Against Drug-Resistant Helicobacter Pylori via Urease Inhibition","authors":"Huizhen Fan, Ka Ioi Wong, Yingying Ma, Ming Li, Hanqing Li, Li Wei, Shen Wang, Min Yao, Min Lu","doi":"10.1002/adfm.202412893","DOIUrl":"https://doi.org/10.1002/adfm.202412893","url":null,"abstract":"Metal ion-based inhibition of urease activity is a promising strategy for treating <i>Helicobacter pylori</i> (<i>H. pylori</i>) infections. However, the challenges of safe delivery and reducing cytotoxicity persist. In this study, an innovative nanocarrier capable of acid-responsive release of Ag<sup>+</sup> and antibiotics is developed, with complete degradation after treatment. Mesoporous organosilica nanoparticle (MON) is encapsulated with hyaluronic acid (HA) to prevent drug leakage and further coated with bacterial outer membrane vesicle (OMV) from <i>Escherichia coli</i> Nissle 1917, creating a nanocarrier with cell-protective capabilities. Ag<sup>+</sup> and antibiotic clarithromycin (CLR) are incorporated into the nanocarrier to form CLR-Ag<sup>+</sup>@MON@HA@OMV (CAMO), designed for the targeted treatment of gastric <i>H. pylori</i> infection. The HA encapsulation ensures acid-responsive release of CLR and Ag<sup>+</sup> in the stomach, preventing premature release at non-inflammatory sites. There is a potential for Ag⁺ in CAMO to replace Ni<sup>2</sup>⁺ at the active site of urease, enhancing the bactericidal effect of CLR through urease inhibition. Furthermore, the OMV provides additional cytoprotection, mitigating cell damage and inflammation response induced by the <i>H. pylori</i> infection. This study introduces a safe and effective nanocarrier that eradicates <i>H. pylori</i> and alleviates gastric inflammation.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"48 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665388","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}
Youngsang Ko, Suji Lee, Jieun Jang, Goomin Kwon, Kangyun Lee, Youngho Jeon, Ajeong Lee, Teahoon Park, Jeonghun Kim, Jungmok You
Clean-water harvesting through solar interfacial evaporation technology has recently emerged as a strategy for resolving global water scarcity. In this study, rapid carbon-dioxide-laser-induced carbonization and facile ice-templating is employed to construct a cellulose-based solar evaporator bearing a hybrid multi-layer micro-/nano-architecture (i.e., a laser-induced carbon (LC) nanostructure and a cellulose aerogel (CA) nano/microstructure). The LC exhibits a light-absorbing/photothermal nanoporous carbon structure that offers high light absorption and multiple light scattering. Additionally, the CA exhibits numerous nanopores and unidirectional microchannels that facilitate rapid water transport via capillary action. This hybrid LC/CA micro-/nano-architecture enabled rapid vapor generation with an average water evaporation rate (ν) of 1.62 kg m−2 h−1 and an evaporation efficiency (η) of 66.6%. To further enhance the evaporation performance, a polydimethylsiloxane (PDMS) layer is coated onto the side of the LC/CA evaporator to increase its floatability in the simulated water; ν and η of the PDMS-coated LC/CA evaporator (LC/CA/PDMS) increased to 1.9 kg m−2 h−1 and 83.8%, respectively. Additionally, the LC/CA/PDMS evaporator exhibited a high ν value of 1.68 kg m−2 h−1 in simulated seawater, originating from excellent resistance to salt accumulation via its self-cleaning ability. Furthermore, the solar evaporator exhibited scalability for fabrication as well as biodegradable properties.
