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Deprotonated of layered double hydroxides during electrocatalytic water oxidation for multi-cations intercalation 多阳离子插层电催化水氧化过程中层状双氢氧化物的去质子化
Pub Date : 2024-04-10 DOI: 10.1002/smo.20230026
Bowen Jin, Jianxiong Gao, Yunqi Zhang, Mingfei Shao
Aqueous rechargeable batteries using abundant multi-ion cations have received increasing attention in the energy storage field for their high safety and low cost. Layered double hydroxides (LDHs) possess a two-dimensional structure and exhibit great potential as cathodes for multi-ion intercalation. However, the insufficient active sites of LDHs result in low capacities in the discharging process. Interestingly, the LDHs after the deprotonation process exhibit favorable electrochemical performance of multi-cation intercalation. The deprotonation process of LDHs has been widely found in the oxygen evolution reaction and energy storage field, where LDHs lose H in laminates and converts to deprotonated γ-phase MOOHs (MOOs). Herein, we take a comprehensive overview of the dynamics structure transformation of the deprotonation process of LDHs. Furthermore, the development of advanced aqueous battery cathode and metal battery anode based on deprotonated LDHs for energy storage is explored and summarized. Finally, the perspective of deprotonated LDHs in the energy storage field is discussed.
使用丰富的多离子阳离子的水性可充电电池因其安全性高、成本低而在储能领域受到越来越多的关注。层状双氢氧化物(LDHs)具有二维结构,具有作为多离子插层阴极的巨大潜力。然而,由于 LDHs 的活性位点不足,导致其在放电过程中容量较低。有趣的是,经过去质子化过程的 LDHs 在多离子插层方面表现出良好的电化学性能。LDHs 的去质子化过程在氧进化反应和储能领域被广泛发现,LDHs 在层状结构中失去 H,转化为去质子化的 γ 相 MOOHs(MOOs)。在此,我们将全面概述 LDHs 去质子化过程的动力学结构转变。此外,还对基于去质子化 LDHs 的先进水电池正极和金属电池负极的储能开发进行了探讨和总结。最后,讨论了去质子化 LDHs 在储能领域的前景。
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引用次数: 0
Smart emulsion system driven by light-triggered ionic liquid molecules and its application in eco-friendly water-saving dyeing 光触发离子液体分子驱动的智能乳液系统及其在环保节水染色中的应用
Pub Date : 2024-03-19 DOI: 10.1002/smo.20230030
Aiqin Gao, Jiahui Liang, Mingxiao Jing, Xiyu Song, Aiqin Hou, Kongliang Xie
The smart emulsification and demulsification system with the light response is a useful tool in various industries, including green chemistry, catalytic reaction, pharmaceuticals, and environmental remediation. Herein, an ionic liquid crystal compound with a light triggered switch based on the azobenzene group [(4-{3-methyl-1-[3-(8-octyloxyoctyl)oxy-4-oxobutanoyl]imidazo-lium-1-yl}octyl)oxy] -N-(4-methylphenyl)benzene-1,2-diazene bromide (MOIAzo), was designed and synthesized, which could cause reversible transition between emulsification and demulsification through the light trigger. The ionic liquid has an efficient photoinduced liquefaction process, which dramatically lowers the melting point of ionic liquids from 79 to 9.2 oC. This significantly broadens the liquid state temperature of the ionic liquid crystal. The ionic liquid crystal MOIAzo exhibits both photoinduced and thermally induced nematic liquid crystal properties. The smart emulsion system was effectively employed in an eco-friendly water-saving dyeing process of cationic dyes for cationic dyeable polyester (CDP) fabrics, which used only half the amount of water compared with the conventional water bath dyeing method. After dyeing, the oil and water phases can be efficiently separated through the light irradiation, and the oil phase can be reused for the subsequent dyeing process. This novel smart emulsion dyeing method greatly reduces the water consumption and wastewater discharge. MOIAzo as a light-triggered ionic liquid molecule opens up new dimensions in green chemistry.
