Mengmeng Li, Tingting Wu, Zhiyang Zhao, Lei Li, Tongxin Shan, Hui Wu, Robert Zboray, Francesco Bernasconi, Yongjie Cui, Peiying Hu, Wim J. Malfait, Qinghua Zhang, Shanyu Zhao
Mitigating embodied emissions is becoming increasingly crucial as the energy supply shifts toward more sustainable sources. Bio-based materials present a potentially more sustainable alternative to synthetic polymers; however, it often do not yet match the performance of synthetic materials. Given the ongoing reliance on high-performance, high-environmental-impact materials, it is essential to ensure their complete recyclability. Aerogels, recognized by IUPAC as one of the top ten emerging technologies, are witnessing rapid market growth in thermal insulation and thermal protection applications. In certain applications, synthetic and composite aerogels exhibit superior performance, particularly under high temperatures. Here, molecular simulation tools are employed to elucidate the interaction forces between polymers and solvents, develop a recycling strategy for polyimide-based aerogels, and demonstrate their application in thermal protection for firefighter textiles and thermal runaway protection for Li-ion battery packs. These composites are engineered for disassembly, allowing for the complete recovery of starting materials without any degradation of components after multiple recycling cycles. The recyclable composites can be fabricated using various manufacturing techniques to produce fibers (1D), membranes (2D), and complex structures (3D). This unique combination of outstanding performance and excellent recyclability facilitates the sustainable utilization of aerogels in protective clothing, electric mobility, consumer goods, and aeronautics.
{"title":"Multiscale Manufacturing of Recyclable Polyimide Composite Aerogels","authors":"Mengmeng Li, Tingting Wu, Zhiyang Zhao, Lei Li, Tongxin Shan, Hui Wu, Robert Zboray, Francesco Bernasconi, Yongjie Cui, Peiying Hu, Wim J. Malfait, Qinghua Zhang, Shanyu Zhao","doi":"10.1002/adma.202411599","DOIUrl":"https://doi.org/10.1002/adma.202411599","url":null,"abstract":"Mitigating embodied emissions is becoming increasingly crucial as the energy supply shifts toward more sustainable sources. Bio-based materials present a potentially more sustainable alternative to synthetic polymers; however, it often do not yet match the performance of synthetic materials. Given the ongoing reliance on high-performance, high-environmental-impact materials, it is essential to ensure their complete recyclability. Aerogels, recognized by IUPAC as one of the top ten emerging technologies, are witnessing rapid market growth in thermal insulation and thermal protection applications. In certain applications, synthetic and composite aerogels exhibit superior performance, particularly under high temperatures. Here, molecular simulation tools are employed to elucidate the interaction forces between polymers and solvents, develop a recycling strategy for polyimide-based aerogels, and demonstrate their application in thermal protection for firefighter textiles and thermal runaway protection for Li-ion battery packs. These composites are engineered for disassembly, allowing for the complete recovery of starting materials without any degradation of components after multiple recycling cycles. The recyclable composites can be fabricated using various manufacturing techniques to produce fibers (1D), membranes (2D), and complex structures (3D). This unique combination of outstanding performance and excellent recyclability facilitates the sustainable utilization of aerogels in protective clothing, electric mobility, consumer goods, and aeronautics.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"36 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601911","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Metal–organic framework (MOF) heterostructures with hybrid architectures and abundant functional sites possess great potential applications in advanced information security, yet still suffer from the harsh stimuli mechanisms with restrained emission control. Herein, the differentiated design strategy on intra-ligand charge transfer is first reported to realize smart-responsive multicolor MOF heterostructures as robust anticounterfeiting labels. Designed similar MOF blocks with the differentiated intra-ligand charge transfer are integrated via time-dependent epitaxial growth to form multicolor MOF heterostructures. Different numbers of electron-donating groups in MOF blocks offer distinct space regulation on the torsion of charge transfer ligands, which trigger the diverse responsive emissions under the same mild stimuli, thus generating multiple tunable color patterns in heterostructures. These spatial-resolved MOF heterostructures with stable multicolor responsive modes permit the encoding of fingerprint information, which further functions as robust anti-counterfeiting labels with high-security convert states. These results offer a promising route for the function-oriented exploitation of smart-responsive MOF heterosystems for advanced information anticounterfeiting.
