Yunshan Zheng, Yuefeng Meng, Xia Hu, Haoyang Peng, Lanlan Feng, Yao Wang, Baohua Li
{"title":"Synthesis-Structure-Property of High-Entropy Layered Oxide Cathode for Li/Na/K-Ion Batteries","authors":"Yunshan Zheng, Yuefeng Meng, Xia Hu, Haoyang Peng, Lanlan Feng, Yao Wang, Baohua Li","doi":"10.1002/adma.202413202","DOIUrl":"https://doi.org/10.1002/adma.202413202","url":null,"abstract":"Increasing demand for rechargeable batteries necessitates improvements in electrochemical performance. Traditional optimal approaches such as elemental doping and surface modification are insufficient for practical applications of the batteries. High-entropy materials (HEMs) possess stable solid-state phases and unparalleled flexibility in composition and electronic structure, which facilitate rapid advancements in battery materials. This review demonstrates the properties of HEMs both qualitatively and quantitatively, and the mechanisms of their enhancement on battery properties. It also illustrates the progress in high-entropy layered oxide cathode materials (HELOs) for lithium/sodium/potassium ion batteries (LIBs/SIBs/PIBs) in the perspectives of synthesis, characterization and application, and elucidating the synthesis-structure-property relationship. Furthermore, it outlines future directions for high-entropy strategies in battery study: precise synthesis control, understanding of reaction mechanisms through structural characterization, elucidation of structure-performance correlations, and the computational and experimental methods integration for rapid screening and analysis of HEMs. The perspective aims to inspire researchers in the development of high-performance rechargeable batteries.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"255 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142690939","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}
Lan Yao, Geru Zhang, Yun Wang, Zhiqiang Liu, Jiale Liang, Jiafei Sun, Songhang Li, Taoran Tian, Yunfeng Lin
{"title":"Development of an Inhalable DNA Tetrahedron MicroRNA Sponge","authors":"Lan Yao, Geru Zhang, Yun Wang, Zhiqiang Liu, Jiale Liang, Jiafei Sun, Songhang Li, Taoran Tian, Yunfeng Lin","doi":"10.1002/adma.202414336","DOIUrl":"https://doi.org/10.1002/adma.202414336","url":null,"abstract":"In designing aerosolized drugs, the challenge lies in achieving optimal penetration and retention. Existing delivery systems prioritize larger particles for prolonged intrapulmonary retention, compromising penetration speed. Conversely, smaller nanoparticles face rapid clearance and limited retention. RNA sponges featuring multiple microRNA binding sites exhibit promising potential for gene expression regulation. However, the complex structure of the frequently utilized cyclic RNA sponge impedes rapid penetration and cellular uptake, restricting its application. This study proposes an innovative approach using a compact tetrahedral framework of nucleic acid to construct an inhalable microRNA sponge. Distinguished by its simplified structure, this microRNA sponge ensures effective microRNA inhibition, rapid tissue penetration, and prolonged residency through prompt endocytosis. Validated in acute lung inflammation models, the approach demonstrates swift restoration of local immune homeostasis. This design addresses the critical need for aerosol vehicles that balance efficient penetration and sustained retention, offering a promising solution for effective gene expression regulation.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"20 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142690936","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Hardware-Feasible and Efficient N-Type Organic Neuromorphic Signal Recognition via Reservoir Computing","authors":"Riping Liu, Yifei He, Xiuyuan Zhu, Jiayao Duan, Chuan Liu, Zhuang Xie, Iain McCulloch, Wan Yue","doi":"10.1002/adma.202409258","DOIUrl":"https://doi.org/10.1002/adma.202409258","url":null,"abstract":"Organic electrochemical synaptic transistors (OESTs), inspired by the biological nervous system, have garnered increasing attention due to their multifunctional applications in neuromorphic computing. However, the practical implementation of OESTs for signal recognition—particularly those utilizing n-type organic mixed ionic-electronic conductors (OMIECs)—still faces significant challenges at the hardware level. Here, a state-of-the-art small-molecule n-type OEST integrated within a physically simple and hardware feasible reservoir-computing (RC) framework for practical temporal signal recognition is presented. This integration is achieved by leveraging the adjustable synaptic properties of the n-OEST, which exhibits tunable nonlinear short-term memory, transitioning from volatility to nonvolatility, and demonstrating adaptive temporal specificity. Additionally, the nonvolatile OEST offers 256 conductance levels and a wide dynamic range (≈147) in long-term potentiation/depression (LTP/LTD), surpassing previously reported n-OESTs. By combining volatile n-OESTs as reservoirs with a single-layer perceptron readout composed of nonvolatile n-OEST networks, this physical RC system achieves substantial recognition accuracy for both handwritten-digit images (94.9%) and spoken digit (90.7%), along with ultrahigh weight efficiency. Furthermore, this system demonstrates outstanding accuracy (98.0%) by grouped RC in practical sleep monitoring, specifically in snoring recognition. Here, a reliable pathway for OMIEC-driven computing is presented to advance bioinspired hardware-based neuromorphic computing in the physical world.