Accounts of materials research最新文献_第2页

IF 14

Accounts of materials research Pub Date : 2025-07-25

Stephan Müssig, Andreas Wolf, Tero Kämäräinen and Karl Mandel*,

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IF 14

Accounts of materials research Pub Date : 2025-07-25

Peiyun Li, and , Ting Lei*,

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IF 14

Accounts of materials research Pub Date : 2025-07-25

Yu-Wu Zhong*, Meng-Jia Sun, Chun-Yun Ding, Zhong-Qiu Li and Jiannian Yao*,

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IF 14

Accounts of materials research Pub Date : 2025-07-25

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IF 14

Accounts of materials research Pub Date : 2025-07-25

Kostiantyn V. Kravchyk*, Matthias Klimpel, Huanyu Zhang and Maksym V. Kovalenko*,

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Supercritical Solvothermal Synthesis of Single-Crystalline Covalent Organic Frameworks and Their Applications 单晶共价有机骨架的超临界溶剂热合成及其应用

IF 14.7

Accounts of materials research Pub Date : 2025-07-22 DOI: 10.1021/accountsmr.5c00118

Lan Peng*, Yunqi Liu and Dacheng Wei*,

{"title":"Supercritical Solvothermal Synthesis of Single-Crystalline Covalent Organic Frameworks and Their Applications","authors":"Lan Peng*, Yunqi Liu and Dacheng Wei*, ","doi":"10.1021/accountsmr.5c00118","DOIUrl":"https://doi.org/10.1021/accountsmr.5c00118","url":null,"abstract":"Covalent organic frameworks (COFs) are a rapidly evolving class of crystalline porous materials with customizable topologies, tunable functionalities, and a broad scope of applications ranging from catalysis to optoelectronics. Despite substantial progress in framework design, the controlled growth of single-crystalline COFs remains a formidable challenge due to the relatively poor reversibility of covalent bond formation and the difficulty in modulating nucleation and growth kinetics. Traditional solvothermal strategies often yield polycrystalline powders and require prolonged reaction times, limiting access to defect-free structures essential for in-depth structural characterization and advanced functional applications.In this Account, we present the supercritical solvothermal method as a transformative strategy that simultaneously achieves ultrarapid synthesis and high crystallinity of COFs. By leveraging the unique physicochemical properties of supercritical carbon dioxide (sc-CO2), notably its low viscosity, high diffusivity, and tunable solvent density, this method overcomes the trade-off between synthesis duration and crystal quality. This approach enables the synthesis of single-crystalline COFs in a few minutes, compared to hours or days in conventional systems. Mechanistically, sc-CO2 facilitates dynamic mass transport and enhanced molecular mobility, which accelerate nucleation while promoting defect self-healing during framework propagation. Time-resolved characterization combined with template infiltration experiments reveals that the exceptional penetrability of sc-CO2 enables framework formation even within confined micropores and allows for precise morphological tuning of COFs. Furthermore, we demonstrate that weak intermolecular forces such as interlayer electrostatic repulsions and hydrogen bonding can be amplified under supercritical fluid conditions to modulate crystal morphology, leading to the formation of rare helical COF crystals and enabling structure manipulation via rational side-group engineering.Single-crystalline COFs exhibit specific properties and potential applications, particularly in nonlinear optics, optoelectronics, and chemical sensing. These crystals display high second harmonic generation efficiencies due to their noncentrosymmetric packing, as well as robust third-order nonlinear responses enabled by chromophore alignment and π-electron delocalization. In optoelectronic applications, dual-state COF phototransistors demonstrate room-temperature responsivity of ∼4.6 × 1010 A·W–1 and detectivity of 1.62 × 1016 Jones, enabling high-contrast neuromorphic imaging under low-light and aqueous conditions. In chemical sensing applications, COF/graphene heterostructures synthesized via this method deliver unprecedented detection limits, down to 10–19 M for methylglyoxal and 10–10 M for mercury ions in biofluids","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 8","pages":"991–1005"},"PeriodicalIF":14.7,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144885149","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

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Hydrogen Medicine Materials 氢医药材料