最近，通过太阳能界面蒸发技术收集清洁水源已成为解决全球水资源短缺问题的一种策略。在这项研究中，利用激光诱导的二氧化碳快速碳化和简便的铸冰技术，构建了一种纤维素基太阳能蒸发器，该蒸发器具有多层微/纳米混合结构（即激光诱导碳（LC）纳米结构和纤维素气凝胶（CA）纳米/微结构）。LC 具有光吸收/光热纳米多孔碳结构，具有高光吸收性和多重光散射性。此外，CA 具有大量纳米孔和单向微通道，可通过毛细作用促进水的快速传输。这种混合 LC/CA 微/纳米结构能够快速产生水蒸气，平均水蒸发率 (ν) 为 1.62 kg m-2 h-1，蒸发效率 (η) 为 66.6%。为了进一步提高蒸发性能，在 LC/CA 蒸发器的侧面涂上了一层聚二甲基硅氧烷 (PDMS)，以增加其在模拟水中的漂浮性；涂有 PDMS 的 LC/CA 蒸发器（LC/CA/PDMS）的 ν 和 η 分别增加到 1.9 kg m-2 h-1 和 83.8%。此外，LC/CA/PDMS 蒸发器在模拟海水中的 ν 值高达 1.68 kg m-2 h-1，这源于其出色的自清洁能力，可有效防止盐分积累。此外，太阳能蒸发器还具有可扩展性和可生物降解性。
{"title":"Nanocellulose-Based Interfacial Solar Evaporator: Integrating Sustainable Materials and Micro-/Nano-Architectures for Solar Desalination","authors":"Youngsang Ko, Suji Lee, Jieun Jang, Goomin Kwon, Kangyun Lee, Youngho Jeon, Ajeong Lee, Teahoon Park, Jeonghun Kim, Jungmok You","doi":"10.1002/adfm.202414576","DOIUrl":"https://doi.org/10.1002/adfm.202414576","url":null,"abstract":"Clean-water harvesting through solar interfacial evaporation technology has recently emerged as a strategy for resolving global water scarcity. In this study, rapid carbon-dioxide-laser-induced carbonization and facile ice-templating is employed to construct a cellulose-based solar evaporator bearing a hybrid multi-layer micro-/nano-architecture (i.e., a laser-induced carbon (LC) nanostructure and a cellulose aerogel (CA) nano/microstructure). The LC exhibits a light-absorbing/photothermal nanoporous carbon structure that offers high light absorption and multiple light scattering. Additionally, the CA exhibits numerous nanopores and unidirectional microchannels that facilitate rapid water transport via capillary action. This hybrid LC/CA micro-/nano-architecture enabled rapid vapor generation with an average water evaporation rate (ν) of 1.62 kg m<sup>−2</sup> h<sup>−1</sup> and an evaporation efficiency (η) of 66.6%. To further enhance the evaporation performance, a polydimethylsiloxane (PDMS) layer is coated onto the side of the LC/CA evaporator to increase its floatability in the simulated water; ν and η of the PDMS-coated LC/CA evaporator (LC/CA/PDMS) increased to 1.9 kg m<sup>−2</sup> h<sup>−1</sup> and 83.8%, respectively. Additionally, the LC/CA/PDMS evaporator exhibited a high ν value of 1.68 kg m<sup>−2</sup> h<sup>−1</sup> in simulated seawater, originating from excellent resistance to salt accumulation via its self-cleaning ability. Furthermore, the solar evaporator exhibited scalability for fabrication as well as biodegradable properties.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"13 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665573","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}
Tao Sun, Meng Qi, Qing-Xiu Li, Hang-Fei Li, Zhi-Peng Feng, Run-Ze Xu, You Zhou, Yu Wen, Gui-Jun Li, Ye Zhou, Su-Ting Han
Gait is among the most dependable, accurate, and secure methods of biometric identification. However, high power consumption and low computing capability are two major obstacles on wearable sensors-based gait recognition system. In this work, an integrated system is reported combining a triboelectric nanogenerator (TENG), a memristor (Ag/HfOx/Pt), and perovskite-based multicolor LEDs (PMCLED) for the visualization and recognition of foot patterns through signal-on-none and multi-wavelength on-device preprocessing. The flexible TENG acts as a sensory receptor, generating voltage based on the duration and intensity of pressure, which in turn promotes voltage-triggered synaptic plasticity in the memristor. The PMCLED, with its threshold switching and multi-wavelength emission characteristics, enables nonlinear filtering and amplification of the synaptic signal from the memristor, resulting in a simplified system design and reduced background noise. Additionally, the effectiveness of on-device preprocessing is validated based on a 5 × 5 array of integrated devices and software-built neural network for foot pattern visualization and recognition. The proposed system is able to recognize the on-device preprocessed images with high accuracy, indicating great potentials in both healthcare monitoring and human-machine interaction.
