Accounts of materials research最新文献

{"title":"","authors":"","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 6","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":14.0,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/mrv006i006_1951933","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144489186","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}

{"title":"","authors":"Hengrui Zhang, Alexandru B. Georgescu, Suraj Yerramilli, Christopher Karpovich, Daniel W. Apley, Elsa A. Olivetti, James M. Rondinelli* and Wei Chen*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 6","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":14.0,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/accountsmr.5c00011","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144489193","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}

{"title":"","authors":"Yoonhee Kim, Yuna Kwak, Jihyeon Choi and Jwa-Min Nam*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 6","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":14.0,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/accountsmr.5c00043","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144489189","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}

{"title":"","authors":"Zhixue Liu, Junyi Chen and Chunju Li*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 6","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":14.0,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/accountsmr.5c00071","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144489187","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}

{"title":"Multifunctional Spin-Dependent Tunneling: From Tunnel Magnetodielectric to Magneto-Optic and Faraday Effects","authors":"Yang Cao*, Nobukiyo Kobayashi, Hanae Kijima-Aoki, Jun Zhang and Hiroshi Masumoto*, ","doi":"10.1021/accountsmr.5c00113","DOIUrl":"10.1021/accountsmr.5c00113","url":null,"abstract":"<p >Magnetic granular nanocomposites, consisting of magnetic nanogranules dispersed within a host matrix, represent a versatile class of functional materials that enable control over electrical, magnetic, and thermal properties at the nanoscale. Over the past decade, by leveraging electrons as carriers of spin, charge, and heat, these features have enabled the discovery of a family of tunnel related phenomena: tunnel magnetoresistance (TMR), tunnel magneto-Seebeck (TMS), tunnel magnetodielectric (TMD), and most recently tunnel magneto-optical (TMO) effects. Their structural features allow for tuning of granular size, distribution, and intergranular spacing, positioning these materials as promising candidates for miniaturized magnetic field sensors, antennas, microwave devices, and spintronic components.</p><p >In this Account, we summarize our recent advances in understanding TMD effects in complex granular nanocomposites over the past decade. We begin by illustrating how key structural parameters, including intergranular spacing, granule distribution, and magnetic granule composition, govern dielectric variations. From a theoretical standpoint, we derive a formula that predicts the maximum achievable dielectric change. Experimentally, we show that introducing small amounts of ferromagnetic species to balance the ferromagnetic and superparamagnetic components in a nanogranular composite greatly enhances low-field sensitivity. Moreover, by integrating silicon into the films to improve interfaces, the TMD response (i.e., the maximum dielectric variation) reaches a record 8.5% under a 10 kOe magnetic field. We also investigate the heterostructures, such as gradient and multilayer architectures, which effectively broaden the TMD frequency range. Based on the established mechanism of spin-dependent charge oscillations, we demonstrate that optical transmittance in these nanocomposites can be regulated via an external magnetic field (the TMO effect). Transparent FeCo–AlF<sub>3</sub> films exhibit magneto-tunable transmittance across the visible-NIR range, while fluoride- and nitride-based nanogranular films yield giant Faraday rotations, which is more than 40 times greater than that of Bisubstituted yttrium iron garnet. Additionally, we have introduced our recent discovery in granular nanocomposites, including giant Faraday rotation as well as electrically tunable dielectric properties. We demonstrate electric-field control of dielectric relaxation in Co–MgF<sub>2</sub>, enabling MHz-range tunable capacitors driven by a DC bias.</p><p >Finally, we outline the key challenges and future directions in TMD research. Further progress will rely on continued exploration of novel material combinations, including the design of compositionally graded multilayers and heterostructures that couple TMD-active layers with magnonic or photonic elements. Integrating nanogranular films into CMOS-compatible platforms and silicon photonic circuits may open pathways toward ","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 8","pages":"979–990"},"PeriodicalIF":14.7,"publicationDate":"2025-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144237478","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}

