Xiao-Yu Dong, Hong Chen, Shan Wang, Ru-Yi Zou, Shuang-Quan Zang, Jinmeng Cai
{"title":"Introducing La into a Customized Dual Cu Covalent Organic Framework to Steer CO2 Electroreduction Selectivity from C2H4 to CH4","authors":"Xiao-Yu Dong, Hong Chen, Shan Wang, Ru-Yi Zou, Shuang-Quan Zang, Jinmeng Cai","doi":"10.1002/adma.202413710","DOIUrl":"https://doi.org/10.1002/adma.202413710","url":null,"abstract":"Customizing multi-metal site catalysts for achieving controllable CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) product tuning holds immense promise yet poses formidable challenges. The traditional synthesis method of multi-metal sites is the pyrolysis of metal-containing precursors, which is inherently uncontrollable. Herein, a bottom-up strategy is employed to customize and synthesize multi-metal sites in covalent organic frameworks (COFs), aiming to controllably switch the CO<sub>2</sub> reduction selectivity by regulating the electronic structure of active sites. Briefly, La element provides chances for manipulating and finetuning the electronic structure of the customized dual Cu sites, and converts the main catalytic product of CO<sub>2</sub>RR from ethylene to methane. Density functional theory calculations show that the introduction of La alters the electronic structure around Cu, enhances CO<sub>2</sub> and H<sub>2</sub>O activation, and changes the formation of energy barriers of key intermediates. To the best of the author's knowledge, this study constructed the first example of customized multi-metal site COF catalysts and provided new ideas for controllable modulation of products.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"11 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841614","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}
Sung Bae Park, Hojung Kwak, Dohoon Lee, Giyoung Shin, Min Jang, Hyuni Jung, Hyeonyeol Jeon, Hyo Jeong Kim, Jeyoung Park, Dongyeop X. Oh
{"title":"Development of Marine-Degradable Poly(Ester Amide)s with Strong, Up-Scalable, and Up-Cyclable Performance","authors":"Sung Bae Park, Hojung Kwak, Dohoon Lee, Giyoung Shin, Min Jang, Hyuni Jung, Hyeonyeol Jeon, Hyo Jeong Kim, Jeyoung Park, Dongyeop X. Oh","doi":"10.1002/adma.202417266","DOIUrl":"https://doi.org/10.1002/adma.202417266","url":null,"abstract":"Biodegradable polyesters provide an attractive alternative to non-degradable plastics but often encounter a tradeoff between biodegradability and mechanical properties because esters are rotational and lack hydrogen bonds. Conversely, natural polyamides, i.e., silk exhibit excellent mechanical strength because amides are non-rotational and form hydrogen bonds. Unlike esters, the nitrogen in amides can enhance microbial biodegradation. However, protein engineering exhibits limited productivity, and artificial polyamides, i.e., nylon remain non-degradable due to their hydrophobic nature. Herein, a method is proposed for developing poly(ester amide)s (PEA)s, a polyester and polyamide hybrid, to address prevailing production challenges. These materials are synthesized from upcycled monomers in a 10 L reactor and converted into films and yarns. They achieve a tensile strength of 109 MPa and tenacity of 5.0 g de<sup>−1</sup>, while withstanding ironing temperatures. They achieve a remarkable 92% marine biodegradability in 12 months, which is rarely attained by current bioplastics, and exhibit low environmental impact in terms of greenhouse gas emissions. While biodegradable polyesters have remained within the performance range of commodity plastics, PEAs fall into the high-performance category, potentially reaching markets that existing biodegradable plastics have not, such as fishing lines and clothing.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"14 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841152","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":"Advanced Design for Stimuli-Reversible Chromic Wearables With Customizable Functionalities","authors":"Tiandi Chen, Qingjun Yang, Cuiqin Fang, Shenzhen Deng, Bingang Xu","doi":"10.1002/adma.202413665","DOIUrl":"https://doi.org/10.1002/adma.202413665","url":null,"abstract":"Smart wearable devices with dynamically reversible color displays are crucial for the next generation of smart textiles, and promising for bio-robots, adaptive camouflage, and visual health monitoring. The rapid advancement of technology brings out different categories that feature fundamentally different color-reversing mechanisms, including thermochromic, mechanochromic, electrochromic, and photochromic smart wearables. Although some reviews have showcased relevant developments from unique perspectives, reviews focusing on the advanced design of flexible chromic wearable devices within each category have not been reported. In this review, the development history and recent progress in smart chromic wearables across each category are systematically examined. The design strategies for each chromic wearable device are outlined with a focus on functional materials, synthesis processes, and advanced applications. Furthermore, integrated devices based on dual-stimuli and multi-stimuli responsive chromics with customizable functionalities are summarized. Finally, challenges and perspectives on the future development of smart chromic wearables are proposed. Such a systematic summary will serve as a valuable insight for researchers in this field.