Accounts of materials research最新文献

{"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}

{"title":"Toward Ideal Biointerfacing Electronics Using Organic Electrochemical Transistors","authors":"Peiyun Li,&nbsp; and ,&nbsp;Ting Lei*,&nbsp;","doi":"10.1021/accountsmr.5c00030","DOIUrl":"10.1021/accountsmr.5c00030","url":null,"abstract":"<p >The biointerface between biological tissues and electronic devices serves as a medium for matter transport, signal transmission, and energy conversion. However, significant disparities in properties, such as mechanical modulus and water content, between tissues and electronics, present a key challenge in bioelectronics, leading to biointerface mismatches that severely impact their performance and long-term stability. Organic electrochemical transistors (OECTs), fabricated with soft, hydrophilic organic semiconductors, offer unique advantages, including low operating voltage, high transconductance, and compatibility with aqueous environments. These attributes position OECTs as promising candidates for ideal biointerfaces. As neural probes, OECTs have demonstrated superior biocompatibility and signal detection capabilities compared to conventional metal electrodes and inorganic semiconductors. Despite these advantages, the applications of OECT as biointerfaces remain constrained by several limitations, including limited performance, poor stability, mismatches among p-type, n-type, and ambipolar semiconductors, relatively high Young’s modulus, and unsatisfactory biointerfacial properties.</p><p >In this Account, we summarize our group’s efforts to improve both the electronic and biointerfacial properties of OECTs, encompassing structure–property relationship studies, device optimization/fabrication, and biointerface enhancement. To elucidate the structure–property relationship, we explored the material design strategies and device optimization approaches for high-performance OECTs, highlighting the critical role of doped state properties in the OECT system. Recognizing the unique characteristics of OECTs, we designed hydrophilic polymer backbones to replace conventional neutral ones. These hydrophilic ionic backbones foster strong intermolecular interactions, resulting in improved operational stability. Additionally, we demonstrate that constructing high-spin polymers enables the development of high-performance, balanced ambipolar materials. Based on these materials innovations, we advanced fabrication methods of OECT-based logic circuits and fiber-based OECTs, realizing complementary and ambipolar logic circuits, as well as wearable fabric-based biosensors. Finally, we integrated the exceptional biointerface properties of hydrogels with organic semiconductors, pioneering semiconducting hydrogels that exhibit outstanding mechanical, electrical, and biointerfacial properties. These materials enable efficient in vivo amplification of electrophysiological signals. The concept and realization of semiconducting hydrogels redefine the scope of OECTs and hydrogel electronics, providing a novel approach to ideal biointerfaces. We hope that the perspectives shared in this Account will inspire the development of next generation bioelectronic devices with enhanced biointerface compatibility and expanded functionalities.</p>","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 7","pages":"853–864"},"PeriodicalIF":14.7,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165743","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":"Microscale Bipolar Interfaces for High-Power Fuel Cells","authors":"Jianping Chen,&nbsp;Kritika Sharma,&nbsp;Zhongyang Wang*,&nbsp;Shrihari Sankarasubramanian* and Vijay Ramani*,&nbsp;","doi":"10.1021/accountsmr.5c00039","DOIUrl":"10.1021/accountsmr.5c00039","url":null,"abstract":"<p >Electrochemical devices are typically designed for operation over a narrow pH range and are constrained in the choice of catalysts and operating potentials by the pH environment of the electrodes. This is the result of a heretofore lack of a viable strategy to maintain pH gradients between the electrodes over practically significant time durations with only a minimal impact on the device performance. While bipolar interfaces are well-known, they typically result in high junction potential losses that make them impractical in real-life systems. We have demonstrated a way to overcome this long-standing challenge using our tailor-made, microscale bipolar interfaces, which allows the use of acidic electrolytes at one electrode and alkaline electrolytes at the other, without mixing over time. This allows for a much broader selection of fuel and oxidant stream catalysts (moving away from platinum group metals) and electrolytes to be used. Low-temperature aqueous fuel cells have been constrained in their operating voltage to ca. 1.2–1.5 V (as a function of fuel and