Smart materials serve as the fundamental cornerstone supporting humanity's transition into the intelligent era. Smart materials possess the capability to perceive external stimuli and respond accordingly. Light-controlled smart materials (LCSMs) are a significant category that can sense and respond to light stimuli. Light, being a non-invasive, precisely regulated, and remotely controllable source of physical stimulation, makes LCSMs indispensable in certain application scenarios. Recently, the construction of LCSMs using supramolecular strategies has emerged as a significant research focus. Supramolecular assembly, based on non-covalent bonding, offers dynamic, reversible, and biomimetic properties. By integrating supramolecular systems with photoresponsive molecular building blocks, these materials can achieve synergistic and rich intelligent stimulus responses. This review delves into the latest research advancements in LCSMs based on supramolecular strategies. There are four sections in this review. The first section defines LCSMs and outlines their advantages. The second section discusses the design approaches of supramolecular LCSMs. The third section highlights the latest advancements on supramolecular LCSMs over the past 3 years. The fourth section summarizes the current research and provides insights into the future development of this field.
{"title":"Light-controlled smart materials: Supramolecular regulation and applications","authors":"Zi-Hao Liao, Feng Wang","doi":"10.1002/smo.20240036","DOIUrl":"https://doi.org/10.1002/smo.20240036","url":null,"abstract":"Smart materials serve as the fundamental cornerstone supporting humanity's transition into the intelligent era. Smart materials possess the capability to perceive external stimuli and respond accordingly. Light-controlled smart materials (LCSMs) are a significant category that can sense and respond to light stimuli. Light, being a non-invasive, precisely regulated, and remotely controllable source of physical stimulation, makes LCSMs indispensable in certain application scenarios. Recently, the construction of LCSMs using supramolecular strategies has emerged as a significant research focus. Supramolecular assembly, based on non-covalent bonding, offers dynamic, reversible, and biomimetic properties. By integrating supramolecular systems with photoresponsive molecular building blocks, these materials can achieve synergistic and rich intelligent stimulus responses. This review delves into the latest research advancements in LCSMs based on supramolecular strategies. There are four sections in this review. The first section defines LCSMs and outlines their advantages. The second section discusses the design approaches of supramolecular LCSMs. The third section highlights the latest advancements on supramolecular LCSMs over the past 3 years. The fourth section summarizes the current research and provides insights into the future development of this field.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":"1 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249073","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}
Organic afterglow materials have drawn increasing attention for their great potential in practical applications. Until now, most of them just show the lifetimes in milliseconds or seconds, while the realization of long persistent luminescence (LPL) lasting for minutes or even hours is difficult. In 2017, Adachi and Kabe successfully realize the LPL with a duration longer than 1 hour in a purely organic system, which can be even comparable to some excellent inorganic materials. However, partially for the unclear structure-property relationship, organic LPL materials are still rather scarce, especially for the stable ones in air or aqueous solution. In this review, we present the recent progress in organic LPL, mainly focusing on the material design strategy and internal mechanism. It is anticipated that the deep understanding can be beneficial for the further development of organic LPL materials with good stability in air and even aqueous phase.