具有光响应的智能乳化和破乳化系统是绿色化学、催化反应、制药和环境修复等各行各业的有用工具。本文设计并合成了一种基于偶氮苯基团[(4-{3-甲基-1-[3-(8-辛氧基辛基)氧基-4-氧代丁酰基]咪唑-鎓-1-基}辛基)氧基]-N-(4-甲基苯基)苯-1,2-二氮杂溴化物(MOIAzo)的具有光触发开关的离子液晶化合物,该化合物可通过光触发实现乳化和破乳化之间的可逆转换。该离子液体具有高效的光诱导液化过程,可将离子液体的熔点从 79 摄氏度大幅降至 9.2 摄氏度。这大大拓宽了离子液晶的液态温度。离子液晶 MOIAzo 同时具有光诱导和热诱导向列液晶特性。该智能乳液体系被有效地应用于阳离子染料对阳离子可染涤纶(CDP)织物的环保型节水染色工艺中,与传统的水浴染色法相比,只需使用一半的水量。染色后,油相和水相可通过光照射有效分离,油相可重新用于后续染色工艺。这种新型的智能乳液染色方法大大减少了用水量和废水排放量。MOIAzo 作为一种光触发离子液体分子,为绿色化学开辟了新的领域。
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引用次数: 0
Smart molecules in ophthalmology: Hydrogels as responsive systems for ophthalmic applications 眼科中的智能分子:作为眼科应用响应系统的水凝胶
Pub Date : 2024-03-15 DOI: 10.1002/smo.20230021
Merve Kulbay, Kevin Yang Wu, Doanh Truong, Simon D. Tran
This comprehensive review delves into a unique intersection of hydrogels as smart molecules and their transformative applications in ophthalmology. Beginning with the foundational definition, properties, and classification of hydrogels, the review explores their synthesis and responsive capabilities. Specific applications examined encompass topical drug delivery, contact lenses, intravitreal drug delivery, ocular adhesives, vitreous substitutes, and cell-based therapy. A methodical analysis, including an overview of relevant ocular structures and a comparative evaluation of hydrogel-based solutions against traditional treatments, is conducted. Additionally, potential constraints, translation challenges, knowledge gaps, and research areas are identified. Our methodical approach, guided by an extensive literature review from 2017 to 2023, illuminates the unprecedented opportunities offered by hydrogels, along with pinpointing areas for further inquiry to facilitate their transition into clinical practice.
本综述深入探讨了水凝胶作为智能分子的独特交叉点及其在眼科领域的变革性应用。综述从水凝胶的基本定义、特性和分类入手,探讨了水凝胶的合成和反应能力。研究的具体应用包括局部给药、隐形眼镜、玻璃体内给药、眼部粘合剂、玻璃体替代物和细胞疗法。分析方法包括概述相关的眼部结构,以及对基于水凝胶的解决方案与传统治疗方法进行比较评估。此外,还确定了潜在的制约因素、转化挑战、知识差距和研究领域。我们的方法以 2017 年至 2023 年的大量文献综述为指导,揭示了水凝胶带来的前所未有的机遇,同时指出了需要进一步研究的领域,以促进水凝胶向临床实践的过渡。
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引用次数: 0
Precise construction of DNA origami-based materials for functional regulation on biological interface 精确构建基于 DNA 折纸的材料,实现生物界面的功能调控
Pub Date : 2024-03-04 DOI: 10.1002/smo.20230032
Yushuai Wu, Xiaohui Wu, Run Tian, Yiming Wang, Baoquan Ding, Qiao Jiang
Precise design and control of molecular self-assembly as living creatures are exciting ideas in the field of nanotechnology. Characterized with predesigned geometries and accurate spatial addressability, programmable DNA origami nanostructures have been recognized as optimized tools for assembling multiple functional components. A variety of biomolecules can be attached to the nanoscale drawing boards in a site-specific fashion, thus facilitating the precise construction of DNA origami-based materials for studies on biological interface. In this minireview, we highlight the recent advances in the precise construction of DNA origami-based materials with artificial bio-structures and/or biomimicking functions. The regulation of biological functions by these DNA origami-engineered assemblies at the bio-interface has been summarized and discussed.