{"title":"Differentiated Intra-Ligand Charge Transfer Boosting Multicolor Responsive MOF Heterostructures as Robust Anti-Counterfeiting Labels","authors":"Yuanchao Lv, Chenwei Lin, Xinming Liu, Jiashuai Liang, Yunbin Li, Zizhu Yao, Shengchang Xiang, Banglin Chen, Zhangjing Zhang","doi":"10.1002/adma.202412637","DOIUrl":"https://doi.org/10.1002/adma.202412637","url":null,"abstract":"Metal–organic framework (MOF) heterostructures with hybrid architectures and abundant functional sites possess great potential applications in advanced information security, yet still suffer from the harsh stimuli mechanisms with restrained emission control. Herein, the differentiated design strategy on intra-ligand charge transfer is first reported to realize smart-responsive multicolor MOF heterostructures as robust anticounterfeiting labels. Designed similar MOF blocks with the differentiated intra-ligand charge transfer are integrated via time-dependent epitaxial growth to form multicolor MOF heterostructures. Different numbers of electron-donating groups in MOF blocks offer distinct space regulation on the torsion of charge transfer ligands, which trigger the diverse responsive emissions under the same mild stimuli, thus generating multiple tunable color patterns in heterostructures. These spatial-resolved MOF heterostructures with stable multicolor responsive modes permit the encoding of fingerprint information, which further functions as robust anti-counterfeiting labels with high-security convert states. These results offer a promising route for the function-oriented exploitation of smart-responsive MOF heterosystems for advanced information anticounterfeiting.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"37 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610523","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ceramic aerogels hold significant potential for thermal insulation, yet their mechanical stretchability and thermal stability fall short in extreme environments. Here, the study presents a programmable shape-morphing strategy aimed at engineering a binary network topology structure within ceramic aerogels to effectively dissipate stress and block heat transfer. The special topology design, which includes kirigami lamellated aerogels for bearing loading stress and randomly assembled aerogels for mechanical energy pre-storage to transfer tensile stress, effectively achieves unexpected mechanical tensile properties and thermal stability. The resulting robust meta-aerogels demonstrate remarkable structural stability with topology-derived mechanical tensile of up to 85% strain, excellent resilience to 500 cycles of 50% tensile strain, 1000 cycles of 60% buckling strain, and 500 cycles of 50% compressive strain, temperature-invariant tensile recovery capability; simultaneously, low thermal conductivity of 33.01 mW m−1 K−1 and tensile-invariant thermal insulation makes the ceramic meta-aerogels an ideal substitute material for various applications.
{"title":"Programmable Shape-Morphing Enables Ceramic Meta-Aerogel Highly Stretchable for Thermal Protection","authors":"Xuan Zhang, Jianyong Yu, Yang Si","doi":"10.1002/adma.202412962","DOIUrl":"https://doi.org/10.1002/adma.202412962","url":null,"abstract":"Ceramic aerogels hold significant potential for thermal insulation, yet their mechanical stretchability and thermal stability fall short in extreme environments. Here, the study presents a programmable shape-morphing strategy aimed at engineering a binary network topology structure within ceramic aerogels to effectively dissipate stress and block heat transfer. The special topology design, which includes kirigami lamellated aerogels for bearing loading stress and randomly assembled aerogels for mechanical energy pre-storage to transfer tensile stress, effectively achieves unexpected mechanical tensile properties and thermal stability. The resulting robust meta-aerogels demonstrate remarkable structural stability with topology-derived mechanical tensile of up to 85% strain, excellent resilience to 500 cycles of 50% tensile strain, 1000 cycles of 60% buckling strain, and 500 cycles of 50% compressive strain, temperature-invariant tensile recovery capability; simultaneously, low thermal conductivity of 33.01 mW m<sup>−1</sup> K<sup>−1</sup> and tensile-invariant thermal insulation makes the ceramic meta-aerogels an ideal substitute material for various applications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"18 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610585","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pravin Kavle, Aiden M. Ross, Harikrishnan KP, Peter Meisenheimer, Arvind Dasgupta, Jiyuan Yang, Ching-Che Lin, Hao Pan, Piush Behera, Eric Parsonnet, Xiaoxi Huang, Jacob A. Zorn, Yu-Tsun Shao, Sujit Das, Shi Liu, David A. Muller, Ramamoorthy Ramesh, Long-Qing Chen, Lane W. Martin