{"title":"Promise and Perspectives of Garnet-Based Anode-Free Solid-State Batteries","authors":"Jiayun Wen, Yiming Dai, Qian Yu, Zhiyuan Ouyang, Wei Luo* and Yunhui Huang*, ","doi":"10.1021/accountsmr.4c00129","DOIUrl":"10.1021/accountsmr.4c00129","url":null,"abstract":"<p >With the rapid advancement of energy storage technologies, lithium-ion batteries (LIBs) based on graphite anodes and liquid organic electrolytes have achieved remarkable progress. Nevertheless, the limited specific capacity of graphite anodes and the safety concerns associated with organic electrolytes hinder further enhancement of LIBs. In pursuit of higher energy density and improved safety, solid-state Li metal batteries (SSLMBs) have drawn significant attention. Furthermore, anode-free solid-state batteries (AFSSBs), as a particularly promising innovation in the field of energy storage, have gained increasing interest in recent years. With increasing research investment and continuous technological optimization, AFSSBs hold great potential for widespread applications including electric vehicles, grid energy storage, and beyond.</p><p >Central to AFSSBs, solid-state electrolytes (SSEs) are crucial for achieving high energy density and performance. Among the various SSEs, garnet-type oxide SSEs stand out as one of the most promising systems due to their favorable thermodynamic stability with Li metal anodes, excellent ionic conductivity (∼10<sup>–3</sup> S cm<sup>–1</sup>), and wide electrochemical window (>6 V). However, poor solid–solid interface contact and the growth of Li dendrite have led to sluggish interfacial ion and electron transfer kinetics, thereby impeding the commercialization of garnet-based AFSSBs. Although previous reviews have highlighted interfacial challenges and summarized corresponding mitigation strategies, specific case studies remain scarce and a comprehensive understanding of interfacial dynamics in garnet-based AFSSBs has not yet been established.</p><p >In this Account, we critically evaluate the unique advantages of garnet-based AFSSBs, including their enhanced energy density and improved safety, compared to conventional battery technologies. Additionally, we summarize current understanding primarily from the perspective of interfacial dynamics, covering Li nucleation and growth mechanisms, interfacial evolution at the garnet/current collector interface during Li deposition, and dendrite growth behaviors, aiming to provide deeper insights into interfacial dynamics. Building upon this, we summarize the major interfacial challenges in garnet-based AFSSBs that significantly hinder the interfacial ion and electron transport. In order to enhance the interfacial charge transfer kinetics, we discuss critical parameters, including the properties of the garnet electrolyte and current collector as well as the interfacial wettability at the Li/garnet and Li/current collector interface. Furthermore, we present an overview of our innovative strategy designed to improve interfacial contact and Li-ion transport between the garnet electrolyte and current collector. Finally, we summarize the progress and provide an outlook for garnet-based AFSSBs, exploring their future improvements and development directions toward practica","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 7","pages":"902–913"},"PeriodicalIF":14.7,"publicationDate":"2025-06-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144237479","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}

{"title":"Wet Spinning Enabled Advanced PEDOT:PSS Composite Fibers for Smart Devices","authors":"Haodi Zeng, Chunxia Gao*, Yuanyuan Yu, Mengjin Jiang, Tingyin Deng and Jiadeng Zhu*, ","doi":"10.1021/accountsmr.5c00076","DOIUrl":"10.1021/accountsmr.5c00076","url":null,"abstract":"<p >Poly(3,4-ethylenedioxythiophene): poly(styrenesulfonate) (PEDOT:PSS) is a derivative of polythiophene and an intrinsically conductive polymer (CP). Due to its excellent conductivity, processability, and biocompatibility, it has received widespread attention in the past decade and has become a popular material for wearable electronic devices. Thin films and fibers are the two primary dimensions that PEDOT:PSS has been made into. Compared with two-dimensional (2D) thin films, 1D fibers have natural advantages in integration and structural design, remarkably accelerating practical applications.</p><p >Wet spinning has been considered the primary method to fabricate 1D PEDOT:PSS fibers, which can continuously produce fibers on a large scale with the outstanding capability of fine-tuning the compositions and morphologies to achieve the desired properties. For example, untreated wet-spun PEDOT:PSS fibers generally have relatively lower conductivity (0.1 S·cm<sup>–1</sup>), while the coagulation bath obtained by mixing acetone and isopropanol significantly increases the conductivity (310 S·cm<sup>–1</sup>), which has become a classic combination. Nevertheless, the extensive use of such solvents does not meet the requirements of environmental friendliness, and researchers have been searching for suitable alternatives. Even though the coagulation bath composed of ethanol, water, and metal salts compensates for improving that, the performance needs further enhancement, including conductivity, elongation at break, and capacitance. Thus, intensive efforts have been taken to boost the performance of PEDOT:PSS by changing the formula of the coagulation bath, blending other additives with the starting materials, and secondary treatment for the obtained fibers. In addition to ethanol and water, other coagulation baths are also being developed, such as sulfuric acid, N, N-dimethylacetamide, etc., which play a critical role in the above solutions due to the excellent performance of the resultant fibers.</p><p >In this <i>Account</i>, the efforts are mainly concentrated on the advancements and progress in achieving high-performance wet-spun PEDOT:PSS fibers, from coagulation bath regulation to secondary treatment of spinning solution blending. The fundamental electrochemistry and challenges of PEDOT:PSS fibers will also be discussed. It will then focus on the advantages and control mechanisms of preparing PEDOT:PSS fibers through wet spinning from three perspectives: (i) coagulation bath control; (ii) polymer blending; and (iii) post-treatment. For example, we will discuss: 1) how different additives in the coagulation bath regulate the structure and properties of PEDOT:PSS fibers; 2) how polymer blending can improve the stability and durability of PEDOT:PSS fibers; and 3) how post-treatment can endow PEDOT:PSS fibers with unique structures, enhancing their strength and conductivity. Finally, the key research directions required in this field and the remaining ","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 8","pages":"952–963"},"PeriodicalIF":14.7,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144237481","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}