{"title":"Recent advances of organic long persistent luminescence: Design strategy and internal mechanism","authors":"Jie Yang, Zhijian Chen, Manman Fang, Zhen Li","doi":"10.1002/smo.20240034","DOIUrl":"https://doi.org/10.1002/smo.20240034","url":null,"abstract":"Organic afterglow materials have drawn increasing attention for their great potential in practical applications. Until now, most of them just show the lifetimes in milliseconds or seconds, while the realization of long persistent luminescence (LPL) lasting for minutes or even hours is difficult. In 2017, Adachi and Kabe successfully realize the LPL with a duration longer than 1 hour in a purely organic system, which can be even comparable to some excellent inorganic materials. However, partially for the unclear structure-property relationship, organic LPL materials are still rather scarce, especially for the stable ones in air or aqueous solution. In this review, we present the recent progress in organic LPL, mainly focusing on the material design strategy and internal mechanism. It is anticipated that the deep understanding can be beneficial for the further development of organic LPL materials with good stability in air and even aqueous phase.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":"39 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249074","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}
A binder-free Ru@NiMoS electrode was engineered by in situ growth of two-dimensional NiMoS nanosheets on nickel foam. This process effectively promoted the electrostatic-driven aggregation of Ru(bpy)32+, harnessing the synergistic effect to enhance electrochemiluminescence (ECL) performance. The integration (Ru@NiMoS) achieved an impressive ECL efficiency of 70.1%, marking an impressive 36.9-fold enhancement over conventional Ru. Additionally, its ECL intensity was found to be remarkably 172.2 times greater than that of Ru. Within the Ru(bpy)32+/TPA system, NiMoS emerged as a pivotal electrochemical catalyst, markedly boosting both the oxygen evolution reaction and the generation of reactive intermediates. Leveraging these distinctive properties, a highly efficient ECL sensor for lidocaine detection was developed. This sensor exhibited a linear response within the concentration range of 1 nM to 1 μM and achieved a remarkably low detection limit of 0.22 nM, underlining its substantial potential for practical application.
{"title":"Ru@NiMoS aggregate with boosted electrochemical catalysis for enhanced electrochemiluminescence and lidocaine detection","authors":"Yongzhuang Lu, Haoran Wang, Qiyao Li, Qian Liu, Xiaoxu Zhang, Yuying Jia, Xiangyu Cai, Zheng Zhao, Yanfu Huan, Ben Zhong Tang","doi":"10.1002/smo.20240011","DOIUrl":"https://doi.org/10.1002/smo.20240011","url":null,"abstract":"A binder-free Ru@NiMoS electrode was engineered by in situ growth of two-dimensional NiMoS nanosheets on nickel foam. This process effectively promoted the electrostatic-driven aggregation of Ru(bpy)<sub>3</sub><sup>2+</sup>, harnessing the synergistic effect to enhance electrochemiluminescence (ECL) performance. The integration (Ru@NiMoS) achieved an impressive ECL efficiency of 70.1%, marking an impressive 36.9-fold enhancement over conventional Ru. Additionally, its ECL intensity was found to be remarkably 172.2 times greater than that of Ru. Within the Ru(bpy)<sub>3</sub><sup>2+</sup>/TPA system, NiMoS emerged as a pivotal electrochemical catalyst, markedly boosting both the oxygen evolution reaction and the generation of reactive intermediates. Leveraging these distinctive properties, a highly efficient ECL sensor for lidocaine detection was developed. This sensor exhibited a linear response within the concentration range of 1 nM to 1 μM and achieved a remarkably low detection limit of 0.22 nM, underlining its substantial potential for practical application.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":"65 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249077","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}
Xiaoying Kang, Zekun Du, Shuxuan Yang, Mengyun Liang, Qian Liu, Ji Qi
Precision medicine calls for advanced theranostics that integrate controllable diagnostic and therapeutic capabilities into one platform for disease treatment in the early stage. Phototheranostics such as fluorescence imaging (FLI), photoacoustic imaging (PAI), photodynamic therapy (PDT), and photothermal therapy (PTT) have attracted considerable attention in recent years, which mainly employ different excited-state energy dissipation pathways of a chromophore. According to the Jablonski diagram, FLI is related to the radiative process, PAI and PTT are derived from the nonradiative thermal deactivation, and PDT originates from the triplet state energy, in which these processes are usually competitive. Therefore, it is critically important to precisely tune the photophysical energy transformation processes to realize certain diagnosis and treatment properties in optimal state for boosting biomedical applications. Currently, there are mainly two strategies including chemical structure and aggregate behavior changes that relate to the regulation of excited state energy dissipation. In this review, we will discuss the recent advances of smart molecular probes that the photophysical properties can be regulated by external triggers and their applications in biomedical fields. We will summarize the development of activatable phototheranostic molecular probes in response to stimuli such as reactive oxygen species, pH, light, hypoxia, enzyme and gas. The assembly and disassembly of molecular aggregates that greatly affect the photophysical energy transformation processes will also be highlighted. This review aims to provide valuable insights into the development of more accurate diagnostic and therapeutic systems, thereby advancing the emerging field of smart medicine.