The discovery of polar vortices and skyrmions in ferroelectric-dielectric superlattices [such as (PbTiO3)n/(SrTiO3)n] has ushered in an era of novel dipolar topologies and corresponding emergent phenomena. The key to creating such emergent features has generally been considered to be related to counterpoising strongly polar and non-polar materials thus creating the appropriate boundary conditions. This limits the utility these materials can have, however, by rendering (effectively) half of the structure unresponsive to applied stimuli. Here, using advanced thin-film deposition and an array of characterization and simulation approaches, polar vortices are realized in all-ferroelectric trilayers, multilayers, and superlattices built from the fundamental building block of (PbTiO3)n/(PbxSr1−xTiO3)n wherein in-plane ferroelectric polarization in the PbxSr1−xTiO3 provides the appropriate boundary conditions. These superlattices exhibit substantially enhanced electromechanical and ferroelectric responses in the out-of-plane direction that arise from the ability of the polarization in both layers to rotate to the out-of-plane direction under field. In the in-plane direction, the layers are found to be strongly coupled during switching and when heterostructured with ferroelectric-dielectric building blocks, it is possible to produce multistate switching. This approach expands the realm of systems supporting emergent dipolar texture formation and does so with entirely ferroelectric materials thus greatly improving their responses.
{"title":"Highly Responsive Polar Vortices in All-Ferroelectric Heterostructures","authors":"Pravin Kavle, Aiden M. Ross, Harikrishnan KP, Peter Meisenheimer, Arvind Dasgupta, Jiyuan Yang, Ching-Che Lin, Hao Pan, Piush Behera, Eric Parsonnet, Xiaoxi Huang, Jacob A. Zorn, Yu-Tsun Shao, Sujit Das, Shi Liu, David A. Muller, Ramamoorthy Ramesh, Long-Qing Chen, Lane W. Martin","doi":"10.1002/adma.202410146","DOIUrl":"https://doi.org/10.1002/adma.202410146","url":null,"abstract":"The discovery of polar vortices and skyrmions in ferroelectric-dielectric superlattices [such as (PbTiO<sub>3</sub>)<i><sub>n</sub></i>/(SrTiO<sub>3</sub>)<i><sub>n</sub></i>] has ushered in an era of novel dipolar topologies and corresponding emergent phenomena. The key to creating such emergent features has generally been considered to be related to counterpoising strongly polar and non-polar materials thus creating the appropriate boundary conditions. This limits the utility these materials can have, however, by rendering (effectively) half of the structure unresponsive to applied stimuli. Here, using advanced thin-film deposition and an array of characterization and simulation approaches, polar vortices are realized in all-ferroelectric trilayers, multilayers, and superlattices built from the fundamental building block of (PbTiO<sub>3</sub>)<i><sub>n</sub></i>/(Pb<i><sub>x</sub></i>Sr<sub>1−</sub><i><sub>x</sub></i>TiO<sub>3</sub>)<i><sub>n</sub></i> wherein in-plane ferroelectric polarization in the Pb<i><sub>x</sub></i>Sr<sub>1−</sub><i><sub>x</sub></i>TiO<sub>3</sub> provides the appropriate boundary conditions. These superlattices exhibit substantially enhanced electromechanical and ferroelectric responses in the out-of-plane direction that arise from the ability of the polarization in both layers to rotate to the out-of-plane direction under field. In the in-plane direction, the layers are found to be strongly coupled during switching and when heterostructured with ferroelectric-dielectric building blocks, it is possible to produce multistate switching. This approach expands the realm of systems supporting emergent dipolar texture formation and does so with entirely ferroelectric materials thus greatly improving their responses.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"6 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601894","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xiaohong Tan, Jiarui Wang, Yuhang Xiao, Yingying Guo, Weidong He, Binjie Du, Hao Cui, Chengxin Wang
Designing palladium-based formic acid oxidation reaction (FAOR) catalysts to achieve significant breakthroughs in catalytic activity, pathway selectivity, and toxicity resistance is both urgent and challenging. Here, these challenges are addressed by pioneering a novel catalyst design that incorporates both topological and chemical disorder, developing a new class of PdCuLaYMnW high-entropy amorphous alloys with a porous network (Net-Pd-HEAA) as a highly active, selective, and stable FAOR electrocatalyst. This novel Net-Pd-HEAA demonstrates record-breaking FAOR performance, achieving the mass and specific activities of 5.94 A mgPd−1 and 8.94 mA cm−2, respectively, surpassing all previously reported Pd-based catalysts and showing strong competitiveness against advanced Pt-based catalysts. Simulataneously, Net-Pd-HEAA exhibits extraordinary stability in accelerated durability tests (ADT) and chronoamperometry (CA) tests. Advanced characterization and in situ, spectral analysis reveal that the extremely disordered atomic structure effectively regulates the geometric and electronic structure of the Pd sites, enhancing active intermediate coverage, facilitating dehydrogenation pathway, and inhibiting the production/adsorption of CO. Furthermore, when employed as the anode catalyst in proton exchange membrane water electrolysis (PEMWE), Net-Pd-HEAA only requires a potential of 1.28 V to obtain a current density of 1 A cm−2, and operates stably in a highly corrosive electrolyte for over 100 h.