{"title":"Biomimetic Bone Tissue Engineering Scaffolds Combined with Physical Stimulation to Reconstruct Piezoelectric Network for Functional Regeneration in Critical Bone Defects","authors":"Qihong Li,&nbsp;Chen Li,&nbsp;Xiaomei Bie,&nbsp;Jianzheng Zhang and Yantao Zhao*,&nbsp;","doi":"10.1021/accountsmr.5c00029","DOIUrl":"10.1021/accountsmr.5c00029","url":null,"abstract":"<p >In addition to supporting and protecting mobility, bone is essential for regulating systemic homeostasis. Large bone defects have always been a clinical challenge because of their complicated composition and structure, which makes them difficult to repair on their own. Currently, clinical operations employ primarily autologous, allogeneic, and synthetic bone grafting methods, which are still limited by factors such as donor scarcity, complications from infections, and market acceptance. Thus, novel biomimetic artificial bone tissue engineering scaffolds can be created by designing and regulating the composition and structure of materials, drawing inspiration from the intrinsic properties of genuine bone tissue. The combined application of bioactive substances and biomaterials in bone repair has achieved multiple satisfactory clinical outcomes. In this Account, based on the principles of bionic tissue engineering, we constructed various bone repair scaffolds through multidimensional approaches and systematically evaluated their capabilities in vascular regeneration, nerve ingrowth, and osteogenesis. The technological development of scaffolds demonstrated a distinct progressive relationship: The initial stage focused on the bionics of natural bone tissue’s matrix and structure; the advanced stage integrated bioactive components like BMP2 to achieve functional osteoinduction; the deepening stage introduced piezoelectric signals to directly regulate the osteogenic function of scaffolds, while simultaneously controlling angiogenesis and nerve ingrowth to indirectly promote bone repair and regeneration. Ultimately, an innovative bone repair paradigm based on “Piezoelectric Network Theory” was proposed. Extracellular matrix (ECM) engineered scaffolds were reconstructed to provide endogenous effects through surface morphology modulation and bioactive component modification. The synergistic responses between endogenous effect and exogenous physical stimulation achieve rapid repair of a variety of large segmental bone defects in various areas. This advancement will establish new theoretical foundations for functional bone reconstruction and significantly enhance the treatment efficacy for large segmental bone defects.</p>","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 7","pages":"828–841"},"PeriodicalIF":14.7,"publicationDate":"2025-06-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144210993","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}

