The migration of atomic hydrogen species over heterogeneous catalysts is deemed essential for hydrogenation reactions, a process closely related to the catalyst's functionalities. While surface hydroxyls-assisted hydrogen spillover is well documented on reducible oxide supports, its effect on widely-used nonreducible supports, especially in electrocatalytic reactions with water as the hydrogen source, remains a subject of debate. Herein, a nonreducible oxide-anchored copper single-atom catalyst (Cu1/SiO2) is designed and uncover that the surface hydroxyls on SiO2 can serve as efficient transport channels for hydrogen spillover, thereby enhancing the activated hydrogen coverage on the catalyst and favoring the hydrogenation reaction. Using electrocatalytic dechlorination as a model reaction, the Cu1/SiO2 catalyst delivers hydrodechlorination activity 42 times greater than that of commercial Pd/C. An integrated experimental and theoretical investigation elucidates that surface hydroxyls facilitate the spillover of hydrogen intermediates formed at the Cu sites, boosting the coverage of active hydrogen on the surface of the Cu1/SiO2. This work demonstrates the feasibility of surface hydroxyls acting as transport channels for hydrogen-species to boost hydrogen spillover on nonreducible oxide supports and paves the way for designing advanced selective hydrogenation electrocatalysts.
{"title":"Electrocatalytic Hydrogenation Boosted by Surface Hydroxyls-Modulated Hydrogen Migration over Nonreducible Oxides","authors":"Shi-Lin Xu, Wei Wang, Hao-Tong Li, Yu-Xiang Gao, Yuan Min, Peigen Liu, Xusheng Zheng, Dong-Feng Liu, Jie-Jie Chen, Han-Qing Yu, Xiao Zhou, Yuen Wu","doi":"10.1002/adma.202500371","DOIUrl":"https://doi.org/10.1002/adma.202500371","url":null,"abstract":"The migration of atomic hydrogen species over heterogeneous catalysts is deemed essential for hydrogenation reactions, a process closely related to the catalyst's functionalities. While surface hydroxyls-assisted hydrogen spillover is well documented on reducible oxide supports, its effect on widely-used nonreducible supports, especially in electrocatalytic reactions with water as the hydrogen source, remains a subject of debate. Herein, a nonreducible oxide-anchored copper single-atom catalyst (Cu<sub>1</sub>/SiO<sub>2</sub>) is designed and uncover that the surface hydroxyls on SiO<sub>2</sub> can serve as efficient transport channels for hydrogen spillover, thereby enhancing the activated hydrogen coverage on the catalyst and favoring the hydrogenation reaction. Using electrocatalytic dechlorination as a model reaction, the Cu<sub>1</sub>/SiO<sub>2</sub> catalyst delivers hydrodechlorination activity 42 times greater than that of commercial Pd/C. An integrated experimental and theoretical investigation elucidates that surface hydroxyls facilitate the spillover of hydrogen intermediates formed at the Cu sites, boosting the coverage of active hydrogen on the surface of the Cu<sub>1</sub>/SiO<sub>2</sub>. This work demonstrates the feasibility of surface hydroxyls acting as transport channels for hydrogen-species to boost hydrogen spillover on nonreducible oxide supports and paves the way for designing advanced selective hydrogenation electrocatalysts.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"5 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435599","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}
Long Ren, Bing Wang, Di Miao, Pan Xiang, Zhen Zeng, Zhiqian Li, Xiaoting Chen, Chenjie Xu, Qiyong Gong, Kui Luo, Jing Jing
Strategically targeting lymph nodes (LNs) to orchestrate the initiation and regulation of adaptive immune responses is one of the most pressing challenges in the context of vaccination. Herein, a series of polymer-TLR agonist conjugates (PTACs) is developed to investigate the impact of dendritic-topological characteristics on their LN targeting activity in vivo, and their molecular weight (MW) on their pharmacokinetics in support of their LN homing. Notably, the dendritic 6-arm PTAC with a MW of 60 kDa (6A-PTAC-60k) rapidly delivered cargo to draining LNs after administration to peripheral tissues. Specifically, this topologic structure ameliorated the targeting behavior within lymphatic vessels and LNs, including an elevated amount of TLR7/8 agonist delivered to the LNs, an improved distribution pattern among barrier cells and immune cells, increased permeability, and prolonged retention. Furthermore, the 6A-PTAC-60k formulation induced broad antibody and T cell responses, enhancing vaccine immunogenicity and suppressing tumor growth. The results revealed that both the topology and MW of polymers are crucial factors for immunoadjuvant distribution and their functional activity in the draining LNs, which, in turn, enhanced the immunogenicity of the vaccine formulation. This study may provide a chemical and structural basis for optimizing the design of immunoadjuvant delivery systems.