步态是最可靠、准确和安全的生物识别方法之一。然而，高功耗和低计算能力是基于可穿戴传感器的步态识别系统的两大障碍。在这项工作中，报告了一种集成系统，该系统结合了三电纳米发电机（TENG）、忆阻器（Ag/HfOx/Pt）和基于过氧化物的多色发光二极管（PMCLED），通过无信号和多波长设备预处理实现脚型的可视化和识别。柔性 TENG 可充当感觉受体，根据压力的持续时间和强度产生电压，进而促进忆阻器中电压触发的突触可塑性。PMCLED 具有阈值开关和多波长发射特性，能够对来自忆阻器的突触信号进行非线性过滤和放大，从而简化了系统设计并降低了背景噪声。此外，基于 5 × 5 集成器件阵列和用于脚型可视化和识别的软件内置神经网络，验证了器件上预处理的有效性。所提议的系统能够高精度地识别设备上预处理的图像，这表明该系统在医疗保健监测和人机交互方面具有巨大潜力。
{"title":"Integration of Sensory Memory Process Display System for Gait Recognition","authors":"Tao Sun, Meng Qi, Qing-Xiu Li, Hang-Fei Li, Zhi-Peng Feng, Run-Ze Xu, You Zhou, Yu Wen, Gui-Jun Li, Ye Zhou, Su-Ting Han","doi":"10.1002/adfm.202416619","DOIUrl":"https://doi.org/10.1002/adfm.202416619","url":null,"abstract":"Gait is among the most dependable, accurate, and secure methods of biometric identification. However, high power consumption and low computing capability are two major obstacles on wearable sensors-based gait recognition system. In this work, an integrated system is reported combining a triboelectric nanogenerator (TENG), a memristor (Ag/HfO<sub>x</sub>/Pt), and perovskite-based multicolor LEDs (PMCLED) for the visualization and recognition of foot patterns through signal-on-none and multi-wavelength on-device preprocessing. The flexible TENG acts as a sensory receptor, generating voltage based on the duration and intensity of pressure, which in turn promotes voltage-triggered synaptic plasticity in the memristor. The PMCLED, with its threshold switching and multi-wavelength emission characteristics, enables nonlinear filtering and amplification of the synaptic signal from the memristor, resulting in a simplified system design and reduced background noise. Additionally, the effectiveness of on-device preprocessing is validated based on a 5 × 5 array of integrated devices and software-built neural network for foot pattern visualization and recognition. The proposed system is able to recognize the on-device preprocessed images with high accuracy, indicating great potentials in both healthcare monitoring and human-machine interaction.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"13 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665574","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}
Stimuli-responsive materials have been applied for sensor devices because they can transform and amplify various target stimuli into observable signals. Much effort has been devoted to exploring effective molecular designs for obtaining stimuli-responsive behaviors by taking advantage of the unique optoelectronic properties of π-conjugated molecules involving various elements. This study focuses on the modulation of the electronic state of the π-conjugated scaffolds by the oxidation number change of the hypervalent antimony. This study demonstrate that the strength of the intramolecular interaction between hypervalent antimony and the π-conjugated framework can be tuned with ligand structure, substituent effect, and oxidation number shifts of hypervalent antimony. In particular, the color changes represented by hypsochromic and bathochromic wavelength shifts of optical bands are achieved by the oxidative reaction of hypervalent antimony in the solid state. Significantly, the direction of the color changes can be confidently predicted by quantum chemical calculations. The findings, based on the electronic interaction between π-conjugated scaffolds and hypervalent main-group elements, provide logical design strategies for advanced stimuli-responsive materials.