精准医疗需要先进的治疗技术，将可控诊断和治疗功能整合到一个平台中，以便在早期阶段进行疾病治疗。近年来，荧光成像（FLI）、光声成像（PAI）、光动力疗法（PDT）和光热疗法（PTT）等光热学疗法备受关注，它们主要采用了发色团的不同激发态能量耗散途径。根据雅布隆斯基图，FLI 与辐射过程有关，PAI 和 PTT 来自非辐射热失活，而 PDT 则源于三重态能量，这些过程通常是竞争性的。因此，精确调节光物理能量转换过程，使其在最佳状态下实现特定的诊断和治疗特性，对于促进生物医学应用至关重要。目前，与激发态能量耗散调控相关的策略主要有两种，包括化学结构和聚集行为变化。在这篇综述中，我们将讨论可通过外部触发器调节光物理性质的智能分子探针的最新进展及其在生物医学领域的应用。我们将总结针对活性氧、pH 值、光、缺氧、酶和气体等刺激的可激活光热分子探针的发展情况。我们还将重点介绍对光物理能量转化过程有重大影响的分子聚集体的组装和解体。本综述旨在为开发更精确的诊断和治疗系统提供有价值的见解，从而推动智能医学这一新兴领域的发展。
{"title":"Smart molecular probes with controllable photophysical property for smart medicine","authors":"Xiaoying Kang, Zekun Du, Shuxuan Yang, Mengyun Liang, Qian Liu, Ji Qi","doi":"10.1002/smo.20240033","DOIUrl":"https://doi.org/10.1002/smo.20240033","url":null,"abstract":"Precision medicine calls for advanced theranostics that integrate controllable diagnostic and therapeutic capabilities into one platform for disease treatment in the early stage. Phototheranostics such as fluorescence imaging (FLI), photoacoustic imaging (PAI), photodynamic therapy (PDT), and photothermal therapy (PTT) have attracted considerable attention in recent years, which mainly employ different excited-state energy dissipation pathways of a chromophore. According to the Jablonski diagram, FLI is related to the radiative process, PAI and PTT are derived from the nonradiative thermal deactivation, and PDT originates from the triplet state energy, in which these processes are usually competitive. Therefore, it is critically important to precisely tune the photophysical energy transformation processes to realize certain diagnosis and treatment properties in optimal state for boosting biomedical applications. Currently, there are mainly two strategies including chemical structure and aggregate behavior changes that relate to the regulation of excited state energy dissipation. In this review, we will discuss the recent advances of smart molecular probes that the photophysical properties can be regulated by external triggers and their applications in biomedical fields. We will summarize the development of activatable phototheranostic molecular probes in response to stimuli such as reactive oxygen species, pH, light, hypoxia, enzyme and gas. The assembly and disassembly of molecular aggregates that greatly affect the photophysical energy transformation processes will also be highlighted. This review aims to provide valuable insights into the development of more accurate diagnostic and therapeutic systems, thereby advancing the emerging field of smart medicine.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":"5 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249076","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}
Zhirong Zhu, Shichang Liu, Xupeng Wu, Qianqian Yu, Yi Duan, Shanshan Hu, Wei-Hong Zhu, Qi Wang
The development of efficient aggregation-induced emission (AIE) active probes is crucial for disease diagnosis, particularly for tumors and cardiovascular diseases. Current AIE-active probes primarily focus on improving their water solubility to resist aggregation, thereby achieving an initial fluorescence-off state. However, the complex biological environment can cause undesirable aggregation, resulting in false signals. To address this issue, we have ingeniously introduced an azo group into the AIE luminogen (AIEgen), developing a reductase-activated AIE probe, Azo-quinoline-malononitrile (QM)-PN, for imaging hypoxic environments. In this probe, the azo group promotes intramolecular motion through rapid E/Z isomerization, causing the excited state energy to dissipate via non-radiative decay, thus turning off the initial fluorescence. In the presence of reductase, Azo-QM-PN is reduced and cleaved to produce the hydrophobic AIEgen NH2-QM-PN, which subsequently aggregates and generates an in situ AIE signal, thereby imaging the hypoxic environment with reductase. Encapsulation of Azo-QM-PN with DSPE-PEG2000 results in the formation of the nanoprobe Azo-QM-PN NPs, which can effectively penetrate cell membranes, specifically illuminate tumor cells, monitor fluctuations in azo reductase levels, and deeply penetrate and image multicellular tumor spheroids, demonstrating potential for hypoxic tumor imaging. Additionally, the nanoprobe Azo-QM-PN NPs can selectively image hypoxic atherosclerotic plaque tissues, showing potential for detecting atherosclerosis. Therefore, in this study, we successfully developed an enzyme-activated AIE probe for imaging hypoxic environments, laying the foundation for further clinical applications.