{"title":"Topology-Oriented Lymph Node Drainage of Dendritic Polymer-TLR Agonist Conjugates to Enhance Vaccine Immunogenicity","authors":"Long Ren, Bing Wang, Di Miao, Pan Xiang, Zhen Zeng, Zhiqian Li, Xiaoting Chen, Chenjie Xu, Qiyong Gong, Kui Luo, Jing Jing","doi":"10.1002/adma.202417704","DOIUrl":"https://doi.org/10.1002/adma.202417704","url":null,"abstract":"Strategically targeting lymph nodes (LNs) to orchestrate the initiation and regulation of adaptive immune responses is one of the most pressing challenges in the context of vaccination. Herein, a series of polymer-TLR agonist conjugates (PTACs) is developed to investigate the impact of dendritic-topological characteristics on their LN targeting activity in vivo, and their molecular weight (MW) on their pharmacokinetics in support of their LN homing. Notably, the dendritic 6-arm PTAC with a MW of 60 kDa (6A-PTAC-60k) rapidly delivered cargo to draining LNs after administration to peripheral tissues. Specifically, this topologic structure ameliorated the targeting behavior within lymphatic vessels and LNs, including an elevated amount of TLR7/8 agonist delivered to the LNs, an improved distribution pattern among barrier cells and immune cells, increased permeability, and prolonged retention. Furthermore, the 6A-PTAC-60k formulation induced broad antibody and T cell responses, enhancing vaccine immunogenicity and suppressing tumor growth. The results revealed that both the topology and MW of polymers are crucial factors for immunoadjuvant distribution and their functional activity in the draining LNs, which, in turn, enhanced the immunogenicity of the vaccine formulation. This study may provide a chemical and structural basis for optimizing the design of immunoadjuvant delivery systems.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"70 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435605","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}
Yunfei Ren, Xiaoci Liang, Xiuyuan Lu, Baiquan Liu, Li Zhang, Lingjiao Zhang, Yi Huang, Huajian Zheng, Yizheng Jin, Chuan Liu
Electroluminescence (EL) is essential for modern technologies, such as displays, lighting, and optical communications. To date, some kinds of artificial EL devices have been developed, including organic light-emitting diodes (OLEDs), quantum-dot (QD) LEDs, and light-emitting electrochemical cells. However, issues (e.g., inefficient charge injection, exciton quenching) limit the further EL performance. Here, another promising kind of EL device is reported, which is called QD-electrolyte LED (QE-LED). The key feature of QE-LED is that an ionic liquid is doped into QDs as the electrolyte emitter of multi-layer device architectures. Both theoretical and experimental analyses reveal that an enhanced interface electric field from the in situ formed electrical double layer is leveraged to improve the charge injection and transport. With the introduction of insulating polymers into QD-electrolyte emitters, red QE-LED achieves an external quantum efficiency of 20.5% and a lifetime (T95) over 3.74 × 105 h at the display-related luminance of 100 cd m−2, indicating that the QE-LED is among the best EL devices. Furthermore, an active-matrix QE-LED display is demonstrated with superior stability that overtakes the commercial benchmark. These results offer an avenue to discover unexplored EL devices and provide potential pathways to enhance charge dynamics for EL devices.
