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Redox-active sp2-c connected metal covalent organic frameworks for selective detection and reductive separation of uranium 用于选择性检测和还原分离铀的氧化还原活性 sp2-c 连接金属共价有机框架
Pub Date : 2024-09-02 DOI: 10.1016/j.asems.2024.100124
Jin-Lan Liu , Zhi-Hai Peng , Jia-Xin Qi , Cheng-Rong Zhang , Zhen-Wen Zhang , Li Zhang , Ru-Ping Liang , Jian-Ding Qiu

It is economically desirable to develop a material that can simultaneously detect and recover uranium. Herein, a CC-bridged two-dimensional metal-covalent organic framework (Cu-BTAN-AO MCOF) was constructed by condensation of metal single crystals with a rigid structure (Cu3(PyCA)3) and cyano monomers (BTAN) via Knoevenagel reaction for simultaneous detection and adsorption of uranium. The amidoxime group within the pore and the presence of unsaturated Cu(I) in the framework facilitate the adsorption of uranyl ions onto the amidoxime group, leading to fluorescence quenching via the photoinduced electron transfer (PET) mechanism, achieving a detection limit of as low as 167 nM uranyl ions. Furthermore, Cu-BTAN-AO demonstrates exceptional efficiency in capturing uranium from wastewater characterized by rapid kinetics and superior selectivity. It is noteworthy that Cu-BTAN-AO is the first example of simultaneous detection, adsorption and chemical reduction of uranium using metal centers and functional groups in MCOF, indicating that Cu-BTAN-AO has great potential for the detection and recovery of uranium-containing wastewater. This design strategy may also be applicable to advancing sensing and energy materials for other important metal ions.

开发一种可同时检测和回收铀的材料具有经济上的可取性。在此,通过克诺文纳格尔反应,将具有刚性结构的金属单晶(Cu3(PyCA)3)与氰基单体(BTAN)缩合,构建了一种 CC 桥接的二维金属-共价有机框架(Cu-BTAN-AO MCOF),可同时检测和吸附铀。孔隙中的脒肟基团和框架中存在的不饱和 Cu(I)促进了铀酰离子对脒肟基团的吸附,从而通过光诱导电子转移(PET)机制导致荧光淬灭,实现了低至 167 nM 的铀酰离子检测限。此外,Cu-BTAN-AO 在捕获废水中的铀方面表现出卓越的效率,其特点是快速的动力学和出色的选择性。值得注意的是,Cu-BTAN-AO 是利用 MCOF 中的金属中心和官能团同时检测、吸附和化学还原铀的第一个实例,这表明 Cu-BTAN-AO 在检测和回收含铀废水方面具有巨大潜力。这种设计策略也可用于推进其他重要金属离子的传感和能源材料。
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引用次数: 0
Porphyrin-based metal-organic frameworks for cancer theranostics 用于癌症治疗的卟啉基金属有机框架
Pub Date : 2024-08-28 DOI: 10.1016/j.asems.2024.100123
Liandi Guan , Fang Liu , Cun Zhang , Wei Wang , Jianwei Zhang , Qionglin Liang
Theranostics, integrating diagnostic and therapeutic functionalities, have emerged as advanced systems for timely cancer diagnosis and effective treatment. The development of versatile materials suitable for cancer theranostics is intensifying. Porphyrin-based metal-organic frameworks (MOFs) leverage the structural diversity and designability inherent in MOFs, alongside the robust photophysical, catalytic, and biological properties of porphyrins. These materials enhance the solubility and stability of porphyrins and facilitate their stable functionalized assemblies, conferring the potential for multimodal imaging diagnostics and precision therapeutics. In this review, we summarized the potential of porphyrin-based MOFs as cancer theranostics platforms, focusing on recent advancements in porphyrin-based MOFs, and highlighting their functionalized strategies and developments in diagnostic imaging and synergistic therapies. Finally, we proposed the challenges and prospects of these emerging materials in cancer theranostics.
集诊断和治疗功能于一体的疗法已成为及时诊断和有效治疗癌症的先进系统。适用于癌症治疗的多功能材料的开发正在不断加强。基于卟啉的金属有机框架(MOFs)利用了 MOFs 固有的结构多样性和可设计性,以及卟啉强大的光物理、催化和生物特性。这些材料提高了卟啉的溶解性和稳定性,促进了卟啉稳定的功能化组装,为多模式成像诊断和精准治疗带来了潜力。在这篇综述中,我们总结了卟啉基 MOFs 作为癌症治疗平台的潜力,重点介绍了卟啉基 MOFs 的最新进展,并强调了其在诊断成像和协同治疗方面的功能化策略和发展。最后,我们提出了这些新兴材料在癌症治疗学中面临的挑战和前景。
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引用次数: 0
Corrigendum to “Electrocatalytic CO2 and HCOOH interconversion on Pd-based catalysts” [Adv Sensor Energy Mater 1 (2022) 100007] 钯基催化剂上的电催化 CO2 和 HCOOH 相互转化"[Adv Sensor Energy Mater 1 (2022) 100007] 更正
Pub Date : 2024-08-27 DOI: 10.1016/j.asems.2024.100122
Guiru Zhang , Xianxian Qin , Chengwei Deng , Wen-Bin Cai , Kun Jiang
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引用次数: 0
Spherical nucleic acids for biomedical applications 球形核酸的生物医学应用
Pub Date : 2024-07-30 DOI: 10.1016/j.asems.2024.100117
Chunxin Xia , Hemei Cheng , Xinwei Hou , Yu Zhang , Xinchi Zhou , Qinglong Yan , Shuting Cao