IF 14.7

Accounts of materials research Pub Date : 2025-07-17 DOI: 10.1021/accountsmr.5c00144

Chao Xia, Lingdong Jiang, Zhaokui Jin and Qianjun He*,

{"title":"Hydrogen Medicine Materials","authors":"Chao Xia, Lingdong Jiang, Zhaokui Jin and Qianjun He*, ","doi":"10.1021/accountsmr.5c00144","DOIUrl":"https://doi.org/10.1021/accountsmr.5c00144","url":null,"abstract":"Hydrogen medicine materials are defined as a new concept of biomedical materials specifically engineered to overcome critical challenges in hydrogen medicine, including exploration of biological effects and mechanisms of H2 by in vivo monitoring of H2 transportation, metabolism and transformation, enhancement of H2 therapeutic efficacy against various oxidative stress-related diseases by high-efficiency and site-specific delivery and controlled release of H2, etc. As the smallest and weakly reductive molecule, H2 exhibits some unique biological characteristics, including high tissue permeability, antioxidative stress (OS), anti-inflammation, antiapoptosis, antisenescence, pro-regeneration/pro-self-repairing, anticancer, antibiofilm, high biocompatibility, and biosafety, holding a high value of biomedical applications. However, the related biological mechanisms are not very clear. Typically, multifaceted biological behaviors of H2 in varied pathological microenvironments, such as inflammation, cancer, and injured tissue, have not been well elucidated. Moreover, as a therapeutic agent, the pharmacokinetics of H2, involving absorption, biodistribution, metabolism, and excretion, has to be clarified before clinical application, which needs the development of hydrogen bioprobes to resolve. Based on high biosafety and therapeutic validity of H2, both hydrogen gas inhalator and hydrogen-rich water generator have been clinically approved for adjuvant therapy of some respiratory and digestive system diseases including chronic obstructive pulmonary disease (COPD), hyperuricemia, hyperlipemia, gastrelcosis and coprostasis, but they hardly realize effective delivery toward remote diseased focuses. Therefore, efficient, site-specific and controlled/sustained H2-delivering materials with high biosafety urgently need to be developed for improving the outcome of hydrogen therapy. Based on these unique advantages and unsolved key issues in hydrogen medicine, hydrogen medicine materials as an emerging interdisciplinary field have attracted increasing attention in recent years.In this Account, we present a brief overview of the recent advances of hydrogen medicine materials including hydrogen bioprobes and hydrogen-delivering materials (hydrogen carriers, hydrolytic hydrogen-generating materials, and catalytic hydrogen-generating materials), as well as their typical biomedical applications including targeted inflammation therapy, targeted tumor therapy, and local tissue repair/regeneration. Finally, a forward-looking perspective on hydrogen medicine materials is demonstrated, which attempts to address the current clinical challenges in the field of hydrogen medicine. Especially, the development of small molecular bioprobes for in vivo H2 detection, the understanding of H2 pharmacokinetics and potential bioeffects,","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 8","pages":"1020–1032"},"PeriodicalIF":14.7,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144885266","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

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Stable Metal–Organic Frameworks for Air and Water Pollution Control 稳定金属-有机框架用于空气和水污染控制

IF 14.7

Accounts of materials research Pub Date : 2025-07-16 DOI: 10.1021/accountsmr.5c00138