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"10 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841159","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}
Shuting Wang, Zhenqing Wang, Zhenjie Zang, Xiaojie Liang, Bin Jia, Tan Ye, Yang Lan, Xuetao Shi
{"title":"A Mitochondrion-Targeting Piezoelectric Nanosystem for the Treatment of Erectile Dysfunction via Autophagy Regulation","authors":"Shuting Wang, Zhenqing Wang, Zhenjie Zang, Xiaojie Liang, Bin Jia, Tan Ye, Yang Lan, Xuetao Shi","doi":"10.1002/adma.202413287","DOIUrl":"https://doi.org/10.1002/adma.202413287","url":null,"abstract":"Mitochondrial damage caused by external stimuli, such as high glucose levels and inflammation, results in excessive reactive oxygen species (ROS) production. Existing antioxidants can only scavenge ROS and cannot address the root cause of ROS production, namely, abnormal mitochondria. To overcome this limitation, the study develops a piezoelectric synergistic drug-loaded nanosystem (BaTCG nanosystem) that targets mitochondria. The BaTCG nanosystem is delivered to mitochondria via triphenylphosphine modification, and generates current under the stimulation of ultrasound, thereby promoting mitochondrial autophagy and restoring mitochondrial homeostasis. In a model of diabetes-related erectile dysfunction (ED), the BaTCG nanosystem, through the current induced by the piezoelectric effect, not only promoted mitophagy, thereby reducing ROS production, but also released long-acting glucagon-like peptide-1 receptor agonists (GLP-1RAs) to effectively reduce blood glucose levels and mitochondrial damage. Each component of this nanosystem functions individually as well as synergistically, thus facilitating corpus cavernosum repair and restoring erectile function. In conclusion, the findings offer a novel therapeutic strategy for diabetes-related ED and a target for the treatment of diabetes-related conditions with functionalized nanoparticles to regulate mitophagy.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"88 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832756","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":"Programmable Morphology-Adaptive Peptide Nanoassembly for Enhanced Catalytic Therapy","authors":"Xue-Hao Zhang, Ben-Li Song, Ning-Bo Yi, Guang-Xu Zhang, Wen-Fu Zheng, Dong-Bing Cheng, Zeng-Ying Qiao, Hao Wang","doi":"10.1002/adma.202417089","DOIUrl":"https://doi.org/10.1002/adma.202417089","url":null,"abstract":"Nanocatalytic therapy holds significant promise in cancer treatment by exploiting the high oxidative stress within tumor cells. However, efficiently delivering nanocatalytic agents to tumor tissues and maximizing their catalytic activity in situ remain critical challenges. Morphology-adaptive delivery systems, capable of adjusting their physical form in response to physiological conditions, offer unique spatiotemporal control for navigating complex biological environments like the tumor microenvironment. While designing systems that undergo multiple shape transformations often involves complex stimuli-responsive mechanisms, making programmable responses through simple designs highly desirable yet challenging. Here, FeFKC, an innovative adaptive material is introduced that achieves multi-step morphological transformations at the tissue level and amplifies catalytic activity through a straightforward design. As the microenvironmental pH decreases during drug delivery, FeFKC dynamically transitions between single chains, nanoparticles, and nanofibers. This programmable shape-shifting facilitates deep tumor penetration, enhanced cellular uptake, and lysosomal escape, significantly improving its catalytic efficiency in nanocatalytic tumor therapy. In vivo studies demonstrate that FeFKC achieves impressive tumor suppression efficacy of up to 95% without notable biosafety concerns. The findings highlight the potential of adaptive nanomaterials with programmable shape-transforming capabilities to overcome biological barriers and enhance catalytic therapy, opening new avenues for cancer treatment and other complex diseases.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"5 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832761","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}