oxidant combination) by the water splitting side reactions (hydrogen evolution reaction (HER) and oxygen evolution reaction (OER)). This relatively low cell voltage translates to larger stack volumes for a desired power output and poor specific power output. By employing our pH-gradient enabled microscale bipolar interfaces (PMBIs) we have demonstrated aqueous direct borohydride fuel cells (DBFC) that provide a 2.4 times higher power density at 1.5 V, compared to state-of-the-art polymer electrolyte membrane fuel cells (PEMFCs) that typically operate at 0.75 V. This Account traces the &gt;10 year development of PMBIs. We detail the development of a recessed planar electrode that provided experimental evidence that the PMBI was able to maintain a sharp local pH gradient (0.82 pH units nm^–1 on average) at the electrocatalytic reaction sites. We go on to trace the evolution of a series of highly selective anion exchange ionomer (AEIs) that enabled ever higher intercell pH gradients and culminated in the demonstration of the highest power operation of a bipolar DBFC reported in the literature. PMBIs have also enabled recent developments in high power bipolar direct methanol- and direct ethanol fuel cells (DMFC and DEFC) employing hydrogen peroxide oxidants. PMBI-based DMFC and DEFC achieved open-circuit voltages near their theoretical maxima (∼1.7 V and ∼1.65 V, respectively). Emerging strategies such as molecular modeling-guided ionomer design, self-healing bipolar interfaces, and optoelectronic coupling represent promising future directions to further enhance PMBI stability, ion transport efficiency, and expand their practical applicability in high-performance electrochemical energy conversion devices.</p>","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 7","pages":"865–875"},"PeriodicalIF":14.7,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144137206","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":"Brightening the Microcrystals of Polyazine Iridium and Ruthenium Complexes via Light-Harvesting Energy Transfer","authors":"Yu-Wu Zhong*,&nbsp;Meng-Jia Sun,&nbsp;Chun-Yun Ding,&nbsp;Zhong-Qiu Li and Jiannian Yao*,&nbsp;","doi":"10.1021/accountsmr.5c00052","DOIUrl":"10.1021/accountsmr.5c00052","url":null,"abstract":"<p >Luminescent nano/micro molecular crystals with well-defined shapes and morphologies have exhibited great potential for various photonic applications. The molecular orientation and packing greatly influence the optical and electronic characters of the crystals. Noncovalent intermolecular interactions can not only determine the growth direction but also induce the formation of polymorphs, bringing more possibilities for the property optimization and functional applications. Besides, light-harvesting energy transfer (LHEnT) is a vital process in natural photosynthesis, the mimic of which provides a simple and practical means for solar energy conversion and the preparation of luminescent materials. With an energy donor and acceptor pair with suitable energy levels and similar molecular size and solubility, it is convenient to fabricate LHEnT molecular crystals with tunable optoelectronic and emission properties by dispersing acceptors into the donor lattices.</p><p >We describe in this Account our recent research progress on the use of octahedral iridium (Ir^III) and ruthenium (Ru^II) complexes to prepare luminescent crystals for potential applications in nanophotonics. By introducing simple substituents on the coordination ligands, such as a methyl group, fluoro atom, and trifluoromethyl group, as the functional unit to direct assembly, we have been able to obtain well-defined nano/microcrystals from these complexes. Furthermore, by using a molecular doping strategy accompanied by the LHEnT process, the obtained binary crystals show efficient and tunable luminescence properties. With these endeavors, we have realized the luminescence amplification of an Ir^III energy acceptor that suffers severely from the aggregation-caused quenching effect. Molecular crystals with high-performance linearly polarized luminescence, circularly polarized luminescence, and electrochemiluminescence have been prepared, and their applications in polarized light waveguides and chemical sensing have been demonstrated. By using a stepwise binary assembly method, optical heterostructures are prepared to show their potential in optical information processing and thermosensing.