{"title":"Quantum-Dot-Electrolyte Light-Emitting Diodes for Displays","authors":"Yunfei Ren, Xiaoci Liang, Xiuyuan Lu, Baiquan Liu, Li Zhang, Lingjiao Zhang, Yi Huang, Huajian Zheng, Yizheng Jin, Chuan Liu","doi":"10.1002/adma.202417330","DOIUrl":"https://doi.org/10.1002/adma.202417330","url":null,"abstract":"Electroluminescence (EL) is essential for modern technologies, such as displays, lighting, and optical communications. To date, some kinds of artificial EL devices have been developed, including organic light-emitting diodes (OLEDs), quantum-dot (QD) LEDs, and light-emitting electrochemical cells. However, issues (e.g., inefficient charge injection, exciton quenching) limit the further EL performance. Here, another promising kind of EL device is reported, which is called QD-electrolyte LED (QE-LED). The key feature of QE-LED is that an ionic liquid is doped into QDs as the electrolyte emitter of multi-layer device architectures. Both theoretical and experimental analyses reveal that an enhanced interface electric field from the in situ formed electrical double layer is leveraged to improve the charge injection and transport. With the introduction of insulating polymers into QD-electrolyte emitters, red QE-LED achieves an external quantum efficiency of 20.5% and a lifetime (T<sub>95</sub>) over 3.74 × 10<sup>5</sup> h at the display-related luminance of 100 cd m<sup>−2</sup>, indicating that the QE-LED is among the best EL devices. Furthermore, an active-matrix QE-LED display is demonstrated with superior stability that overtakes the commercial benchmark. These results offer an avenue to discover unexplored EL devices and provide potential pathways to enhance charge dynamics for EL devices.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"85 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435601","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}
Han Huang, Ruiyang Zhao, Yunfei Li, Ying Ji, Yuan Li, Yibo Deng, Qing Liao, Hongbing Fu
The development of ultra-high-definition (UHD) displays demands organic light-emitting diodes (OLEDs) with high color purity of all three primary colors for a wide color gamut and high brightness essential for future AR/VR applications. However, the vibronic coupling in organic emitters typically results in broad emissions, with a full width at half maximum (FWHM) exceeding 40–50 nm. Herein, multicolor organic single-crystal microcavity light-emitting diodes (SC-MC-OLEDs) are demonstrated by embedding ultrathin 2D organic single crystals (2D-OSCs) between two silver layers that serve as both electrodes and mirrors. By leveraging the microcavity effect, the resonant output frequencies of SC-MC-OLEDs can be continuously tuned from 448 to 602 nm by adjusting the thickness of 2D-OSCs (i.e., the microcavity length), achieving high color purity with a full width at half maximum (FWHM) of <10 nm. Furthermore, the Purcell effect in SC-MC-OLEDs enhances the radiative rate and improves light-coupling efficiency, resulting in a maximum external quantum efficiency (EQE) of up to 4% and minimal efficiency roll-off. Due to the excellent bipolar transport properties of OSCs, the brightness of SC-MC-OLEDs surpasses 106 cd m−2, along with a degree of linear polarization exceeding 0.9, unlocking new application opportunities.