Yan-Peng Feng, Han Wu, Yin-Lian Zhu, Yu-Jia Wang, Yun-Long Tang, Xiu-Liang Ma
{"title":"Reversible Manipulation of Polar Topologies in Oxide Ferroelectrics via Electric Fields","authors":"Yan-Peng Feng, Han Wu, Yin-Lian Zhu, Yu-Jia Wang, Yun-Long Tang, Xiu-Liang Ma","doi":"10.1002/adma.202414346","DOIUrl":"https://doi.org/10.1002/adma.202414346","url":null,"abstract":"Polar topologies show great potentials in memories and other nano-micro devices. To integrate with silicon conducting circuits, it is vital to understand the dynamic evolution and the transformation of different domain configurations under external stimulus. Here in situ transmission electron microscopy is performed and the electrically controlled creation and annihilation of large-scale polar flux-closure array from typical <i>c/a</i> domains in PbTiO<sub>3</sub>/SrTiO<sub>3</sub> bilayers is directly observed. It is found that the transformation is reversible after removal of external electric fields. Increasing external electric fields on (PbTiO<sub>3</sub>/SrTiO<sub>3</sub>)<sub>5</sub> multilayered films, it is further found that the flux-closure domains are nucleated and propagated via the steps of first the formation of new <i>c</i> domains and then connection with neighboring <i>c</i> domains. The transition from <i>a</i>/<i>c</i> domains to flux-closure arrays under electric fields is collaborated with evaluating energy variations by phase-field simulations in which the electrostatic energy plays an important role. These results demonstrate the polar topologies can be reversibly manipulated by external stimuli, which sheds light on further understanding the dynamics behavior of polar topologies and helps for future nanoelectric applications.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"24 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841155","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":"Tunable Electron Correlation in Epitaxial 1T-TaS2 Spirals","authors":"Chung-Jen Chen, Chun-An Chen, Yu-Hsiang Cheng, Chia-Tzu Chung, Yu-Ting Lin, Yi-Cheng Chiang, Ting-Kuo Lee, Yi-Hsien Lee","doi":"10.1002/adma.202413926","DOIUrl":"https://doi.org/10.1002/adma.202413926","url":null,"abstract":"Tantalum disulfide (1T-TaS<sub>2</sub>), being a Mott insulator with strong electron correlation, is highlighted for diverse collective quantum states in the 2D lattice, including charge density wave (CDW), spin liquid, and unconventional superconductivity. The Mott physics embedded in the 2D triangular CDW lattice has raised debates on stacking-dependent properties because interlayer interactions are sensitive to van der Waals (vdW) spacing. However, control of interlayer distance remains a challenge. Here, spiral lattices in the epitaxial TaS<sub>2</sub> spirals are studied to probe collective properties with tunable interlayer interactions. A scalable synthesis of epitaxial TaS<sub>2</sub> spirals is presented. A more than 50%-increased interlayer spacing enables prototype decoupled monolayers for enhanced electronic correlation exhibiting Mott physics at room-temperature and a simplified system to explore collective properties in vdW materials.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"64 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841615","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":"Polyphenol Mediated Assembly: Tailored Nano-Dredger Unblocks Axonal Autophagosomes Retrograde Transport Traffic Jam for Accelerated Alzheimer's Waste Clearance","authors":"Ran Meng, Yixian Li, Xiyu Yang, Yunlong Cheng, Minjun Xu, LingLing Zhou, Chengqin Wu, Shuai Yu, Wenyi Huang, Tianying Wang, Qizhi Zhang","doi":"10.1002/adma.202413614","DOIUrl":"https://doi.org/10.1002/adma.202413614","url":null,"abstract":"Clear-cut evidence has linked defective autophagy to Alzheimer's disease (AD). Recent studies underscore a unique hurdle in AD neuronal autophagy: impaired retrograde axonal transport of autophagosomes, potent enough to induce autophagic stress and neurodegeneration. Nonetheless, pertinent therapy is unavailable. Here, a novel combinational therapy composed of siROCK2 and lithospermic acid B (LA) is introduced, tailored to dredge blocked axonal autophagy by multi-mitigating microtubule disruption, ATP depletion, oxidative stress, and autophagy initiation impediments in AD. Leveraging the recent discovery of multi-interactions between polyphenol LA and siRNA, ε-Poly-L-lysine, and anionic lipid nanovacuoles, LA and siROCK2 are successfully co-loaded into a fresh nano-drug delivery system, LIP@PL-LA/siRC, via a ratio-flexible and straightforward fabrication process. Further modification with the TPL peptide onto LIP@PL-LA/siRC creates a brain-neuron targeted, biocompatible, and pluripotent nanomedicine, named “Nano-dredger” (T-LIP@PL-LA/siRC). Nano-dredger efficiently accelerates axonal retrograde transport and lysosomal degradation of autophagosomes, thereby facilitating the clearance of neurotoxic proteins, improving neuronal complexity, and alleviating memory defects in 3×Tg-AD transgenic mice. This study provides a fresh and flexible polyphenol/siRNA co-delivery paradigm and furnishes conceptual proof that dredging axonal autophagy represents a promising AD therapeutic avenue.