精确设计和控制分子自组装生物是纳米技术领域令人兴奋的想法。可编程 DNA 折纸纳米结构具有预先设计的几何形状和精确的空间寻址能力,被认为是组装多种功能组件的优化工具。各种生物分子都能以特定位点的方式附着在纳米级图板上,从而有助于精确构建基于 DNA 折纸的材料,用于生物界面研究。在这篇微型综述中,我们将重点介绍在精确构建具有人工生物结构和/或仿生功能的 DNA 折纸材料方面的最新进展。我们还总结并讨论了这些 DNA 折纸工程组装体在生物界面上对生物功能的调控。
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引用次数: 0
Smart chiral liquid crystal elastomers: Design, properties and application 智能手性液晶弹性体:设计、特性和应用
Pub Date : 2024-02-29 DOI: 10.1002/smo.20230025
Yuan Liu, Jiazhe Ma, Yanzhao Yang, Cristian Valenzuela, Xuan Zhang, Ling Wang, Wei Feng
Smart chiral liquid crystal elastomers are a class of soft photonic crystals with periodic nanostructures. There are two kinds of chiral liquid crystal elastomers with structural colors: cholesteric liquid crystal elastomers with a one-dimensional helical nanostructure and blue-phase liquid crystal elastomers with a three-dimensional photonic crystal nanostructure. The self-assembled nanostructure of chiral liquid crystal elastomers can be dynamically controlled under external stimulation, and the reflected color can be adjusted throughout the visible light range. Along with the development of innovative material systems and cutting-edge manufacturing technologies, researchers have proposed diverse strategies to design and synthesize chiral liquid crystal elastomers and have thoroughly investigated their properties and potential applications. Here, we provide a systematic review of the progress in the design and fabrication of smart chiral liquid crystal elastomers, focusing on the cholesteric liquid crystal elastomers via surface-enforced alignment, bar coating, 3D printing, anisotropic deswelling methods as well as the three-dimensional self-assembly of blue-phase liquid crystal elastomers without additional alignment. Smart chiral liquid crystal elastomers are able to respond quickly to external stimuli and have a wide range of applications in areas such as adaptive optics, color-changing camouflage, soft robotics, and information encryption. This review concludes with a perspective on the opportunities and challenges for the future development of smart chiral liquid crystal elastomers.
智能手性液晶弹性体是一类具有周期性纳米结构的软光子晶体。手性液晶弹性体有两种结构颜色:具有一维螺旋纳米结构的胆甾液晶弹性体和具有三维光子晶体纳米结构的蓝相液晶弹性体。手性液晶弹性体的自组装纳米结构可在外部刺激下动态控制,反射颜色可在整个可见光范围内调节。随着创新材料体系和尖端制造技术的发展,研究人员提出了设计和合成手性液晶弹性体的多种策略,并对其性能和潜在应用进行了深入研究。在此,我们系统回顾了智能手性液晶弹性体的设计与制造进展,重点介绍了通过表面强化配位、棒状涂层、三维打印、各向异性脱胶方法以及无需额外配位的蓝相液晶弹性体的三维自组装等方法制备的胆甾液晶弹性体。智能手性液晶弹性体能够对外界刺激做出快速反应,在自适应光学、变色伪装、软机器人和信息加密等领域有着广泛的应用。本综述最后展望了智能手性液晶弹性体未来发展的机遇和挑战。
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引用次数: 0
Activatable theranostic prodrug scaffold with tunable drug release rate for sequential photodynamic and chemotherapy 具有可调药物释放率的可激活治疗原药支架,用于光动力和化疗的连续治疗
Pub Date : 2024-02-20 DOI: 10.1002/smo.20230024
Si-Yu Wang, Ying-Hao Pan, Yu-Chen Qu, Xiao-Xiao Chen, Na Shao, Li-Ya Niu, Qing-Zheng Yang
Glutathione (GSH)-activated prodrugs are promising for overcoming the limitations of conventional anti-tumor drugs. However, current GSH-responsive disulfide groups exhibit unregulated reactivity, making it impossible to precisely control the drug release rate. We herein report a series of GSH-responsive prodrugs with a “three-in-one” molecular design by integrating a fluorescence report unit, stimuli-responsive unit and chemodrug into one scaffold with tunable aromatic nucleophilic substitution (SNAr) reactivity. The drug release rate of these prodrugs is tailored by modification of substituent groups with different electron-withdrawing or -donating abilities on the BODIPY core. Furthermore, the prodrugs self-assemble in water to form nanoparticles that serve as photosensitizers to produce reactive oxygen species upon irradiation for photodynamic therapy (PDT). The PDT process also increases the concentration of GSH in cells, further promoting the release of drugs for chemotherapy. This strategy provides a powerful platform for sequential photodynamic and chemotherapy with tunable drug release rates and synergistic therapeutic effects.