Guang-Rui Si, Tao He, Xiang-Jing Kong, Lin-Hua Xie and Jian-Rong Li*,

{"title":"Stable Metal–Organic Frameworks for Air and Water Pollution Control","authors":"Guang-Rui Si, Tao He, Xiang-Jing Kong, Lin-Hua Xie and Jian-Rong Li*, ","doi":"10.1021/accountsmr.5c00138","DOIUrl":"https://doi.org/10.1021/accountsmr.5c00138","url":null,"abstract":"Industrial emissions, agricultural runoff, and waste discharge have introduced numerous hazardous pollutants into ecosystems, including volatile organic compounds (VOCs), toxic gases (e.g., SO2, NOx, and O3), heavy metal ions, and organic contaminants (e.g., dyes, antibiotics). These pollutants pose significant risks to environmental sustainability and human health, contributing to respiratory illnesses, waterborne diseases, and environmental harm. To address these challenges, there is an urgent need for advanced materials that can efficiently and selectively capture and degrade pollutants. Metal–organic frameworks (MOFs), with their modular nature, precise architectures, and tunable functionalities, have attracted considerable attention for environmental remediation. Their structural diversity enables the incorporation of active sites such as open metal sites, functionalized ligands, and hierarchical pores, facilitating targeted interactions with a broad range of pollutants. Despite these advantages, the practical application of MOFs remains limited by their chemical instability under harsh environmental conditions (e.g., extreme pH, oxidative or reductive atmospheres). Most MOFs are prone to degrade via ligand displacement or framework collapse, posing a significant barrier to their use in environmental remediation.This Account provides a comprehensive overview of our recent advances in the rational design and synthesis of chemically robust MOFs for the efficient capture, degradation, and detection of air and water pollution. First, we outline a combined strategy that integrates thermodynamic stabilization through strong metal–ligand coordination and kinetic enhancement via framework interpenetration and high connectivity, ensuring structural integrity under environmental conditions. Crystal engineering enables the incorporation of versatile binding sites, such as open metal sites and low-coordination nodes, while ligand design enhances electronic properties and luminescence response for selective detection. Additionally, precise control of the pore microenvironment improves molecular transport and pollutant binding efficiency. These synergistic approaches have been successfully demonstrated across a wide range of applications, including VOC adsorption and photocatalytic degradation, the removal of reactive, toxic gases (e.g., O3, SO2, NH3), and the detection and remediation of organic contaminants, heavy metal ions, and radioactive species in water. Finally, we also discuss ongoing challenges and future directions essential for the practical application of stable MOFs in environmental remediation. This work aims to provide design principles and valuable insights that will advance the development of next-generation MOFs as sustainable platforms for comprehensive environmental pollution control.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 8","pages":"1006–1019"},"PeriodicalIF":14.7,"publicationDate":"2025-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144885243","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

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Microswimmers That Flex: Advancing Microswimmers with Templated Assembly and Responsive DNA Nanostructures 微游泳者，Flex：推进微游泳者与模板组装和响应DNA纳米结构

IF 14.7

Accounts of materials research Pub Date : 2025-07-14 DOI: 10.1021/accountsmr.5c00009

Taryn Imamura, Sarah Bergbreiter and Rebecca E. Taylor*,

{"title":"Microswimmers That Flex: Advancing Microswimmers with Templated Assembly and Responsive DNA Nanostructures","authors":"Taryn Imamura, Sarah Bergbreiter and Rebecca E. Taylor*, ","doi":"10.1021/accountsmr.5c00009","DOIUrl":"https://doi.org/10.1021/accountsmr.5c00009","url":null,"abstract":"The concept of micrometer-scale swimming robots, also known as microswimmers, navigating the human body to perform robotic tasks has captured the public imagination and inspired researchers through its numerous representations in popular media. This attention highlights the enormous interest in and potential of this technology for biomedical applications, such as cargo delivery, diagnostics, and minimally invasive surgery, as well as for applications in microfluidics and manufacturing. To achieve the collective behavior and control required for microswimmers to effectively perform such actions within complex, in vivo and microfluidic environments, they must meet a strict set of engineering criteria. These requirements include, but are not limited to, small size, structural monodispersity, flexibility, biocompatibility, and multifunctionality. Additionally, microswimmers must be able to adapt to delicate environments, such as human vasculature, while safely performing preprogrammed tasks in response to chemical and mechanical signals.Naturally information-bearing biopolymers, such as peptides, RNA, and DNA, can provide programmability, multifunctionality, and nanometer-scale precision for manufactured structures. In particular, DNA is a useful engineering material because of its predictable and well-characterized material properties, as well as its biocompatibility. Moreover, recent advances in DNA nanotechnology have enabled unprecedented abilities to engineer DNA nanostructures with tunable mechanics and responsiveness at nano- and micrometer scales. Incorporating DNA nanostructures as subcomponents in microswimmer systems can grant these structures enhanced deformability, reconfigurability, and responsiveness to biochemical signals while maintaining their biocompatibility, providing a versatile pathway for building programmable, multifunctional micro- and nanoscale machines with robotic capabilities.In this Account, we highlight our recent progress toward the experimental realization of responsive microswimmers made with compliant DNA components. We present a hybrid top-down, bottom-up fabrication method that combines templated assembly with structural DNA nanotechnology to address the manufacturing limitations of flexibly linked microswimmers. Using this method, we construct microswimmers with enhanced structural complexity and more controlled particle placement, spacing, and size, while maintaining the compliance of their DNA linkage. We also present a novel experimental platform that utilizes two-photon polymerization (TPP) to fabricate millimeter-scale swimmers (milliswimmers) with fully customizable shapes and integrated flexible linkers. This platform addresses limitations related to population-level heterogeneity in micrometer-scale systems, allowing us to isolate the effects of milliswimmer designs from variations in their physical dimensions. Using this platform, we interrogate established hydrodynamic models of m","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 8","pages":"927–938"},"PeriodicalIF":14.7,"publicationDate":"2025-07-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/accountsmr.5c00009","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144885242","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