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"26 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832824","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":"Engineering Mild-Photothermal Responsive and NO Donor Prussian Blue Nanozymes Using Mild Synthesis for Inflammation Regulation and Bacterial Eradication in Periodontal Disease","authors":"Zheng Li, Xiaowan Fan, Ying Liu, Muxin Yue, Tingting Wu, Xing Wang, Wei Jiang, Kelong Fan","doi":"10.1002/adma.202409840","DOIUrl":"https://doi.org/10.1002/adma.202409840","url":null,"abstract":"Periodontitis, an infectious disease of periodontal tissues caused by oral bacterial biofilms, is characterized by reactive oxygen species (ROS) accumulation and immune microenvironment imbalance. Multifunctional nanozymes, leveraging their physiochemical properties and enzymatic activities, offer promising antibacterial and anti-inflammatory strategies for managing periodontitis. In particular, Prussian blue nanozymes (PBzymes) exhibit exceptional ROS control due to their robust catalytic activity, diverse antioxidant functions, and high biocompatibility. However, the practical application of traditional high-temperature synthesis methods is limited. This study introduces a class of metal-engineered PBzymes synthesized at room temperature, identified for their potent antioxidative activity and excellent photothermal performance at mild temperatures. Nitric oxide (NO) gas therapy offers promising strategies for targeting deep infections in periodontal tissues. Thus, sodium nitroprusside is introduced into PBzyme to create SPBzyme via an in situ loading method. NO release by SPBzyme enhances antibacterial effects and overcomes resistance linked to bacterial biofilms, resulting in mild-photothermal antibacterial properties and synergistic antioxidant effects. In vitro antibacterial assays demonstrate the superior efficacy of SPBzyme under mild temperature conditions and near-infrared light exposure. Furthermore, SPBzyme effectively reduces inflammation and has positive therapeutic effects in periodontal animal models. Overall, mild-temperature photothermal NO release nanozyme therapy represents a novel approach for treating periodontitis.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"14 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841613","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":"Recent Progress and Challenges of Li-Rich Mn-Based Cathode Materials for Solid-State Lithium-Ion Batteries","authors":"Qiqiang Huang, Jinquan Liu, Xinman Chen, Peng Zhang, Languang Lu, Dongsheng Ren, Minggao Ouyang, Xiang Liu","doi":"10.1002/adma.202410006","DOIUrl":"https://doi.org/10.1002/adma.202410006","url":null,"abstract":"Li-rich Mn-based (LRM) cathode materials, characterized by their high specific capacity (>250 mAh g<sup>−</sup>¹) and cost-effectiveness, represent promising candidates for next-generation lithium-ion batteries. However, their commercial application is hindered by rapid capacity degradation and voltage fading, which can be attributed to transition metal migration, lattice oxygen release, and the toxicity of Mn ions to the anode solid electrolyte interphase (SEI). Recently, the application of LRM cathode in all-solid-state batteries (ASSBs) has garnered significant interest, as this approach eliminates the liquid electrolyte, thereby suppressing transition metal crosstalk and solid–liquid interfacial side reactions. This review first examines the historical development, crystal structure, and mechanisms underlying the high capacity of LRM cathode materials. It then introduces the current challenges facing LRM cathode and the associated degradation mechanisms and proposes solutions to these issues. Additionally, it summarizes recent research on LRM materials in ASSBs and suggests strategies for improvement. Finally, the review discusses future research directions for LRM cathode materials, including optimized material design, bulk doping, surface coating, developing novel solid electrolytes, and interface engineering. This review aims to provide further insights and new perspectives on applying LRM cathode materials in ASSBs.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"10 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832758","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}