谷胱甘肽(GSH)活化原药有望克服传统抗肿瘤药物的局限性。然而,目前的 GSH 反应性二硫化物基团表现出不受调节的反应性,因此无法精确控制药物释放率。我们在此报告了一系列具有 "三合一 "分子设计的 GSH 响应原药,它们将荧光报告单元、刺激响应单元和化学药物整合到一个具有可调芳香族亲核取代(SNAr)反应性的支架中。通过对 BODIPY 核心上具有不同吸电子或弃电子能力的取代基团进行修饰,可定制这些原药的药物释放速率。此外,这些原药还能在水中自组装形成纳米颗粒,作为光敏剂在光动力疗法(PDT)照射时产生活性氧。光动力疗法过程还能提高细胞中 GSH 的浓度,进一步促进化疗药物的释放。这种策略为顺序光动力疗法和化疗提供了一个强大的平台,可调节药物释放率并产生协同治疗效果。
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引用次数: 0
Smart molecular crystal switches 智能分子晶体开关
Pub Date : 2024-02-16 DOI: 10.1002/smo.20230031
Ian Cheng-Yi Hou, Liang Li, Hongyu Zhang, Panče Naumov
The multifaceted switches are part of our everyday life from the macroscopic to the molecular world. A molecular switch operating in the solution and in the crystalline state is very different. In this review, we summarize the state-of-the-art of smart molecular crystal switches based on molecular martensites. These crystal switches respond to external stimuli and reversibly change between states, retaining their macroscopic integrity. The operation of the switches predominantly relies on temperature alterations or mechanical stress, with emerging methods based on photothermal effects, photoisomerization, and host-guest chemistry. The capability of changing the molecular orientation and interaction in smart molecular crystal switches offers opportunities in several applications, including actuators, reversibly shaping structural materials, optoelectronic and magnetic materials, as well as switchable porous materials. Smart molecular crystal switches have vast potential in modern scientific and technological progress. The ongoing research shapes a rich landscape for innovation and future scientific exploration across diverse disciplines.
从宏观世界到分子世界,多方面的开关都是我们日常生活的一部分。在溶液和晶体状态下工作的分子开关截然不同。在这篇综述中,我们总结了基于分子马氏体的智能分子晶体开关的最新进展。这些晶体开关会对外界刺激做出反应,并在不同状态之间进行可逆变化,同时保持其宏观完整性。开关的运行主要依赖于温度变化或机械应力,还有基于光热效应、光异构化和主客体化学的新兴方法。智能分子晶体开关中改变分子取向和相互作用的能力为多种应用提供了机会,包括致动器、可逆成型结构材料、光电和磁性材料以及可切换多孔材料。智能分子晶体开关在现代科学和技术进步中具有巨大潜力。正在进行的研究为不同学科的创新和未来科学探索勾勒出一幅丰富的图景。
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引用次数: 0
Electron-withdrawing inductive effects enhanced strategy for protein thiol sensing and blocking agent design 电子牵引感应效应增强了蛋白质硫醇传感和阻断剂的设计策略
Pub Date : 2024-02-14 DOI: 10.1002/smo.20230022
Liangwei Zhang, Shudi Liu, Xia Zhang, Jinyu Sun, Lingxin Chen
It is a great challenge to discover novel chemical reactions suitable for biological analysis in a living system. The development of novel protein thiol blocking agents is a crucial need for exploring protein thiol functions in protein refolding, signal transduction, and redox regulation. We are always keen on seeking novel chemical reactions applied to endogenous biological macromolecules or protein thiol sensing, blocking, and labeling. In the present work, we have successfully developed a novel agent to block protein thiol by enhanced electron-withdrawing inductive effects. This sensing and blocking process was detailedly monitored by UV-vis, fluorescent spectra, and SDS-Page gel separation. The spectral studies demonstrated that the agent could react ultrafastly with thiol within seconds at μM level. Furthermore, fluorescent imaging in cells and in vivo was further used for the validation of its ability to sensing and blocking thiol, providing evidence of downregulated protein thiols in Parkinson's disease. The enhanced electron-withdrawing inductive effect strategy in this work may provide a general guideline for designing protein thiol agent.