{"title":"An azo substituted quinoline-malononitrile enzyme-activable aggregation-induced emission nanoprobe for hypoxia imaging","authors":"Zhirong Zhu, Shichang Liu, Xupeng Wu, Qianqian Yu, Yi Duan, Shanshan Hu, Wei-Hong Zhu, Qi Wang","doi":"10.1002/smo.20240028","DOIUrl":"https://doi.org/10.1002/smo.20240028","url":null,"abstract":"The development of efficient aggregation-induced emission (AIE) active probes is crucial for disease diagnosis, particularly for tumors and cardiovascular diseases. Current AIE-active probes primarily focus on improving their water solubility to resist aggregation, thereby achieving an initial fluorescence-off state. However, the complex biological environment can cause undesirable aggregation, resulting in false signals. To address this issue, we have ingeniously introduced an azo group into the AIE luminogen (AIEgen), developing a reductase-activated AIE probe, Azo-quinoline-malononitrile (QM)-PN, for imaging hypoxic environments. In this probe, the azo group promotes intramolecular motion through rapid <i>E</i>/<i>Z</i> isomerization, causing the excited state energy to dissipate via non-radiative decay, thus turning off the initial fluorescence. In the presence of reductase, Azo-QM-PN is reduced and cleaved to produce the hydrophobic AIEgen NH<sub>2</sub>-QM-PN, which subsequently aggregates and generates an in situ AIE signal, thereby imaging the hypoxic environment with reductase. Encapsulation of Azo-QM-PN with DSPE-PEG<sub>2000</sub> results in the formation of the nanoprobe Azo-QM-PN NPs, which can effectively penetrate cell membranes, specifically illuminate tumor cells, monitor fluctuations in azo reductase levels, and deeply penetrate and image multicellular tumor spheroids, demonstrating potential for hypoxic tumor imaging. Additionally, the nanoprobe Azo-QM-PN NPs can selectively image hypoxic atherosclerotic plaque tissues, showing potential for detecting atherosclerosis. Therefore, in this study, we successfully developed an enzyme-activated AIE probe for imaging hypoxic environments, laying the foundation for further clinical applications.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":"38 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249075","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}
The clinical approval of platinum-based drugs has prompted the development of novel metallo-complexes during the last several decades, while severe problems, especially for poor water solubility, drug resistance and toxicity in patients, greatly hindered the clinical trials and curative efficacy. To address these issues, the concept of metallo-prodrugs has been proposed for oncology. Some stimuli-activable metallo-prodrugs provide new insights for designing and preparing site-specific prodrugs with maximized therapeutic efficacy and negligible unfavorable by-effects. In this review, recent progress in stimuli-activable metallo-prodrugs in the past 20 years has been overviewed, where endogenous and exogenous stimuli have been involved. Typical examples of smart stimuli-activable metallo-prodrugs are discussed regarding to their molecular structure, activation mechanism, and promising biomedical applications. In the end, challenges and future perspectives in metallo-prodrugs have been discussed.