设计钯基甲酸氧化反应（FAOR）催化剂，以便在催化活性、途径选择性和抗毒性方面实现重大突破，既紧迫又具有挑战性。本文通过开创性地结合拓扑和化学无序性的新型催化剂设计，开发出一类具有多孔网络的新型 PdCuLaYMnW 高熵无定形合金（Net-Pd-HEAA），作为一种高活性、高选择性和高稳定性的甲酸氧化反应电催化剂，来应对这些挑战。这种新型 Net-Pd-HEAA 具有破纪录的 FAOR 性能，其质量活性和比活性分别达到了 5.94 A mgPd-1 和 8.94 mA cm-2，超过了之前报道的所有钯基催化剂，与先进的铂基催化剂相比具有很强的竞争力。同时，Net-Pd-HEAA 在加速耐久性试验（ADT）和计时器测定法（CA）试验中表现出非凡的稳定性。先进的表征和原位光谱分析显示，极度无序的原子结构有效地调节了钯位点的几何和电子结构，提高了活性中间体的覆盖率，促进了脱氢途径，并抑制了 CO 的产生/吸附。此外，在质子交换膜电解水（PEMWE）中用作阳极催化剂时，Net-Pd-HEAA 只需要 1.28 V 的电位就能获得 1 A cm-2 的电流密度，并能在高腐蚀性电解质中稳定运行 100 小时以上。
{"title":"Engineering Topological and Chemical Disorder in Pd Sites for Record-Breaking Formic Acid Electrocatalytic Oxidation","authors":"Xiaohong Tan, Jiarui Wang, Yuhang Xiao, Yingying Guo, Weidong He, Binjie Du, Hao Cui, Chengxin Wang","doi":"10.1002/adma.202414283","DOIUrl":"https://doi.org/10.1002/adma.202414283","url":null,"abstract":"Designing palladium-based formic acid oxidation reaction (FAOR) catalysts to achieve significant breakthroughs in catalytic activity, pathway selectivity, and toxicity resistance is both urgent and challenging. Here, these challenges are addressed by pioneering a novel catalyst design that incorporates both topological and chemical disorder, developing a new class of PdCuLaYMnW high-entropy amorphous alloys with a porous network (Net-Pd-HEAA) as a highly active, selective, and stable FAOR electrocatalyst. This novel Net-Pd-HEAA demonstrates record-breaking FAOR performance, achieving the mass and specific activities of 5.94 A mg<sub>Pd</sub><sup>−1</sup> and 8.94 mA cm<sup>−2</sup>, respectively, surpassing all previously reported Pd-based catalysts and showing strong competitiveness against advanced Pt-based catalysts. Simulataneously, Net-Pd-HEAA exhibits extraordinary stability in accelerated durability tests (ADT) and chronoamperometry (CA) tests. Advanced characterization and in situ, spectral analysis reveal that the extremely disordered atomic structure effectively regulates the geometric and electronic structure of the Pd sites, enhancing active intermediate coverage, facilitating dehydrogenation pathway, and inhibiting the production/adsorption of CO. Furthermore, when employed as the anode catalyst in proton exchange membrane water electrolysis (PEMWE), Net-Pd-HEAA only requires a potential of 1.28 V to obtain a current density of 1 A cm<sup>−2</sup>, and operates stably in a highly corrosive electrolyte for over 100 h.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"17 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601909","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yanze Wang, Biyun Ren, Weilin Zheng, Dengfeng Peng, Feng Wang
Near-infrared (NIR) light is promising for bioimaging and information technology due to its high penetration ability and resistance to interference with environmental radiation. Here, a new class of lanthanide-doped SrZnOSe crystals are developed for the self-sustainable generation of NIR emissions under mechanical excitation. It is shown that the SrZnOSe crystals render ≈5-fold stronger NIR emissions than the well-established CaZnOS due to the low phonon energies of the selenide host, as confirmed by Raman spectroscopy. The potential utility of the crystals is demonstrated by integration with a mouthguard, which can generate bright NIR emissions by bite force to transmit encrypted optical signals through thick tissues (up to 8 mm) in ambient environments. The findings provide a powerful addition to the toolbox of self-recovery mechanoluminescent materials and open new possibilities for applied research.