{"title":"3D Graphene for Energy Technologies: Chemical Strategies and Industrial Challenges","authors":"Bibhuti Kumar Jha,&nbsp;Jong-Chul Yoon and Ji-Hyun Jang*,&nbsp;","doi":"10.1021/accountsmr.4c00381","DOIUrl":"10.1021/accountsmr.4c00381","url":null,"abstract":"<p >Graphene, a groundbreaking two-dimensional (2D) material, has attracted significant attention across various fields due to its exceptional properties. However, 2D graphene sheets tend to restack or agglomerate, reducing their performance and active surface area. To overcome these limitations and expand graphene’s potential applications, researchers have developed three-dimensional (3D) graphene structures with diverse architectures, including 3D graphene fibers, foams, aerogels, hydrogels, tubes, and cages. These structures, along with modifications such as functionalization, doping, preintercalation, and compositing, prevent stacking and enhance specific properties for targeted applications.</p><p >3D graphene’s high surface area, mechanical stability, lightweight nature, and abundant active sites make it ideal for applications requiring superior optical properties, thermal and electronic conductivity, and structural stability. Additionally, its unique architecture and chemical modifications facilitate efficient electron, ion, and mass transport. This makes 3D graphene highly suitable for various applications, including batteries, solar cells, supercapacitors, water splitting, and solar desalination.</p><p >Despite these advancements, further improvements are needed to enhance the commercial feasibility and adaptability of 3D graphene. A deeper understanding of how synthesis techniques and chemical modifications influence its properties is crucial, as current knowledge remains limited. Achieving precise control over its properties during the transition from 2D graphene or polymers to 3D graphene also remains a significant challenge. Additionally, while graphene prices have decreased over the years, it remains relatively expensive compared to alternative materials, and scaling up production while maintaining high quality continues to be a major barrier.</p><p >In this Account, we provide a comprehensive analysis of various synthesis methods and chemical modifications of 3D graphene, emphasizing its transformative potential across energy storage, energy conversion, and environmental applications. We explore a range of chemical strategies, including the manipulation of structural building blocks, preintercalation, doping, compositing, functionalization, and synthesis, and their effects on different applications. By highlighting recent advancements in 3D graphene research and addressing the challenges hindering its commercial adoption, we aim to underscore its significance and the critical challenges that remain in its development and application within materials science and engineering.</p>","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 7","pages":"799–813"},"PeriodicalIF":14.7,"publicationDate":"2025-06-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144193003","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}

{"title":"4D Synchrotron X-ray Nanoimaging for Early Age Cement Curing: Where Are We and Where Should We Go?","authors":"Miguel A.G. Aranda*,&nbsp;","doi":"10.1021/accountsmr.5c00018","DOIUrl":"10.1021/accountsmr.5c00018","url":null,"abstract":"&lt;p &gt;The production of cement is a key indicator of a region’s level of development. As such, its use is essential for any society aiming to create healthy, comfortable, safe and secure living and working environments. However, these benefits come at a price; Portland cement production accounts for ≈8% of the total anthropogenic CO&lt;sub&gt;2&lt;/sub&gt; emissions. If cement fabrication was considered a country, it would rank as the third largest emitter, after China and the United States. Consequently, reducing the CO&lt;sub&gt;2&lt;/sub&gt; footprint of the construction industry is a societal need. Numerous low-carbon cement alternatives have been proposed, primarily involving the partial substitution of Portland clinker with materials that possess much lower CO&lt;sub&gt;2&lt;/sub&gt; footprints. However, these cements have not been widely adopted because they exhibit reduced mechanical strength at 1 day of hydration, failing to meet current practices for formwork stripping. Therefore, a primary objective is to elucidate the mechanisms of early age cement hydration to accelerate their hydration rates.&lt;/p&gt;&lt;p &gt;Portland cement and low-carbon cements are complex, multimineral materials comprising at least seven crystalline components. Additionally, during the hydration process, new hydrate phases – both crystalline and amorphous – are formed, resulting in the development of intricate, time-dependent microstructures. The compositional and spatial complexity, along with the inherent heterogeneity, underscores the necessity for additional analytical tools such as 3D synchrotron X-ray imaging techniques. Furthermore, as dissolution and precipitation processes are time-dependent, advanced 4D (3D + time) imaging tools are essential. Many pertinent features, such as alite etch-pits, alite reaction zone, and calcium silicate hydrate (C–S–H) gel shells and needles, are submicrometric in size, necessitating the use of &lt;i&gt;4D synchrotron X-ray nanoimaging&lt;/i&gt;. Consequently, various synchrotron X-ray imaging techniques are presented, with a particular emphasis on those leveraging the coherent properties of synchrotron radiation, which are better suited for 4D nanoimaging. The five stringent requirements necessary for obtaining relevant results to investigate early age cement hydration are thoroughly discussed. Following this, examples of such studies are presented, highlighting the key data that can be obtained. Both the advantages and current limitations of these techniques are addressed. Particular emphasis is placed on the spatial dissolution rates of alite, which seem to be strongly dependent on the initial particle sizes. Additionally, descriptors related to the C–S–H gel shells, such as growth rate and densification over time, are provided. Unfortunately, to date, 4D nanoimaging lacks the temporal and spatial resolution required to measure the growth rates of C–S–H gel needles. However, optimized beamlines at fourth-generation synchrotron sources are expected to enable these types of studi","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 7","pages":"814–827"},"PeriodicalIF":14.7,"publicationDate":"2025-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/accountsmr.5c00018","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177270","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}