{"title":"Multicolor Organic Single-Crystal Microcavity Light Emitting Diodes With High Color-Purity and High Brightness","authors":"Han Huang, Ruiyang Zhao, Yunfei Li, Ying Ji, Yuan Li, Yibo Deng, Qing Liao, Hongbing Fu","doi":"10.1002/adma.202418278","DOIUrl":"https://doi.org/10.1002/adma.202418278","url":null,"abstract":"The development of ultra-high-definition (UHD) displays demands organic light-emitting diodes (OLEDs) with high color purity of all three primary colors for a wide color gamut and high brightness essential for future AR/VR applications. However, the vibronic coupling in organic emitters typically results in broad emissions, with a full width at half maximum (FWHM) exceeding 40–50 nm. Herein, multicolor organic single-crystal microcavity light-emitting diodes (SC-MC-OLEDs) are demonstrated by embedding ultrathin 2D organic single crystals (2D-OSCs) between two silver layers that serve as both electrodes and mirrors. By leveraging the microcavity effect, the resonant output frequencies of SC-MC-OLEDs can be continuously tuned from 448 to 602 nm by adjusting the thickness of 2D-OSCs (i.e., the microcavity length), achieving high color purity with a full width at half maximum (FWHM) of <10 nm. Furthermore, the Purcell effect in SC-MC-OLEDs enhances the radiative rate and improves light-coupling efficiency, resulting in a maximum external quantum efficiency (EQE) of up to 4% and minimal efficiency roll-off. Due to the excellent bipolar transport properties of OSCs, the brightness of SC-MC-OLEDs surpasses 10<sup>6</sup> cd m<sup>−2</sup>, along with a degree of linear polarization exceeding 0.9, unlocking new application opportunities.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"29 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435565","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}
Fluoride ion batteries (FIBs) have garnered significant attention due to their ultrahigh theoretical energy density, dendrite-free safety, and resource abundance. Although some anion acceptors have been proposed to address the insolubility of inorganic fluoride salts, the difficulty in dissociating fluoride ions from acceptors results in short lifespan and extremely low specific capacity of FIBs. Here, a fluoride ion battery is demonstrated with unprecedented long life and ultrahigh specific capacity through the design of an acceptor-multi-F state electrolyte. The high Lewis acidity of triphenylantimony chloride (TSbCl) as a novel anion acceptor in electrolyte facilitates the complete dissociation of CsF, and the resulting TSbCl-F complex can further interact with fluoride ions to form the acceptor-multi-F states. This strategy combines the high dissociation capability for fluoride salts with the minimal thermodynamic barriers for releasing fluoride ions at electrode-electrolyte interface. This electrolyte design endows FIBs with durable reversible fluorination/defluorination reaction (3700 cycles with high coulombic efficiency of 99.5% and small voltage polarization of 30 mV) and ultrahigh reversible capacity (580 mAh g−1 after 40 cycles at 100 mA g−1). The high-output voltage FIBs of CuF2//Li configuration (with discharge plateau of 2.9 V) and larger-sized pouch-type FIBs of CuF2//Sn+SnF2 configuration (with reversible capacity of 530 mAh g−1) are demonstrated.
{"title":"Construction of Acceptor-Multi-F State Electrolyte to Enable Unprecedented Long-Life and High-Capacity Fluoride-Ion Batteries","authors":"Decheng Li, Guyue Li, Yifan Yu, Chilin Li","doi":"10.1002/adma.202415106","DOIUrl":"https://doi.org/10.1002/adma.202415106","url":null,"abstract":"Fluoride ion batteries (FIBs) have garnered significant attention due to their ultrahigh theoretical energy density, dendrite-free safety, and resource abundance. Although some anion acceptors have been proposed to address the insolubility of inorganic fluoride salts, the difficulty in dissociating fluoride ions from acceptors results in short lifespan and extremely low specific capacity of FIBs. Here, a fluoride ion battery is demonstrated with unprecedented long life and ultrahigh specific capacity through the design of an acceptor-multi-F state electrolyte. The high Lewis acidity of triphenylantimony chloride (TSbCl) as a novel anion acceptor in electrolyte facilitates the complete dissociation of CsF, and the resulting TSbCl-F complex can further interact with fluoride ions to form the acceptor-multi-F states. This strategy combines the high dissociation capability for fluoride salts with the minimal thermodynamic barriers for releasing fluoride ions at electrode-electrolyte interface. This electrolyte design endows FIBs with durable reversible fluorination/defluorination reaction (3700 cycles with high coulombic efficiency of 99.5% and small voltage polarization of 30 mV) and ultrahigh reversible capacity (580 mAh g<sup>−1</sup> after 40 cycles at 100 mA g<sup>−1</sup>). The high-output voltage FIBs of CuF<sub>2</sub>//Li configuration (with discharge plateau of 2.9 V) and larger-sized pouch-type FIBs of CuF<sub>2</sub>//Sn+SnF<sub>2</sub> configuration (with reversible capacity of 530 mAh g<sup>−1</sup>) are demonstrated.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"69 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435598","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}