{"title":"Synthesis of SrZnOSe Crystals with Low Phonon Energy for Enhancing Near-Infrared Mechanoluminescence","authors":"Yanze Wang, Biyun Ren, Weilin Zheng, Dengfeng Peng, Feng Wang","doi":"10.1002/adma.202406899","DOIUrl":"https://doi.org/10.1002/adma.202406899","url":null,"abstract":"Near-infrared (NIR) light is promising for bioimaging and information technology due to its high penetration ability and resistance to interference with environmental radiation. Here, a new class of lanthanide-doped SrZnOSe crystals are developed for the self-sustainable generation of NIR emissions under mechanical excitation. It is shown that the SrZnOSe crystals render ≈5-fold stronger NIR emissions than the well-established CaZnOS due to the low phonon energies of the selenide host, as confirmed by Raman spectroscopy. The potential utility of the crystals is demonstrated by integration with a mouthguard, which can generate bright NIR emissions by bite force to transmit encrypted optical signals through thick tissues (up to 8 mm) in ambient environments. The findings provide a powerful addition to the toolbox of self-recovery mechanoluminescent materials and open new possibilities for applied research.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"23 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599943","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Linqi Cheng, Xiaoli Yan, Jie Yu, Xupeng Zhang, Heng-Guo Wang, Fengchao Cui, Yinghui Wang
Redox-active covalent organic frameworks (COFs) are promising candidates for sodium-ion batteries (SIBs). However, the construction of redox-bipolar COFs with the anions and cations co-storage feature for SIBs is rarely reported. Herein, redox-bipolar COF constructed from aniline-fused quinonoid units (TPAD-COF) is developed as the cathode material in SIBs for the first time. The unique integration of conductive aniline skeletons and quinone redox centers endows TPAD-COF with high ionic/electrical conductivity, abundant redox-active sites, and fascinating bipolar features. Consequently, the elaborately tailored TPAD-COF cathode exhibits higher specific capacity (186.4 mAh g−1 at 0.05 A g−1) and superior cycling performance (over 2000 cycles at 1.0 A g−1 with 0.015% decay rate per cycle). Impressively, TPAD-COF also displays a high specific capacity of 101 mAh g−1 even at −20 °C. As a proof of concept, all-organic SIBs (AOSIBs) are assembled using TPAD-COF cathode and disodium terephthalate anode, which also show impressive electrochemical properties, indicating the potential application of TPAD-COF cathode in AOSIBs. The work will pave the avenue toward advanced COFs cathode for rechargeable batteries through rational molecular design.