{"title":"Stimuli-Responsive Optical Materials Based on Hypervalent Antimony-Containing Conjugated Molecules","authors":"Kazuya Tanimura, Masayuki Gon, Kazuo Tanaka, Yoshiki Chujo","doi":"10.1002/adfm.202418600","DOIUrl":"https://doi.org/10.1002/adfm.202418600","url":null,"abstract":"Stimuli-responsive materials have been applied for sensor devices because they can transform and amplify various target stimuli into observable signals. Much effort has been devoted to exploring effective molecular designs for obtaining stimuli-responsive behaviors by taking advantage of the unique optoelectronic properties of π-conjugated molecules involving various elements. This study focuses on the modulation of the electronic state of the π-conjugated scaffolds by the oxidation number change of the hypervalent antimony. This study demonstrate that the strength of the intramolecular interaction between hypervalent antimony and the π-conjugated framework can be tuned with ligand structure, substituent effect, and oxidation number shifts of hypervalent antimony. In particular, the color changes represented by hypsochromic and bathochromic wavelength shifts of optical bands are achieved by the oxidative reaction of hypervalent antimony in the solid state. Significantly, the direction of the color changes can be confidently predicted by quantum chemical calculations. The findings, based on the electronic interaction between π-conjugated scaffolds and hypervalent main-group elements, provide logical design strategies for advanced stimuli-responsive materials.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"50 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665390","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}
Kun Yu, Huichao Ji, Guangli Ye, Liangjie Fu, Xiongbo Dong, Huaming Yang
Reactive oxygen species (ROS) have been growing as an emerging “hot” topic in antimicrobial applications. However, optimizing antimicrobial activity by enhancing ROS generation remains a formidable challenge. Here, using bassanite as a proof of concept, the facet engineering of bassanite matrix can enhance the ROS generation efficiency via tuning the d-band center of Cu atom is proposed. Theoretical calculation and experimental investigations reveal that the d-band center of Cu atoms is significantly shifted upward when Cu doped into the (204) facet of bassanite compared to the (400) facet. A higher d-band center facilitates adsorption and activation between Cu and O2 through the formation of stronger d-π* orbital hybridization, resulting in increased ROS production. Through engineering, the material exhibits better antimicrobial activity when Cu doped into the (204) facet, which presents a clear potential in construction materials and personal protection. This work shed light on designing new materials with high antimicrobial activity and the application of facet engineering.
活性氧（ROS）已逐渐成为抗菌应用中的一个新兴 "热门 "话题。然而，通过增强 ROS 生成来优化抗菌活性仍然是一项艰巨的挑战。在此，我们以巴桑石为概念验证，提出了通过调整铜原子的 d 波段中心来提高 ROS 生成效率的巴桑石基体刻面工程。理论计算和实验研究表明，与（400）面相比，当铜掺杂到巴山石的（204）面时，铜原子的 d 带中心会明显上移。更高的 d 带中心通过形成更强的 d-π* 轨道杂化，促进了 Cu 和 O2 之间的吸附和活化，从而增加了 ROS 的产生。通过工程设计，当 Cu 掺杂到 (204) 面时，该材料表现出更好的抗菌活性，在建筑材料和个人防护方面具有明显的潜力。这项工作为设计具有高抗菌活性的新材料以及面工程的应用提供了启示。
{"title":"Facet Engineering Modulates d-π* Hybridization for Boosting Antimicrobial Activity","authors":"Kun Yu, Huichao Ji, Guangli Ye, Liangjie Fu, Xiongbo Dong, Huaming Yang","doi":"10.1002/adfm.202418440","DOIUrl":"https://doi.org/10.1002/adfm.202418440","url":null,"abstract":"Reactive oxygen species (ROS) have been growing as an emerging “hot” topic in antimicrobial applications. However, optimizing antimicrobial activity by enhancing ROS generation remains a formidable challenge. Here, using bassanite as a proof of concept, the facet engineering of bassanite matrix can enhance the ROS generation efficiency via tuning the <i>d</i>-band center of Cu atom is proposed. Theoretical calculation and experimental investigations reveal that the <i>d</i>-band center of Cu atoms is significantly shifted upward when Cu doped into the (204) facet of bassanite compared to the (400) facet. A higher <i>d</i>-band center facilitates adsorption and activation between Cu and O<sub>2</sub> through the formation of stronger <i>d</i>-<i>π<sup>*</sup></i> orbital hybridization, resulting in increased ROS production. Through engineering, the material exhibits better antimicrobial activity when Cu doped into the (204) facet, which presents a clear potential in construction materials and personal protection. This work shed light on designing new materials with high antimicrobial activity and the application of facet engineering.