Yang Zong, Minjie Xi, Yunqi Wang, Guohonghao Zeng, Dongliang Hu, Huihui Hu, Xiaoqi Hou, Kewang Nan, Xiangzhong Chen, Fan Xu, Oliver G. Schmidt, Yongfeng Mei, Jizhai Cui
Precisely capturing and manipulating microscale objects, such as individual cells and microorganisms, is fundamental to advancements in biomedical research and microrobotics. Photoactuators based on optical fibers serving as flexible, unobstructed waveguides are well-suited for these operations, particularly in confined locations where free-space illumination is impractical. However, integrating optical fibers with microscale actuators poses significant challenges due to size mismatch, resulting in slow responses inadequate for handling motile micro-objects. This study designs microactuators based on hydrogel/Au bilayer heterostructures that self-roll around a tapered optical fiber. This self-rolling mechanism enables the use of thin hydrogel layers only a few micrometers thick, which rapidly absorb and release water molecules during a phase transition. The resulting microactuators exhibit low bending stiffness and extremely fast responses, achieving large bending angles exceeding 800° within 0.55 s. Using this technique, this study successfully captures rapidly swimming Chlamydomonas and Paramecium, and demonstrates programmable non-reciprocal motion for effective non-contact manipulation of yeast cells. This approach provides a versatile platform for microscale manipulations and holds promise for advanced biomedical applications.
{"title":"Waveguide Microactuators Self-Rolled Around an Optical Fiber Taper","authors":"Yang Zong, Minjie Xi, Yunqi Wang, Guohonghao Zeng, Dongliang Hu, Huihui Hu, Xiaoqi Hou, Kewang Nan, Xiangzhong Chen, Fan Xu, Oliver G. Schmidt, Yongfeng Mei, Jizhai Cui","doi":"10.1002/adma.202418316","DOIUrl":"https://doi.org/10.1002/adma.202418316","url":null,"abstract":"Precisely capturing and manipulating microscale objects, such as individual cells and microorganisms, is fundamental to advancements in biomedical research and microrobotics. Photoactuators based on optical fibers serving as flexible, unobstructed waveguides are well-suited for these operations, particularly in confined locations where free-space illumination is impractical. However, integrating optical fibers with microscale actuators poses significant challenges due to size mismatch, resulting in slow responses inadequate for handling motile micro-objects. This study designs microactuators based on hydrogel/Au bilayer heterostructures that self-roll around a tapered optical fiber. This self-rolling mechanism enables the use of thin hydrogel layers only a few micrometers thick, which rapidly absorb and release water molecules during a phase transition. The resulting microactuators exhibit low bending stiffness and extremely fast responses, achieving large bending angles exceeding 800° within 0.55 s. Using this technique, this study successfully captures rapidly swimming Chlamydomonas and Paramecium, and demonstrates programmable non-reciprocal motion for effective non-contact manipulation of yeast cells. This approach provides a versatile platform for microscale manipulations and holds promise for advanced biomedical applications.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"9 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418467","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}
Zhenghong Xiong, Yun-Sung Jeon, Hongguang Wang, Guiming Fu, Seong-Ho Cho, Seung-Joo Chang, Peter A. van Aken, Nam-Gyu Park
The stability of the FAPbI3 perovskite phase is significantly affected by internal strain. In this report, additives in the perovskite precursor solution are designed to prevent local lattice mismatch of the resulting perovskite layer. Instead of using a conventional methylammonium chloride (Control), triple additives (Target) are introduced by considering ion association and formation energy. The out-of-plane orientation for the (100) plane is less pronounced by the triple additives compared to the Control film with a highly enhanced preferred orientation, which reduces the strain gradient and the Pb─I bond distance. Moreover, the anisotropic atomic-level lattice strain along (111) plane, associated with the α-to-δ phase transition, is more uniformly distributed by the triple additives. The triple-additive strategy demonstrates exceptional phase stability under relative humidity as high as 90% and the International Summit on Organic Photovoltaic Stability (ISOS)-L-2 protocol. The device lifetime measured under the ISOS-D-1 condition shows that the Target perovskite solar cell (PSC) maintains 95% of its initial power conversion efficiency (PCE) for over 8000 h, and the best PCE of 24.50% is achieved.