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Machine-Learning-Assisted Molecular Design of Innovative Polymers 创新聚合物的机器学习辅助分子设计

IF 14.7

Accounts of materials research Pub Date : 2025-07-09 DOI: 10.1021/accountsmr.5c00151

Tianle Yue, Jianxin He and Ying Li*,

{"title":"Machine-Learning-Assisted Molecular Design of Innovative Polymers","authors":"Tianle Yue, Jianxin He and Ying Li*, ","doi":"10.1021/accountsmr.5c00151","DOIUrl":"https://doi.org/10.1021/accountsmr.5c00151","url":null,"abstract":"A new paradigm driven by artificial intelligence (AI) and machine learning (ML) is significantly accelerating the iterative pace of polymer materials research. Traditional experimental approaches to polymer discovery have long relied on trial and error, requiring extensive time and resources while offering limited access to the vast chemical design space. In contrast, ML-assisted strategies provide a transformative framework for efficiently navigating this complex landscape. This paper focuses specifically on polymer design at the molecular level. By integrating data-driven methodologies, researchers can extract structure–property relationships, predict polymer properties, and optimize molecular architectures with unprecedented speed. ML-driven polymer design follows a structured approach: (1) database construction, (2) structural representation and feature engineering, (3) development of ML-based property prediction models, (4) virtual screening of potential candidates, and (5) validation through experiments and/or numerical simulations. This workflow faces two central challenges. First is the limited availability of high-quality polymer datasets, particularly for advanced materials with specialized properties. Second is the generation of virtual polymer structures. Unlike small-molecule drug discovery, where vast libraries of candidate compounds exist, polymer chemistry lacks an equivalent repository of hypothetical structures. Recent efforts have leveraged rule-based polymerization reactions and generative models to create large-scale databases of hypothetical polymers, significantly expanding the design space. Additionally, the diversity of polymer structures, the broad range of their properties, and the limited availability of training samples add complexity to developing accurate predictive models. Addressing these challenges requires innovative ML techniques, such as transfer learning, multitask learning, and generative models, to extract meaningful insights from sparse data and improve prediction reliability. This data-driven approach has enabled the discovery of novel, high-performance polymers for applications in aerospace, electronics, energy storage, and biomedical engineering. Despite these advancements, several hurdles remain. The interpretability of ML models, particularly deep neural networks, is a pressing concern. While black-box models can achieve remarkable predictive accuracy, understanding their decision-making processes remains challenging. Explainable AI methods are increasingly being explored to provide insights into feature importance, model uncertainty, and the underlying chemistry driving polymer properties. Additionally, the synthesizability and processability of ML-generated candidates must be carefully considered to ensure practical experimental validation and real-world application. In this paper, we review recent progress in ML-assisted molecular design of polymer materials, focusing on database development, f","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 8","pages":"1033–1045"},"PeriodicalIF":14.7,"publicationDate":"2025-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144885154","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0