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"76 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142690934","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Screening Fluorination Additives for Efficient Perovskite Light-Emitting Diodes","authors":"Yu Xia, Chen Zou, Yan-Hui Lou, Yu-Hang Zhou, Aleyna Nar, Yu-Han Li, Namatullah Nizamani, Kai-Li Wang, Chun-Hao Chen, Jing Chen, Nan Li, Ilhan Yavuz, Liang-Sheng Liao, Zhao-Kui Wang","doi":"10.1002/adma.202411231","DOIUrl":"https://doi.org/10.1002/adma.202411231","url":null,"abstract":"Fluorinated additives are proposed to address the issue of domain polydispersity in quasi-2D perovskites. However, the lack of established screening criteria for these additives necessitates a laborious and costly trial-and-error process. Herein, this work explores the behind nature for the first time how various fluorination in fluorinated additives affect domain distribution in quasi-2D perovskites. The studies reveal that fully fluorinated additives could suppress undesirable low-dimensional domains, facilitating efficient energy transfer, while partially fluorinated additives adversely cause deteriorated optical properties. The observed trend is ascribed to the molecular dipole moment of the fluorinated additives, offering a reasonable explanation for experimental phenomena that has never been reported before. By employing fully fluorinated additives, the fabricated sky-blue perovskite light-emitting diodes (PeLEDs) deliver a peak external quantum efficiency (EQE) of 20.38% (@488 nm), marking as one of the highest efficiencies reported to date. The finding provides a screening criterion for fluorinated additives to realize efficient PeLEDs.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"34 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142690941","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}
Xingmei Chen, Yinghui Feng, Pei Zhang, Zhipeng Ni, Yu Xue, Ji Liu
{"title":"Hydrogel Fibers-Based Biointerfacing","authors":"Xingmei Chen, Yinghui Feng, Pei Zhang, Zhipeng Ni, Yu Xue, Ji Liu","doi":"10.1002/adma.202413476","DOIUrl":"https://doi.org/10.1002/adma.202413476","url":null,"abstract":"The unique 1D structure of fibers offers intriguing attributes, including a high length-to-diameter ratio, miniatured size, light-weight, and flexibility, making them suitable for various biomedical applications, such as health monitoring, disease treatment, and minimally invasive surgeries. However, traditional fiber devices, typically composed of rigid, dry, and non-living materials, are intrinsically different from the soft, wet, and living essence of biological tissues, thereby posing grand challenges for long-term, reliable, and seamless interfacing with biological systems. Hydrogel fibers have recently emerged as a promising candidate, in light of their similarity to biological tissues in mechanical, chemical and biological aspects, as well as distinct fiber geometry. In this review, a comprehensive overview of recent progress in hydrogel fibers-based biointerfacing technology is provided. It thoroughly summarizes the manufacturing strategy and functional design, especially for hydrogel fibers with distinct optical and electron conductive performance, as well as responsiveness to triggers including thermal, magnetic field and ultrasonic wave, etc. Such unique attributes enable various biomedical applications, which are also examined in detail. Future challenges and potential directions, including biosafety, long-term reliability, sterilization, multi-modalities integration and intelligent therapeutic systems, are raised. This review will serve as a valuable resource for further advancement and implementation as next-generation biointerfacing technology.