</p>","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 7","pages":"876–888"},"PeriodicalIF":14.7,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144130121","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":"","authors":"Zhiqiang Sun,&nbsp;Zhen Dong,&nbsp;Feng Yu,&nbsp;Sitong Feng and Zhong-Ren Chen*,&nbsp;","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 5","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":14.0,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/accountsmr.5c00057","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144447716","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":"Wei Gong*,&nbsp;Yifei Gao,&nbsp;Jinqiao Dong,&nbsp;Yan Liu* and Yong Cui*,&nbsp;","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 5","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":14.0,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/accountsmr.4c00337","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144447719","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":"Yulian Liu,&nbsp;Yi Wei and Zewei Quan*,&nbsp;","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 5","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":14.0,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/accountsmr.5c00033","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144359334","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":"Information-Providing Magnetic Supraparticles: Particle Designs to Record Environmental Stimuli with Readout by Magnetic Particle Spectroscopy","authors":"Stephan Müssig,&nbsp;Andreas Wolf,&nbsp;Tero Kämäräinen and Karl Mandel*,&nbsp;","doi":"10.1021/accountsmr.5c00027","DOIUrl":"10.1021/accountsmr.5c00027","url":null,"abstract":"&lt;p &gt;The ability to gather information about materials and products, such as their origin, physicochemical properties or history of experienced environmental stimuli, is valuable for quality control, predictive maintenance, delivery tracking, recycling, and more. Integrating additives capable of recording and storing information into materials offers a flexible approach to create “materials intelligence”. Common strategies utilize luminescent markers or DNA sequences that enable object identification and environmental impact monitoring.&lt;/p&gt;&lt;p &gt;In contrast to optical methods limited to surface-level analysis, magnetic fields penetrate materials, enabling nondestructive readout even from the inside of opaque or multicomponent objects. While magnetic particle technologies have traditionally been used for biosensing and imaging with highly sensitive instruments like magnetic resonance imaging, these methods are unsuitable for quick, on-site analysis of macroscopic objects. During the past decade, magnetic particle spectroscopy (MPS) has emerged as a faster and more accessible characterization technique. MPS measures the magnetic response of particles in ambient conditions under alternating fields, offering high temporal resolution (∼1–10 s) and more geometric freedom than other magnetometry techniques.&lt;/p&gt;&lt;p &gt;Magnetic nanoparticles are a widely studied material class that have been synthesized and optimized, e.g., for various MPS-based application scenarios and to obtain fundamental understanding of magnetic particle systems. Supraparticles (SPs) represent the next structural hierarchy level, as they are composed of one or multiple types of (magnetic) nanoparticles in a defined particulate structure. By ingenious control of structure and composition of such SPs, we have shown that various kinds of information can be obtained from them upon readout with MPS.&lt;/p&gt;&lt;p &gt;In this Account, we present SP design concepts facilitating to obtain information about environmental stimuli (e.g., temperature, moisture, UV light, chemical gases) based on irreversible spectral magnetic signal changes upon readout with MPS. Initially, the state of the art on nanoparticles, which provide information by stimulus-induced agglomeration, is summarized. Subsequently, SPs consisting of multiple different nanoparticle types and their capabilities to obtain information on environmental stimuli are considered. Specifically, the advantages of using one or more signal transducing magnetic nanoparticle types used in conjunction with one or more nonmagnetic secondary materials susceptible to the desired environmental stimuli (sensitizer) are discussed. Finally, our latest findings on pronounced large-scale SP structure formation (millimeter-scale) through strongly interacting SPs and their implications on the integration of SPs in macroscopic objects of interest are described. Each of the three structural hierarchy levels, namely nanoparticles, SPs, and the macroscopic object of intere","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 7","pages":"842–852"},"PeriodicalIF":14.7,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144122765","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":"","authors":"","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 5","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":14.0,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/mrv006i005_1938592","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144359335","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}