氧化还原活性共价有机框架（COF）是钠离子电池（SIB）的理想候选材料。然而，为钠离子电池构建具有阴阳离子共储功能的氧化还原双极 COF 的研究却鲜有报道。本文首次开发了由苯胺融合类醌单元构建的氧化还原双极 COF（TPAD-COF），作为 SIB 的阴极材料。导电苯胺骨架和醌氧化还原中心的独特结合赋予了 TPAD-COF 高离子/导电性、丰富的氧化还原活性位点和迷人的双极特性。因此，精心定制的 TPAD-COF 阴极具有更高的比容量（0.05 A g-1 时为 186.4 mAh g-1）和卓越的循环性能（1.0 A g-1 时超过 2000 个循环，每个循环的衰减率为 0.015%）。令人印象深刻的是，TPAD-COF 即使在零下 20 °C，也能显示出 101 mAh g-1 的高比容量。作为概念验证，使用 TPAD-COF 阴极和对苯二甲酸二钠阳极组装的全有机 SIB（AOSIB）也显示出令人印象深刻的电化学特性，表明 TPAD-COF 阴极在 AOSIB 中的潜在应用。这项工作将为通过合理的分子设计将先进的 COFs 阴极用于可充电电池铺平道路。
{"title":"Redox-Bipolar Covalent Organic Framework Cathode for Advanced Sodium-Organic Batteries","authors":"Linqi Cheng, Xiaoli Yan, Jie Yu, Xupeng Zhang, Heng-Guo Wang, Fengchao Cui, Yinghui Wang","doi":"10.1002/adma.202411625","DOIUrl":"https://doi.org/10.1002/adma.202411625","url":null,"abstract":"Redox-active covalent organic frameworks (COFs) are promising candidates for sodium-ion batteries (SIBs). However, the construction of redox-bipolar COFs with the anions and cations co-storage feature for SIBs is rarely reported. Herein, redox-bipolar COF constructed from aniline-fused quinonoid units (TPAD-COF) is developed as the cathode material in SIBs for the first time. The unique integration of conductive aniline skeletons and quinone redox centers endows TPAD-COF with high ionic/electrical conductivity, abundant redox-active sites, and fascinating bipolar features. Consequently, the elaborately tailored TPAD-COF cathode exhibits higher specific capacity (186.4 mAh g<sup>−1</sup> at 0.05 A g<sup>−1</sup>) and superior cycling performance (over 2000 cycles at 1.0 A g<sup>−1</sup> with 0.015% decay rate per cycle). Impressively, TPAD-COF also displays a high specific capacity of 101 mAh g<sup>−1</sup> even at −20 °C. As a proof of concept, all-organic SIBs (AOSIBs) are assembled using TPAD-COF cathode and disodium terephthalate anode, which also show impressive electrochemical properties, indicating the potential application of TPAD-COF cathode in AOSIBs. The work will pave the avenue toward advanced COFs cathode for rechargeable batteries through rational molecular design.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"61 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599947","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Platinum group metals (PGM) have yet to be the most active catalysts in various sustainable energy reactions. Their high cost, however, has made maximizing the activity and minimizing the dosage become an urgent priority for the practical applications of emerging technologies. Herein, a novel 2D Pd nanomesh structure possessing hole inner reconstructed edges (HIER) with exposed high energy facets and overstretched lattice parameters is fabricated through a facile room-temperature reduction method at gram-scale yields. The HIER enhances the catalytic performance of Pd in electrochemical oxygen reduction reaction (ORR), achieving superior mass activity (MA) of 2.672 A mgPd−1, which is 27.8 fold and 23.6 fold higher, respectively, than those of the commercial Pt/C (0.096 A mgPt−1) and Pd/C (0.113 A mgPd−1) at 0.9 VRHE. Most significantly, in H2-air anion exchange membrane fuel cell (AEMFC) and Zn-air battery (ZAB) applications, this unique Pd catalyst delivers a much-outperformed peak power density of 0.86 and 0.22 W cm−2, respectively, compared with 0.54 and 0.13 W cm−2 of the commercial Pt/C catalyst, indicating a novel pathway in electrocatalyst designs through HIER engineering.
