Stephan Müssig, Andreas Wolf, Tero Kämäräinen and Karl Mandel*,
{"title":"","authors":"Stephan Müssig, Andreas Wolf, Tero Kämäräinen and Karl Mandel*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 7","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":14.0,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/accountsmr.5c00027","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144696192","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}
Yu-Wu Zhong*, Meng-Jia Sun, Chun-Yun Ding, Zhong-Qiu Li and Jiannian Yao*,
{"title":"","authors":"Yu-Wu Zhong*, Meng-Jia Sun, Chun-Yun Ding, Zhong-Qiu Li and Jiannian Yao*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 7","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":14.0,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/accountsmr.5c00052","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144696196","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}
Kostiantyn V. Kravchyk*, Matthias Klimpel, Huanyu Zhang and Maksym V. Kovalenko*,
{"title":"","authors":"Kostiantyn V. Kravchyk*, Matthias Klimpel, Huanyu Zhang and Maksym V. Kovalenko*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 7","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":14.0,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/accountsmr.5c00124","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144696191","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":"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":"<p >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.</p><p >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-CO<sub>2</sub>), 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-CO<sub>2</sub> 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-CO<sub>2</sub> 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.</p><p >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 × 10<sup>10</sup> A·W<sup>–1</sup> and detectivity of 1.62 × 10<sup>16</sup> 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<sup>–19</sup> M for methylglyoxal and 10<sup>–10</sup> 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}
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":"<p >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 H<sub>2</sub> by <i>in vivo</i> monitoring of H<sub>2</sub> transportation, metabolism and transformation, enhancement of H<sub>2</sub> therapeutic efficacy against various oxidative stress-related diseases by high-efficiency and site-specific delivery and controlled release of H<sub>2</sub>, <i>etc</i>. As the smallest and weakly reductive molecule, H<sub>2</sub> 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 H<sub>2</sub> in varied pathological microenvironments, such as inflammation, cancer, and injured tissue, have not been well elucidated. Moreover, as a therapeutic agent, the pharmacokinetics of H<sub>2</sub>, 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 H<sub>2</sub>, 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 H<sub>2</sub>-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.</p><p >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 <i>in vivo</i> H<sub>2</sub> detection, the understanding of H<sub>2</sub> 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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