{"title":"Recent progress in stimuli-activable metallo-prodrugs for cancer therapy","authors":"Jinzhe Liang, Fangmian Wei, Hui Chao","doi":"10.1002/smo.20240030","DOIUrl":"https://doi.org/10.1002/smo.20240030","url":null,"abstract":"The clinical approval of platinum-based drugs has prompted the development of novel metallo-complexes during the last several decades, while severe problems, especially for poor water solubility, drug resistance and toxicity in patients, greatly hindered the clinical trials and curative efficacy. To address these issues, the concept of metallo-prodrugs has been proposed for oncology. Some stimuli-activable metallo-prodrugs provide new insights for designing and preparing site-specific prodrugs with maximized therapeutic efficacy and negligible unfavorable by-effects. In this review, recent progress in stimuli-activable metallo-prodrugs in the past 20 years has been overviewed, where endogenous and exogenous stimuli have been involved. Typical examples of smart stimuli-activable metallo-prodrugs are discussed regarding to their molecular structure, activation mechanism, and promising biomedical applications. In the end, challenges and future perspectives in metallo-prodrugs have been discussed.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":"51 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249078","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}
Icing detection is critically important for preventing safety accidents and economic losses, especially concerning ice formation from invalidated anti-icing fluids (water and ethylene glycol) under extreme conditions. Traditional technologies like ultrasonics and capacitor-antenna face challenges with limited detection areas, lower accuracy, and susceptibility to electromagnetic interference. Here, we introduce a novel viscosity-ultrasensitive fluorescent probe 4′,4‴-(2,2-diphenylethene-1,1-diyl) bis-(3,5-dicarboxylate) (TPE-2B4C) based on AIEgens for monitoring ice formation of anti-icing fluids in low-temperature environments. TPE-2B4C, consisting of four sodium carboxylate groups and multiple freely rotating benzene rings, demonstrates outstanding solubility in anti-icing fluids and exhibits no fluorescent background signal even at low temperatures (<−20°C). Upon freezing, TPE-2B4C relocates from the water phase to higher viscosity ethylene glycol, causing restriction of benzene rings and a significantly increased green fluorescence signal. TPE-2B4C can successfully determine whether the anti-icing fluids are icing from −5 to −20°C with a high contrast ratio. Due to its simple setup, fast operation, and broad applicability, our new method is anticipated to be employed for rapid, real-time, and large-scale icing detection.
{"title":"Visual detection of anti-icing fluids freezing by a low-temperature viscosity-sensitive aggregation-induced emission probe","authors":"Honghong Zhang, Fanghui Li, Jiahong Yu, Weijun Zhao","doi":"10.1002/smo.20240014","DOIUrl":"https://doi.org/10.1002/smo.20240014","url":null,"abstract":"Icing detection is critically important for preventing safety accidents and economic losses, especially concerning ice formation from invalidated anti-icing fluids (water and ethylene glycol) under extreme conditions. Traditional technologies like ultrasonics and capacitor-antenna face challenges with limited detection areas, lower accuracy, and susceptibility to electromagnetic interference. Here, we introduce a novel viscosity-ultrasensitive fluorescent probe 4′,4‴-(2,2-diphenylethene-1,1-diyl) bis-(3,5-dicarboxylate) (<b>TPE-2B4C</b>) based on AIEgens for monitoring ice formation of anti-icing fluids in low-temperature environments. <b>TPE-2B4C</b>, consisting of four sodium carboxylate groups and multiple freely rotating benzene rings, demonstrates outstanding solubility in anti-icing fluids and exhibits no fluorescent background signal even at low temperatures (<−20°C). Upon freezing, <b>TPE-2B4C</b> relocates from the water phase to higher viscosity ethylene glycol, causing restriction of benzene rings and a significantly increased green fluorescence signal. <b>TPE-2B4C</b> can successfully determine whether the anti-icing fluids are icing from −5 to −20°C with a high contrast ratio. Due to its simple setup, fast operation, and broad applicability, our new method is anticipated to be employed for rapid, real-time, and large-scale icing detection.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":"28 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249079","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}
In situ precise detection of bioactive molecules with high sensitivity and spatiotemporal resolution is essential for studying physiological events and disease diagnosis. The utilization of versatile fluorescent probes in fluorescence imaging offers a powerful tool for in vivo imaging of biomarkers closely associated with pathological conditions. However, the dynamic behavior leading to rapid clearance of small molecule probes from regions of interest severely compromises their potential for precise imaging. Notably, self-immobilizing fluorescent probes that selectively recognize diseased tissues while improving in situ retention and enrichment enable accurate high-fidelity fluorescence imaging. In this review, we aim to summarize the strategies employed for recent advances in the performance and precision of in vivo fluorescence imaging using self-immobilizing techniques. Lastly, we discuss the prospects and potential challenges associated with self-immobilizing fluorescent probes to promote further development and application of more delicate fluorescent probes.