在各种可持续能源反应中，铂族金属（PGM）一直是最活跃的催化剂。然而，铂族金属的高成本使得最大限度地提高活性和减少用量成为新兴技术实际应用的当务之急。在此，我们通过一种简单的室温还原方法，以克级产量制造出了一种新型二维钯纳米网状结构，这种结构具有孔内重构边（HIER），具有暴露的高能面和过度拉伸的晶格参数。HIER 增强了钯在电化学氧还原反应（ORR）中的催化性能，在 0.9 VRHE 条件下，钯的质量活度（MA）达到 2.672 A mgPd-1，分别比商业铂/钯（0.096 A mgPt-1）和钯/钯（0.113 A mgPd-1）高出 27.8 倍和 23.6 倍。最重要的是，在 H2- 空气阴离子交换膜燃料电池 (AEMFC) 和锌空气电池 (ZAB) 应用中，这种独特的钯催化剂的峰值功率密度分别为 0.86 W cm-2 和 0.22 W cm-2，远高于商用铂/钯催化剂的 0.54 W cm-2 和 0.13 W cm-2，这表明通过 HIER 工程在电催化剂设计方面开辟了一条新途径。
{"title":"Greatly Enhanced Oxygen Reduction Reaction in Anion Exchange Membrane Fuel Cell and Zn-Air Battery via Hole Inner Edge Reconstruction of 2D Pd Nanomesh","authors":"Jiakang Tian, Yanhui Song, Xiaodong Hao, Xudong Wang, Yongqing Shen, Peizhi Liu, Zebin Wei, Ting Liao, Lei Jiang, Junjie Guo, Bingshe Xu, Ziqi Sun","doi":"10.1002/adma.202412051","DOIUrl":"https://doi.org/10.1002/adma.202412051","url":null,"abstract":"Platinum group metals (PGM) have yet to be the most active catalysts in various sustainable energy reactions. Their high cost, however, has made maximizing the activity and minimizing the dosage become an urgent priority for the practical applications of emerging technologies. Herein, a novel 2D Pd nanomesh structure possessing hole inner reconstructed edges (HIER) with exposed high energy facets and overstretched lattice parameters is fabricated through a facile room-temperature reduction method at gram-scale yields. The HIER enhances the catalytic performance of Pd in electrochemical oxygen reduction reaction (ORR), achieving superior mass activity (MA) of 2.672 A mg<sub>Pd</sub><sup>−1</sup>, which is 27.8 fold and 23.6 fold higher, respectively, than those of the commercial Pt/C (0.096 A mg<sub>Pt</sub><sup>−1</sup>) and Pd/C (0.113 A mg<sub>Pd</sub><sup>−1</sup>) at 0.9 V<sub>RHE</sub>. Most significantly, in H<sub>2</sub>-air anion exchange membrane fuel cell (AEMFC) and Zn-air battery (ZAB) applications, this unique Pd catalyst delivers a much-outperformed peak power density of 0.86 and 0.22 W cm<sup>−2</sup>, respectively, compared with 0.54 and 0.13 W cm<sup>−2</sup> of the commercial Pt/C catalyst, indicating a novel pathway in electrocatalyst designs through HIER engineering.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"196 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599973","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Mechanically regulated wound dressings require a rational combination of contraction and adhesion functions as well as balancing exudate-induced swelling issues. However, many of the reported dressings face the dilemma of impaired function and impeded wound self-contraction due to fluid-absorbing swelling. In this study, inspired by the tree ring, a core–ring structured hydrogel dressing capable of mechanical modulation is designed, and prepare it using a simple two-step photopolymerization process. The core covers the center of the wound, contracts spontaneously at body temperature to generate a contractile force of 3.4 kPa, and resists swelling. Meanwhile, the ring adheres to the normal epidermis around the wound and transfers the contraction stress to the wound edge. The integration of a functionally independent core and ring ultimately achieves effective wound traction and avoids dressing swelling. In murine and porcine skin wound-healing models, this hydrogel with a closely connected core and ring promotes healing by accelerating epidermal closure (50% closure in mouse skin on day 2, 85% closure in pig skin on day 8), collagen deposition, vascular maturation, and extracellular matrix remodeling. These results can guide further research on mechanical force modulation in wound healing, with the potential for clinical translation.