{"title":"Triple-Additive Strategy for Enhanced Material and Device Stability in Perovskite Solar Cells","authors":"Zhenghong Xiong, Yun-Sung Jeon, Hongguang Wang, Guiming Fu, Seong-Ho Cho, Seung-Joo Chang, Peter A. van Aken, Nam-Gyu Park","doi":"10.1002/adma.202413712","DOIUrl":"https://doi.org/10.1002/adma.202413712","url":null,"abstract":"The stability of the FAPbI<sub>3</sub> perovskite phase is significantly affected by internal strain. In this report, additives in the perovskite precursor solution are designed to prevent local lattice mismatch of the resulting perovskite layer. Instead of using a conventional methylammonium chloride (<i>Control</i>), triple additives (<i>Target</i>) are introduced by considering ion association and formation energy. The out-of-plane orientation for the (100) plane is less pronounced by the triple additives compared to the <i>Control</i> film with a highly enhanced preferred orientation, which reduces the strain gradient and the Pb─I bond distance. Moreover, the anisotropic atomic-level lattice strain along (111) plane, associated with the <i>α</i>-to-<i>δ</i> phase transition, is more uniformly distributed by the triple additives. The triple-additive strategy demonstrates exceptional phase stability under relative humidity as high as 90% and the International Summit on Organic Photovoltaic Stability (ISOS)-L-2 protocol. The device lifetime measured under the ISOS-D-1 condition shows that the <i>Target</i> perovskite solar cell (PSC) maintains 95% of its initial power conversion efficiency (PCE) for over 8000 h, and the best PCE of 24.50% is achieved.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"23 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418468","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}
The unique structure of carbon nanotubes (CNTs) endows them with exceptional electrical and mechanical properties, along with a high surface area, making them highly beneficial for use as flexible, high-performing thermoelectric materials. As a result, the application of CNTs in the thermoelectric field has become increasingly widespread. Considering the rapid advancements in this field, this review offers a timely overview of the most recent progress on CNT-based thermoelectric materials and devices over the past five years. This review begins by introducing the fundamental concepts and thermoelectric mechanisms of CNT-based thermoelectric materials. Then new strategies are explored to enhance their thermoelectric performance, focusing on doping and composites, while emphasizing the importance of CNT stability as a key research area. Additionally, the latest design concepts and expanded application scenarios for flexible and wearable CNTs-based thermoelectric devices are summarized. Finally, the current challenges are addressed and future directions for the development of CNT-based thermoelectric materials and devices are discussed.
{"title":"Advances and Outlooks for Carbon Nanotube-Based Thermoelectric Materials and Devices","authors":"Shanshan Zhou, Xiao-Lei Shi, Lan Li, Qian Liu, Boxuan Hu, Wenyi Chen, Chenyang Zhang, Qingfeng Liu, Zhi-Gang Chen","doi":"10.1002/adma.202500947","DOIUrl":"https://doi.org/10.1002/adma.202500947","url":null,"abstract":"The unique structure of carbon nanotubes (CNTs) endows them with exceptional electrical and mechanical properties, along with a high surface area, making them highly beneficial for use as flexible, high-performing thermoelectric materials. As a result, the application of CNTs in the thermoelectric field has become increasingly widespread. Considering the rapid advancements in this field, this review offers a timely overview of the most recent progress on CNT-based thermoelectric materials and devices over the past five years. This review begins by introducing the fundamental concepts and thermoelectric mechanisms of CNT-based thermoelectric materials. Then new strategies are explored to enhance their thermoelectric performance, focusing on doping and composites, while emphasizing the importance of CNT stability as a key research area. Additionally, the latest design concepts and expanded application scenarios for flexible and wearable CNTs-based thermoelectric devices are summarized. Finally, the current challenges are addressed and future directions for the development of CNT-based thermoelectric materials and devices are discussed.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"180 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418471","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}
Ultrasound therapy has turned up as a noninvasive multifunctional tool for cancer immunotherapy. However, the insufficient co-stimulating molecules and loss of peptide-major histocompatibility complex I (MHC-I) expression on tumor cells lead to poor therapy of sonoimmunotherapies. Herein, this work develops a sonosensitive system to augment MHC-I unrestricted natural killer (NK) cell-mediated innate immunity and T cell-mediated adaptive immunity by leveraging antigen presentation cell (APC)-like tumor cells. Genetically engineered tumor cells featuring sufficient co-stimulating molecules are cryo-shocked and conjugated with a sonosensitizer, hematoporphyrin monomethyl ether, using click chemistry. These cells (DPNLs) exhibit characteristics of tumor and draining lymph node homing. Under ultrasound, NK cell-mediated innate immunity within the tumor microenvironment could be activated, and T cells in the tumor-draining lymph nodes (TDLNs) are stimulated through co-stimulatory molecules. In combination with programmed cell death ligand 1 (PD-L1) antibody, DPNLs extend the survival time and inhibited lung metastasis in triple-negative breast cancer (TNBC) models. This study provides an alternative approach for sonoimmunotherapy with precise sonosensitizer delivery and enhanced NK cell and T cell activation.