发现适合在活体系统中进行生物分析的新型化学反应是一项巨大的挑战。开发新型蛋白质硫醇阻断剂是探索蛋白质硫醇在蛋白质重折叠、信号转导和氧化还原调节中的功能的关键需求。我们一直热衷于寻求应用于内源生物大分子或蛋白质硫醇传感、阻断和标记的新型化学反应。在本研究中,我们成功开发了一种新型制剂,通过增强的电子吸收感应效应来阻断蛋白质硫醇。我们通过紫外-可见光谱、荧光光谱和 SDS-Page 凝胶分离对这一感应和阻断过程进行了详细监测。光谱研究表明,该制剂能在μM水平上几秒钟内与硫醇发生超快反应。此外,还进一步利用细胞和体内的荧光成像来验证其感知和阻断硫醇的能力,从而为帕金森病中蛋白质硫醇下调提供证据。这项研究中的增强型电子吸收诱导效应策略可为蛋白质硫醇制剂的设计提供一般性指导。
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引用次数: 0
Recent progress in stimuli-responsive DNA-based logic gates: Design, working principles and biological applications 基于刺激响应 DNA 的逻辑门的最新进展:设计、工作原理和生物应用
Pub Date : 2024-02-14 DOI: 10.1002/smo.20230023
Ling Sum Liu, Hoi Man Leung, Yuzhen Cai, Pik Kwan Lo
Stimuli-responsive DNA-based logic gates have emerged as a promising field at the intersection of synthetic biology and nanotechnology. These gates exploit the unique properties of DNA molecules to perform programmable computational operations in response to specific stimuli. This review provides a comprehensive overview of recent advancements in the design, working principles, and applications of stimuli-responsive DNA-based logic gates. The progress made in developing various types of logic gates triggered by metal ions, pH, oligonucleotides, small molecules, proteins, and light is highlighted. The applications of these logic gates in imaging and biosensing, drug delivery, synthetic biology and molecular computing are discussed. This review underscores the significant contributions and future prospects of stimuli-responsive DNA-based logic gates in advancing the field of nanotechnology.
基于刺激响应 DNA 的逻辑门已成为合成生物学和纳米技术交叉领域的一个前景广阔的领域。这些逻辑门利用 DNA 分子的独特性质,在特定刺激下执行可编程的计算操作。本综述全面概述了基于刺激响应 DNA 逻辑门的设计、工作原理和应用方面的最新进展。重点介绍了在开发由金属离子、pH 值、寡核苷酸、小分子、蛋白质和光触发的各类逻辑门方面取得的进展。讨论了这些逻辑门在成像和生物传感、药物输送、合成生物学和分子计算方面的应用。这篇综述强调了基于刺激响应 DNA 的逻辑门在推动纳米技术领域发展方面的重大贡献和未来前景。
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引用次数: 0
Benzothiazole-endoperoxide conjugates protect PC12 cells against β-amyloid-induced cell death via singlet oxygen mediated oxidative detoxification of fibrils 苯并噻唑-内过氧化物共轭物通过单线态氧介导的纤维氧化解毒作用保护 PC12 细胞免受 β 淀粉样蛋白诱导的细胞死亡影响
Pub Date : 2024-01-04 DOI: 10.1002/smo.20230019
Hao Wu, Lei Wang, Xiao Qian, Wanwan Wang, Yu Si, Rensong Sun, Engin U. Akkaya
Metastable endoperoxides with beta-amyloid fibrils targeting benzothiazole moieties were designed and synthesized. Singlet oxygen released from these endoperoxides by thermal cycloreversion reaction was shown to cause significant structural changes on the amyloid assemblies. Most importantly, the cytotoxicity of the beta-amyloid fibrils on the PC12 cells were significantly reduced in the presence of endoperoxides. This observation, coupled with the fact that neither external oxygen, nor light is needed for this transformation, is very promising.
我们设计并合成了以β-淀粉样蛋白纤维为目标的苯并噻唑分子的可转移内过氧化物。研究表明,这些内过氧化物通过热环化反应释放出的单线态氧能使淀粉样蛋白组合物的结构发生显著变化。最重要的是,在有内过氧化物存在的情况下,β-淀粉样蛋白纤维对 PC12 细胞的细胞毒性显著降低。这一观察结果,再加上这种转变既不需要外部氧气,也不需要光照这一事实,都非常令人期待。
{"title":"Benzothiazole-endoperoxide conjugates protect PC12 cells against β-amyloid-induced cell death via singlet oxygen mediated oxidative detoxification of fibrils","authors":"Hao Wu, Lei Wang, Xiao Qian, Wanwan Wang, Yu Si, Rensong Sun, Engin U. Akkaya","doi":"10.1002/smo.20230019","DOIUrl":"https://doi.org/10.1002/smo.20230019","url":null,"abstract":"Metastable endoperoxides with beta-amyloid fibrils targeting benzothiazole moieties were designed and synthesized. Singlet oxygen released from these endoperoxides by thermal cycloreversion reaction was shown to cause significant structural changes on the amyloid assemblies. Most importantly, the cytotoxicity of the beta-amyloid fibrils on the PC12 cells were significantly reduced in the presence of endoperoxides. This observation, coupled with the fact that neither external oxygen, nor light is needed for this transformation, is very promising.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139093476","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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Smart Molecules
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