{"title":"Naturally Inspired Tree-Ring Structured Dressing Provides Sustained Wound Tightening and Accelerates Closure","authors":"Honggui Chen, Rui Zhang, Guo Zhang, Xiaoyang Liang, Chen Xu, Yang Li, Fu-Jian Xu","doi":"10.1002/adma.202410845","DOIUrl":"https://doi.org/10.1002/adma.202410845","url":null,"abstract":"Mechanically regulated wound dressings require a rational combination of contraction and adhesion functions as well as balancing exudate-induced swelling issues. However, many of the reported dressings face the dilemma of impaired function and impeded wound self-contraction due to fluid-absorbing swelling. In this study, inspired by the tree ring, a core–ring structured hydrogel dressing capable of mechanical modulation is designed, and prepare it using a simple two-step photopolymerization process. The core covers the center of the wound, contracts spontaneously at body temperature to generate a contractile force of 3.4 kPa, and resists swelling. Meanwhile, the ring adheres to the normal epidermis around the wound and transfers the contraction stress to the wound edge. The integration of a functionally independent core and ring ultimately achieves effective wound traction and avoids dressing swelling. In murine and porcine skin wound-healing models, this hydrogel with a closely connected core and ring promotes healing by accelerating epidermal closure (50% closure in mouse skin on day 2, 85% closure in pig skin on day 8), collagen deposition, vascular maturation, and extracellular matrix remodeling. These results can guide further research on mechanical force modulation in wound healing, with the potential for clinical translation.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"6 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601921","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pulmonary hypertension (PH) significantly affects the quality of life and lifespan of humans and has promoted the development of flexible implantable electronic devices for PH diagnosis and prevention. Traditional implantable devices based on the von Neumann architecture face insurmountable challenges in processing large amounts of biological data due to computational bottlenecks. Memristors, with integrated in-memory sensing and computing capabilities, can effectively eliminate computational bottlenecks and become one of the most promising products in implantable devices for health monitoring. Here, a memristor with the Ag/MnO2/BaTiO3/FTO structure is implemented and implanted into Sprague‒Dawley (SD) rats. With polydimethylsiloxane (PDMS) packaging, the device can be continuously worked in vivo for up to four weeks, demonstrating excellent stability and biocompatibility. Furthermore, a memristive sensor array is designed for pulmonary artery blood pressure monitoring based on the pressure-responsive characteristics of the as-prepared memristive device. The front-end memristive sensor array can collect and feedback pressure signal, while noise reduction is achieved through memristive logic circuits, and ultimately the memristor neural network processes and classifies the information. Therefore, this work demonstrates the potential of implantable memristors for pulmonary artery pressure monitoring and provides new inspiration for the design of efficient, real-time, and reliable implantable pressure monitoring devices in medical health monitoring.
{"title":"A High-Stability Pressure-Sensitive Implantable Memristor for Pulmonary Hypertension Monitoring","authors":"Zelin Cao, Yiwei Liu, Bai Sun, Guangdong Zhou, Kaikai Gao, Siyu Sun, Yu Cui, Mengna Wang, Xianxia Yan, Tianfu Zhao, Xiaoliang Chen, Jinyou Shao, Sida Qin","doi":"10.1002/adma.202411659","DOIUrl":"https://doi.org/10.1002/adma.202411659","url":null,"abstract":"Pulmonary hypertension (PH) significantly affects the quality of life and lifespan of humans and has promoted the development of flexible implantable electronic devices for PH diagnosis and prevention. Traditional implantable devices based on the von Neumann architecture face insurmountable challenges in processing large amounts of biological data due to computational bottlenecks. Memristors, with integrated in-memory sensing and computing capabilities, can effectively eliminate computational bottlenecks and become one of the most promising products in implantable devices for health monitoring. Here, a memristor with the Ag/MnO<sub>2</sub>/BaTiO<sub>3</sub>/FTO structure is implemented and implanted into Sprague‒Dawley (SD) rats. With polydimethylsiloxane (PDMS) packaging, the device can be continuously worked in vivo for up to four weeks, demonstrating excellent stability and biocompatibility. Furthermore, a memristive sensor array is designed for pulmonary artery blood pressure monitoring based on the pressure-responsive characteristics of the as-prepared memristive device. The front-end memristive sensor array can collect and feedback pressure signal, while noise reduction is achieved through memristive logic circuits, and ultimately the memristor neural network processes and classifies the information. Therefore, this work demonstrates the potential of implantable memristors for pulmonary artery pressure monitoring and provides new inspiration for the design of efficient, real-time, and reliable implantable pressure monitoring devices in medical health monitoring.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"18 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601914","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","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：