超声波疗法已成为癌症免疫疗法的一种非侵入性多功能工具。然而，辅助刺激分子的不足和肿瘤细胞上多肽-主要组织相容性复合体 I（MHC-I）表达的缺失导致超声免疫疗法的治疗效果不佳。在此，这项研究开发了一种声敏感系统，通过利用抗原呈递细胞（APC）样肿瘤细胞，增强 MHC-I 不受限制的自然杀伤细胞（NK）介导的先天性免疫和 T 细胞介导的适应性免疫。基因工程肿瘤细胞具有足够的协同刺激分子，经低温震荡后，利用点击化学方法与一种声敏剂--血卟啉单甲醚--共轭。这些细胞（DPNLs）表现出肿瘤和引流淋巴结归巢的特征。在超声波作用下，肿瘤微环境中由 NK 细胞介导的先天性免疫可被激活，而肿瘤引流淋巴结（TDLNs）中的 T 细胞则会通过共刺激分子受到刺激。DPNLs与程序性细胞死亡配体1（PD-L1）抗体结合使用，可延长三阴性乳腺癌（TNBC）模型的生存时间并抑制肺转移。这项研究为声波免疫疗法提供了另一种方法，即精确传递声波增敏剂并增强 NK 细胞和 T 细胞的活化。
{"title":"Cryo-Shocked Tumor-Reprogrammed Sonosensitive Antigen-Presenting Cells Improving Sonoimmunotherapy via T Cells and NK Cells Immunity","authors":"Xindi Qian, Wenzhe Yi, Wenlu Yan, Ying Cai, Shuangshuang Hu, Dan Yan, Zhiwen Zhao, Rongzhang Li, Liying Wang, Huixiong Xu, Yaping Li","doi":"10.1002/adma.202413289","DOIUrl":"https://doi.org/10.1002/adma.202413289","url":null,"abstract":"Ultrasound therapy has turned up as a noninvasive multifunctional tool for cancer immunotherapy. However, the insufficient co-stimulating molecules and loss of peptide-major histocompatibility complex I (MHC-I) expression on tumor cells lead to poor therapy of sonoimmunotherapies. Herein, this work develops a sonosensitive system to augment MHC-I unrestricted natural killer (NK) cell-mediated innate immunity and T cell-mediated adaptive immunity by leveraging antigen presentation cell (APC)-like tumor cells. Genetically engineered tumor cells featuring sufficient co-stimulating molecules are cryo-shocked and conjugated with a sonosensitizer, hematoporphyrin monomethyl ether, using click chemistry. These cells (DPNLs) exhibit characteristics of tumor and draining lymph node homing. Under ultrasound, NK cell-mediated innate immunity within the tumor microenvironment could be activated, and T cells in the tumor-draining lymph nodes (TDLNs) are stimulated through co-stimulatory molecules. In combination with programmed cell death ligand 1 (PD-L1) antibody, DPNLs extend the survival time and inhibited lung metastasis in triple-negative breast cancer (TNBC) models. This study provides an alternative approach for sonoimmunotherapy with precise sonosensitizer delivery and enhanced NK cell and T cell activation.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"64 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418476","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}
The practical development of aqueous zinc-iodine (Zn-I2) batteries is greatly hindered by the low energy density resulting from conventional I0/I− conversion and the limited temperature tolerance. Here, a temperature-insensitive polycationic hydrogel electrolyte borax-bacterial cellulose / p(AM-co-VBIMBr) (denoted as BAVBr) for achieving an energy-dense cascade aqueous Zn-I2 battery over a wide temperature range from −50 to 50 °C is designed. A comprehensive investigation, combining advanced spectroscopic investigation and DFT calculations, has revealed that the presence of Br species in the gel electrolyte facilitates the conversion reaction of