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"35 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142690938","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Lignocellulose-Mediated Functionalization of Liquid Metals toward the Frontiers of Multifunctional Materials","authors":"Wei Li, Liyu Zhu, Ying Xu, Guanhua Wang, Ting Xu, Chuanling Si","doi":"10.1002/adma.202415761","DOIUrl":"https://doi.org/10.1002/adma.202415761","url":null,"abstract":"Lignocellulose-mediated liquid metal (LM) composites, as emerging functional materials, show tremendous potential for a variety of applications. The abundant hydroxyl, carboxyl, and other polar groups in lignocellulose facilitate the formation of strong chemical bonds with LM surfaces, enhancing wettability and adhesion for improved interface compatibility. Beyond serving as a supportive matrix, lignocellulose can be tailored to optimize the microstructure of the composites, adapting them for diverse applications. This review comprehensively summarizes the fundamental principles and recent advancements in lignocellulose-mediated LM composites, highlighting the advantages of lignocellulose in composite fabrication, including facile synthesis, versatile interactions, and inherent functionalities. Key modulation strategies for LMs and innovative synthesis methods for functionalized lignocellulose composites are discussed. Furthermore, the roles and structure–performance relationships of these composites in electromagnetic shielding, flexible sensors, and energy storage devices are systematically summarized. Finally, the obstacles and prospective advancements pertaining to lignocellulose-mediated LM composites are thoroughly scrutinized and deliberated upon. This review is expected to provide basic guidance for researchers to boost the popularity of LMs in diverse applications and provide useful references for design strategies of state-of-the-art LMs.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"22 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142684991","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}
Nebojša Ilić, Kui Tan, Felix Mayr, Shujin Hou, Benedikt M. Aumeier, Eder Moisés Cedeño Morales, Uwe Hübner, Jennifer Cookman, Andreas Schneemann, Alessio Gagliardi, Jörg E. Drewes, Roland A. Fischer, Soumya Mukherjee
{"title":"Trace Adsorptive Removal of PFAS from Water by Optimizing the UiO-66 MOF Interface","authors":"Nebojša Ilić, Kui Tan, Felix Mayr, Shujin Hou, Benedikt M. Aumeier, Eder Moisés Cedeño Morales, Uwe Hübner, Jennifer Cookman, Andreas Schneemann, Alessio Gagliardi, Jörg E. Drewes, Roland A. Fischer, Soumya Mukherjee","doi":"10.1002/adma.202413120","DOIUrl":"https://doi.org/10.1002/adma.202413120","url":null,"abstract":"The confluence of pervasiveness, bioaccumulation, and toxicity in freshwater contaminants presents an environmental threat second to none. Exemplifying this trifecta, per- and polyfluoroalkyl substances (PFAS) present an alarming hazard among the emerging contaminants. State-of-the-art PFAS adsorbents used in drinking water treatment, namely, activated carbons and ion-exchange resins, are handicapped by low adsorption capacity, competitive adsorption, and/or slow kinetics. To overcome these shortcomings, metal–organic frameworks (MOFs) with tailored pore size, surface, and pore chemistry are promising alternatives. Thanks to the compositional modularity of MOFs and polymer–MOF composites, herein we report on a series of water-stable zirconium carboxylate MOFs and their low-cost polymer-grafted composites as C<sub>8</sub>–PFAS adsorbents with benchmark kinetics and “parts per billion” removal efficiencies. Bespoke insights into the structure–function relationships of PFAS adsorbents are obtained by leveraging interfacial design principles on solid sorbents, creating a synergy between the extrinsic particle surfaces and intrinsic molecular building blocks.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"71 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142685135","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}
Joo-Hong Lee, Sung-Kwang Jung, Gimoon Kim, Ji-Sang Park, Keonwoo Park, Cheol-Woong Yang, Jin-Wook Lee
{"title":"High Thermal Conductive Crystalline Organohalide for Endurable Resistive Switching Non-Volatile Memory","authors":"Joo-Hong Lee, Sung-Kwang Jung, Gimoon Kim, Ji-Sang Park, Keonwoo Park, Cheol-Woong Yang, Jin-Wook Lee","doi":"10.1002/adma.202413020","DOIUrl":"https://doi.org/10.1002/adma.202413020","url":null,"abstract":"The organic-based memristive devices are widely studied as a next-generation electronics for eco-friendly wearable applications, thanks to materials` flexibility and biocompatibility. However, poor operational reliability and stability of the devices remain a critical challenge. Here, the study demonstrates a crystalline organohalide, Dabconium ammonium triiodide (DABCO-NH<sub>4</sub>-I<sub>3</sub>, DABCO is 1,4-diazabicyclo[2.2.2] octonium)-based memristive device with exceptionally high reliability and endurance. Owing to the low dielectric constant and anisotropic hexagonal crystal structure consisting of hydrogen bonds with a high bandgap, the DABCO-NH<sub>4</sub>-I<sub>3</sub>-based conductive bridging random access memory device demonstrates millivolt-scale operating voltages with a remarkably high on/off ratio of ≈10<sup>9</sup>, capable of multi-level storage. The relatively higher thermal conductivity of the crystalline organohalide (1.06 W m<sup>−1</sup>K<sup>−1</sup>), compared to most of organic materials (0.1–0.5 W m<sup>−1</sup>K<sup>−1</sup>), is found to be beneficial to suppress intense heat accumulation generated by Joule heating effect during device operation. With the facilitated dissipation of the generated heat, the simple planar heterojunction structured device shows remarkably endurable resistive switching over 10<sup>3</sup> cycles of program-erase at both room temperature and 85 °C with high switching reliability. This study introduced a new class of materials that can overcome the limitations of existing organic materials for high-performance next-generation organic electronic devices.