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"18 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665391","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}
Wen Ye, Meng Li, Guixiang Li, Lihua Jiang, Shun Tian, Shihong Dong, Qingfeng Xu, Dongyun Chen, Mohammad Khaja Nazeeruddin, Paul J. Dyson, Antonio Abate, Jian-Mei Lu
Solution-processed lead-free halide perovskite gas sensors possess low gas detection limits, offering promising alternatives to traditional metal oxide chemiresistors. However, halide perovskite chemiresistors often suffer from poor selectivity and durability due to a lack of coordinatively unsaturated surface metal ions and their sensitivity to humidity. To address these issues, a general strategy is presented in which the Cs2PdBr6 perovskite surface is coated with covalent organic framework (COF) to provide hybrid sensor materials that are highly sensitive to specific gases and demonstrate excellent stability under real-working conditions. The hybrid chemiresistors demonstrate high sensitivity and controllable selectivity toward NO2 or NH3 gases. Specifically, TAPB–PDA@Cs2PdBr6 achieves a detection limit of 10 ppb for NO2, the lowest value reported for a perovskite-based gas sensor, maintaining its performance after continuous exposure to ambient air for several weeks. In contrast, COF-5@Cs2PdBr6 shows high selectivity to NH3 and has a detection limit of 40 ppb. Structural and spectroscopic characterization combined with mechanistic studies provide molecular-level insights into the outstanding properties of these new hybrid sensor materials, which set a new benchmark in the field, i.e., surpassing the selectivity and sensitivity of conventional halide perovskite sensors.
{"title":"Covalent Organic Framework-Enhanced Metal Halide Perovskites for Selective and Sensitive Gas Sensing","authors":"Wen Ye, Meng Li, Guixiang Li, Lihua Jiang, Shun Tian, Shihong Dong, Qingfeng Xu, Dongyun Chen, Mohammad Khaja Nazeeruddin, Paul J. Dyson, Antonio Abate, Jian-Mei Lu","doi":"10.1002/adfm.202418897","DOIUrl":"https://doi.org/10.1002/adfm.202418897","url":null,"abstract":"Solution-processed lead-free halide perovskite gas sensors possess low gas detection limits, offering promising alternatives to traditional metal oxide chemiresistors. However, halide perovskite chemiresistors often suffer from poor selectivity and durability due to a lack of coordinatively unsaturated surface metal ions and their sensitivity to humidity. To address these issues, a general strategy is presented in which the Cs<sub>2</sub>PdBr<sub>6</sub> perovskite surface is coated with covalent organic framework (COF) to provide hybrid sensor materials that are highly sensitive to specific gases and demonstrate excellent stability under real-working conditions. The hybrid chemiresistors demonstrate high sensitivity and controllable selectivity toward NO<sub>2</sub> or NH<sub>3</sub> gases. Specifically, TAPB–PDA@Cs<sub>2</sub>PdBr<sub>6</sub> achieves a detection limit of 10 ppb for NO<sub>2</sub>, the lowest value reported for a perovskite-based gas sensor, maintaining its performance after continuous exposure to ambient air for several weeks. In contrast, COF-5@Cs<sub>2</sub>PdBr<sub>6</sub> shows high selectivity to NH<sub>3</sub> and has a detection limit of 40 ppb. Structural and spectroscopic characterization combined with mechanistic studies provide molecular-level insights into the outstanding properties of these new hybrid sensor materials, which set a new benchmark in the field, i.e., surpassing the selectivity and sensitivity of conventional halide perovskite sensors.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"21 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665389","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}