{"title":"Recent advances in self-immobilizing fluorescent probes for in vivo imaging","authors":"Yong Zhang, Xuemei Lv, Yafu Wang, Xueqian Chen, Jinchao Zhang, Dongdong Su","doi":"10.1002/smo.20240031","DOIUrl":"https://doi.org/10.1002/smo.20240031","url":null,"abstract":"In situ precise detection of bioactive molecules with high sensitivity and spatiotemporal resolution is essential for studying physiological events and disease diagnosis. The utilization of versatile fluorescent probes in fluorescence imaging offers a powerful tool for in vivo imaging of biomarkers closely associated with pathological conditions. However, the dynamic behavior leading to rapid clearance of small molecule probes from regions of interest severely compromises their potential for precise imaging. Notably, self-immobilizing fluorescent probes that selectively recognize diseased tissues while improving in situ retention and enrichment enable accurate high-fidelity fluorescence imaging. In this review, we aim to summarize the strategies employed for recent advances in the performance and precision of in vivo fluorescence imaging using self-immobilizing techniques. Lastly, we discuss the prospects and potential challenges associated with self-immobilizing fluorescent probes to promote further development and application of more delicate fluorescent probes.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":"1 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249082","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}
Robust and reliable piezo-ionic materials that are both crack resistant and self-healable like biological skin hold great promise for applications inflexible electronics and intelligent systems with prolonged service lives. However, such a combination of high toughness, superior crack resistance, autonomous self-healing and effective control of ion dynamics is rarely seen in artificial iontronic skin because these features are seemingly incompatible in materials design. Here, we resolve this perennial mismatch through a molecularly engineered strategy of implanting carboxyl-functionalized groups into the dynamic hard domain structure of synthesized poly(urethane-urea). This design provides an ultra-high fracture energy of 211.27 kJ m−2 that is over 123.54 times that of tough human skin, while maintaining skin-like stretchability, elasticity, and autonomous self-healing with a 96.40% healing efficiency. Moreover, the carboxyl anion group allows the dynamic confinement of ionic fluids though electrostatic interaction, thereby ensuring a remarkable pressure sensitivity of 7.03 kPa−1 for the tactile sensors. As such, we successfully demonstrated the enormous potential ability of this skin-like piezo-ionic sensor for biomedical monitoring and robotic item identification, which indicates promising future uses in flexible electronics and human–machine interactions.
{"title":"Highly tough, crack-resistant and self-healable piezo-ionic skin enabled by dynamic hard domains with mechanosensitive ionic channel","authors":"XueBin Wang, Tong Liu, FuYao Sun, Jingyi Zhang, BoWen Yao, JianHua Xu, JiaJun Fu","doi":"10.1002/smo.20240008","DOIUrl":"https://doi.org/10.1002/smo.20240008","url":null,"abstract":"Robust and reliable piezo-ionic materials that are both crack resistant and self-healable like biological skin hold great promise for applications inflexible electronics and intelligent systems with prolonged service lives. However, such a combination of high toughness, superior crack resistance, autonomous self-healing and effective control of ion dynamics is rarely seen in artificial iontronic skin because these features are seemingly incompatible in materials design. Here, we resolve this perennial mismatch through a molecularly engineered strategy of implanting carboxyl-functionalized groups into the dynamic hard domain structure of synthesized poly(urethane-urea). This design provides an ultra-high fracture energy of 211.27 kJ m<sup>−2</sup> that is over 123.54 times that of tough human skin, while maintaining skin-like stretchability, elasticity, and autonomous self-healing with a 96.40% healing efficiency. Moreover, the carboxyl anion group allows the dynamic confinement of ionic fluids though electrostatic interaction, thereby ensuring a remarkable pressure sensitivity of 7.03 kPa<sup>−1</sup> for the tactile sensors. As such, we successfully demonstrated the enormous potential ability of this skin-like piezo-ionic sensor for biomedical monitoring and robotic item identification, which indicates promising future uses in flexible electronics and human–machine interactions.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":"9 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249080","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}