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"17 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142684989","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}
Su Hyun Choi, Seungwoo Shin, Woo Young Kim, Je Min Lee, Seo Rim Park, Hyuntae Kim, Kyoohee Woo, Sin Kwon, Nicholas X Fang, Seok Kim, Young Tae Cho
{"title":"Scalable Multistep Roll-to-Roll Printing of Multifunctional and Robust Reentrant Microcavity Surfaces via a Wetting-Induced Process.","authors":"Su Hyun Choi, Seungwoo Shin, Woo Young Kim, Je Min Lee, Seo Rim Park, Hyuntae Kim, Kyoohee Woo, Sin Kwon, Nicholas X Fang, Seok Kim, Young Tae Cho","doi":"10.1002/adma.202411064","DOIUrl":"https://doi.org/10.1002/adma.202411064","url":null,"abstract":"<p><p>Owing to their unique structural robustness, interconnected reentrant structures offer multifunctionality for various applications. a scalable multistep roll-to-roll printing method is proposed for fabricating reentrant microcavity surfaces, coined as wetting-induced interconnected reentrant geometry (WING) process. The key to the proposed WING process is a highly reproducible reentrant structure formation controlled by the capillary action during contact between prefabricated microcavity structure and spray-coated ultraviolet-curable resins. It demonstrates the superior liquid repellency of the WING structures, which maintain large contact angles even with low-surface-tension liquids, and their robust capability to retain solid particles and liquids under external forces. In addition, the scalable and continuous fabrication approach addresses the limitations of existing methods, providing a cost-effective and high-throughput solution for creating multifunctional reentrant surfaces for anti-icing, biofouling prevention, and particle capture.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":" ","pages":"e2411064"},"PeriodicalIF":27.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142685440","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}
Ben Chen, Chencheng Peng, Runda Guo, Zhiyuan He, Liang Sun, Feihu Zhang, Xiping He, Haibo Zeng, Lei Wang
{"title":"Dual-Function Self-Assembled Molecules as Hole-Transport Layers for Thermally Evaporated High-Efficiency Blue Perovskite Light-Emitting Diodes","authors":"Ben Chen, Chencheng Peng, Runda Guo, Zhiyuan He, Liang Sun, Feihu Zhang, Xiping He, Haibo Zeng, Lei Wang","doi":"10.1002/adma.202411451","DOIUrl":"https://doi.org/10.1002/adma.202411451","url":null,"abstract":"Thermally evaporated perovskite light-emitting diodes (PeLEDs) hold immense potential for future applications in the display industry. However, the performance of blue PeLEDs is far behind, one of the most important reasons is the lack of suitable hole-transporting materials. Herein, the study designs and synthesizes a new class of self-assembled monolayer (SAM) materials, namely, (2-(3,6-bis(4-formylphenyl)-9H-carbazol-9-yl)ethyl)phosphonic acid (<b>C-2PACz)</b> and (2-(3,6-bis(4-(methylsulfonyl)phenyl)-9H-carbazol-9-yl)ethyl)phosphonic acid (<b>S-2PACz)</b>. First, the phosphonic acid is induced to form bidentate bonds with ITO. Second, the strong electron-withdrawing groups are integrated to increase the electron cloud density of the termini contacting with perovskite, which enhances the electrostatic interaction with the Pb<sup>2+</sup>, reduces the interfacial defects. These advantages improve their carrier transport ability and reduce the non-radiative recombination at the interface. Meanwhile, it is found that compound <b>C-2PACz</b> possessing the smaller steric hindrance makes the SAMs have a more homogeneous film and a better interfacial passivation effect. By employing <b>C-2PACz</b> as hole-transporting layer in blue PeLEDs with metal halides as the emitting layer, the device exhibits a high brightness (1843 cd m<sup>−2</sup>) and a maximum external quantum efficiency (10.41% @65.59 cd m<sup>−2</sup>), which among the best of reported thermally evaporated sky-blue PeLEDs. The work provides new insights into design strategies for dual-function SAMs to achieve higher performance in PeLEDs.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"18 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142684984","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}