Yuhong Cui, Guoliang Ru, Tianyi Zhang, Ke Yang, Shujuan Liu, Weihong Qi, Qian Ye, Xuqing Liu, Feng Zhou
With the rapid advancement of wearable electronics, soft robotics, and camouflage technologies, there is an urgent demand for flexible, multifunctional electromagnetic wave absorbing materials. Traditional absorbers, including metal- and carbon-based materials, often lack the flexibility required for such applications. In this work, a novel strategy is proposed for developing a flexible absorber by combining a conductive filler with a Schottky heterogeneous interface and a polymer network framework. Ti3C2Tx MXene is modified with ZnS via a low-temperature hydrothermal method, forming a Ti3C2Tx/ZnS composite. This composite is subsequently embedded in a copolymer matrix of polyvinyl alcohol (PVA) and acrylamide (AAm), dispersed in a binary water-glycerol solution. The Schottky interface between Ti3C2Tx and ZnS enhances electron transfer at the heterophase boundary, significantly improving interface polarisation. Simultaneously, interactions between water and glycerol restrict the rotation of polar molecules under external electromagnetic fields, optimising polarisation loss within the gel. Experimental results demonstrate that the Ti3C2Tx/ZnS gel achieves a minimum reflection loss (RLmin) of −43.76 dB at 8.79 GHz, with an effective absorption bandwidth (EAB) covering the entire X-band. Additionally, the gel exhibit exceptional stretchability, frost resistance, shape adaptability, and photothermal conversion properties.
{"title":"Schottky Interface Engineering in Ti3C2Tx/ZnS Organic Hydrogels for High-Performance Multifunctional Flexible Absorbers","authors":"Yuhong Cui, Guoliang Ru, Tianyi Zhang, Ke Yang, Shujuan Liu, Weihong Qi, Qian Ye, Xuqing Liu, Feng Zhou","doi":"10.1002/adfm.202417346","DOIUrl":"https://doi.org/10.1002/adfm.202417346","url":null,"abstract":"With the rapid advancement of wearable electronics, soft robotics, and camouflage technologies, there is an urgent demand for flexible, multifunctional electromagnetic wave absorbing materials. Traditional absorbers, including metal- and carbon-based materials, often lack the flexibility required for such applications. In this work, a novel strategy is proposed for developing a flexible absorber by combining a conductive filler with a Schottky heterogeneous interface and a polymer network framework. Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> MXene is modified with ZnS via a low-temperature hydrothermal method, forming a Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>/ZnS composite. This composite is subsequently embedded in a copolymer matrix of polyvinyl alcohol (PVA) and acrylamide (AAm), dispersed in a binary water-glycerol solution. The Schottky interface between Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> and ZnS enhances electron transfer at the heterophase boundary, significantly improving interface polarisation. Simultaneously, interactions between water and glycerol restrict the rotation of polar molecules under external electromagnetic fields, optimising polarisation loss within the gel. Experimental results demonstrate that the Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>/ZnS gel achieves a minimum reflection loss (RL<sub>min</sub>) of −43.76 dB at 8.79 GHz, with an effective absorption bandwidth (EAB) covering the entire X-band. Additionally, the gel exhibit exceptional stretchability, frost resistance, shape adaptability, and photothermal conversion properties.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"13 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665392","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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