Surface-supported clusters forming by aggregation of excessive adatoms could be the main defects of 2D materials after chemical vapor deposition. They will significantly impact the electronic/magnetic properties. Moreover, surface supported atoms are also widely explored for high active and selecting catalysts. Severe deformation, even dipping into the surface, of these clusters can be expected because of the very active edge of clusters and strong interaction between supported clusters and surfaces. However, most models of these clusters are supposed to simply float on the top of the surface because ab initio simulations cannot afford the complex reconstructions. Here, we develop an accurate graph neural network machine learning potential (MLP) from ab initio data by active learning architecture through fine-tuning pre-trained models, and then employ the MLP into Monte Carlo to explore the structural evolutions of Mo and S clusters (1–8 atoms) on perfect and various defective MoS2 monolayers. Interestingly, Mo clusters can always sink and embed themselves into MoS2 layers. In contrast, S clusters float on perfect surfaces. On the defective surface, a few S atoms will fill the vacancy and rest S clusters float on the top. Such significant structural reconstructions should be carefully taken into account.
由过多金刚原子聚集形成的表面支撑团簇可能是化学气相沉积后二维材料的主要缺陷。它们会严重影响电子/磁性能。此外，表面支撑原子也被广泛用于高活性和选择性催化剂。由于原子团簇边缘非常活跃，而且支撑原子团簇与表面之间存在强烈的相互作用，因此可以预计这些原子团簇会发生严重变形，甚至浸入表面。然而，由于ab initio 模拟无法进行复杂的重构，因此这些团簇的大多数模型都是简单地漂浮在表面顶端。在这里，我们通过微调预训练模型的主动学习架构，从ab initio数据中开发出精确的图神经网络机器学习势（MLP），然后将MLP应用到蒙特卡洛中，探索完美和各种缺陷MoS2单层上Mo和S团簇（1-8个原子）的结构演变。有趣的是，Mo 团簇总是可以下沉并嵌入 MoS2 层中。相反，S 团簇则漂浮在完美的表面上。在有缺陷的表面上，一些 S 原子会填补空缺，其余的 S 团簇则漂浮在上面。这种重要的结构重构应仔细考虑。
{"title":"Unveiling the unexpected sinking and embedding dynamics of surface supported Mo/S clusters on 2D MoS2 with active machine learning","authors":"Luneng Zhao, Yanhan Ren, Xiaoran Shi, Hongsheng Liu, Zhigen Yu, Junfeng Gao, Jijun Zhao","doi":"10.1002/smo.20240018","DOIUrl":"https://doi.org/10.1002/smo.20240018","url":null,"abstract":"Surface-supported clusters forming by aggregation of excessive adatoms could be the main defects of 2D materials after chemical vapor deposition. They will significantly impact the electronic/magnetic properties. Moreover, surface supported atoms are also widely explored for high active and selecting catalysts. Severe deformation, even dipping into the surface, of these clusters can be expected because of the very active edge of clusters and strong interaction between supported clusters and surfaces. However, most models of these clusters are supposed to simply float on the top of the surface because ab initio simulations cannot afford the complex reconstructions. Here, we develop an accurate graph neural network machine learning potential (MLP) from ab initio data by active learning architecture through fine-tuning pre-trained models, and then employ the MLP into Monte Carlo to explore the structural evolutions of Mo and S clusters (1–8 atoms) on perfect and various defective MoS<sub>2</sub> monolayers. Interestingly, Mo clusters can always sink and embed themselves into MoS<sub>2</sub> layers. In contrast, S clusters float on perfect surfaces. On the defective surface, a few S atoms will fill the vacancy and rest S clusters float on the top. Such significant structural reconstructions should be carefully taken into account.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":"5 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-08-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249081","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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