Br0/Br−. Simultaneously, it activates the high voltage I+/I0 redox reaction through interhalogen formation. Consequently, sequential and highly reversible redox reactions involving I0/I−, I+/I0, and Br0/Br− are achieved with the assistance of −NR3+ units in BAVBr, effectively suppressing interhalogen hydrolysis in aqueous electrolyte. The cascade reactions lead to a high area capacity of 0.76 mAh cm−2 at a low I2 loading of 1 mg cm−2 or 760 mAh g−1 based on the mass of iodine, demonstrating exceptional long-term cycling stability over a wide temperature range from −50 to 50 °C. This study offers valuable insights into the rational design of electrolytes for high-energy aqueous batteries, specifically tailored for wide-temperature operation.
{"title":"All-Climate Energy-Dense Cascade Aqueous Zn-I2 Batteries Enabled by a Polycationic Hydrogel Electrolyte","authors":"Yangyang Liu, Longhai Zhang, Ling Liu, Quanwei Ma, Rui Wang, Peng Xiong, Hongbao Li, Shilin Zhang, Junnan Hao, Chaofeng Zhang","doi":"10.1002/adma.202415979","DOIUrl":"https://doi.org/10.1002/adma.202415979","url":null,"abstract":"The practical development of aqueous zinc-iodine (Zn-I<sub>2</sub>) batteries is greatly hindered by the low energy density resulting from conventional I<sup>0</sup>/I<sup>−</sup> conversion and the limited temperature tolerance. Here, a temperature-insensitive polycationic hydrogel electrolyte borax-bacterial cellulose / <i>p</i>(AM-<i>co</i>-VBIMBr) (denoted as BAVBr) for achieving an energy-dense cascade aqueous Zn-I<sub>2</sub> battery over a wide temperature range from −50 to 50 °C is designed. A comprehensive investigation, combining advanced spectroscopic investigation and DFT calculations, has revealed that the presence of Br species in the gel electrolyte facilitates the conversion reaction of Br<sup>0</sup>/Br<sup>−</sup>. Simultaneously, it activates the high voltage I<sup>+</sup>/I<sup>0</sup> redox reaction through interhalogen formation. Consequently, sequential and highly reversible redox reactions involving I<sup>0</sup>/I<sup>−</sup>, I<sup>+</sup>/I<sup>0</sup>, and Br<sup>0</sup>/Br<sup>−</sup> are achieved with the assistance of −NR<sub>3</sub><sup>+</sup> units in BAVBr, effectively suppressing interhalogen hydrolysis in aqueous electrolyte. The cascade reactions lead to a high area capacity of 0.76 mAh cm<sup>−2</sup> at a low I<sub>2</sub> loading of 1 mg cm<sup>−2</sup> or 760 mAh g<sup>−1</sup> based on the mass of iodine, demonstrating exceptional long-term cycling stability over a wide temperature range from −50 to 50 °C. This study offers valuable insights into the rational design of electrolytes for high-energy aqueous batteries, specifically tailored for wide-temperature operation.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"11 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418329","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}
京公网安备 11010802042870号
京ICP备2023020795号-1
扫码关注我们
求助内容：
应助结果提醒方式：