Spherical nucleic acids (SNAs) are a 3D spherical nanostructure composed of highly oriented, dense layers of oligonucleotides conjugated to a hollow or solid core. This structure allows SNAs to show resistance to nuclease degradation, enter into nearly all cells without transfection agents and enable precise interactions with target molecules. Based on superior biological properties, SNAs can be tailored for diverse biological applications, rendering them a flexible and biosafe tool for biological applications as well as an enabling platform for therapy. In this review, we mainly discuss the structure and conjugation mode of SNAs and focus on recent advances in their applications, such as biomedical detection, imaging, and drug delivery. Finally, the remaining challenges and future directions of SNAs are also discussed and proposed.

球形核酸(SNA)是一种三维球形纳米结构,由高度定向、致密的寡核苷酸层与空心或实心核连接而成。这种结构使 SNA 能够抵抗核酸酶降解,无需转染剂即可进入几乎所有细胞,并能与目标分子发生精确的相互作用。基于优异的生物特性,SNAs 可针对不同的生物应用进行定制,使其成为一种灵活的生物安全工具和治疗平台。在这篇综述中,我们主要讨论了 SNA 的结构和共轭模式,并重点介绍了其在生物医学检测、成像和药物递送等方面的最新应用进展。最后,还讨论并提出了 SNAs 面临的挑战和未来发展方向。
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引用次数: 0
Ligand-free Cs2PdBr6 perovskite microcrystals with narrow bandgap and high photoelectrochemical performance in aqueous solution 在水溶液中具有窄带隙和高光电化学性能的无配体 Cs2PdBr6 包晶微晶
Pub Date : 2024-06-28 DOI: 10.1016/j.asems.2024.100116
Yaling Chen , Guanying Luo , Luyao Xu, Yu Yang, Yunzhong Xu, Jiahui Yu, Wei Chen, Huaping Peng

The exploration of efficient lead-free perovskite photoelectric active materials to develop high-performance photoelectrochemical (PEC) systems in aqueous solution is crucial to expand their PEC applications. Herein, we successfully constructed a high-performance PEC platform using ligand-free perovskite Cs2PdBr6 microcrystals (MCs) as the photoactive substance. The Cs2PdBr6 MCs showed narrow bandgap, wide absorption range, high electronic mobility and good stability in aqueous solutions. Particularly, the Cs2PdBr6 MCs exhibited an excellent photoresponse, the photocurrent density could reach as high as 98 μA/cm2 under 10.18 mW/cm2 light irradiation in the absence of other electron acceptors. In addition of the extremely wide range of response wavelength, wide pH range and accelerated interfacial carrier transfer, the Cs2PdBr6 MCs demonstrated the significant potential of photocathode active material for applications in PEC sensors and optoelectronic devices. Therefore, this work indicates that Cs2PdBr6 MCs design is a highly efficient way to solve the intrinsic issues of perovskite material, predicting a promising strategy for high performance PEC application in aqueous ambience.

探索高效的无铅包晶光电活性材料,以开发水溶液中的高性能光电化学(PEC)系统,对于扩大其 PEC 应用领域至关重要。在此,我们以无配体包晶 Cs2PdBr6 微晶(MCs)为光活性物质,成功构建了一个高性能 PEC 平台。Cs2PdBr6 MCs 在水溶液中表现出窄带隙、宽吸收范围、高电子迁移率和良好的稳定性。特别是,Cs2PdBr6 MCs 具有优异的光响应性能,在没有其他电子受体的情况下,在 10.18 mW/cm2 的光照射下,光电流密度高达 98 μA/cm2。Cs2PdBr6 MCs 具有极宽的响应波长范围、较宽的 pH 值范围和加速的界面载流子转移等特点,显示出光电阴极活性材料在 PEC 传感器和光电器件中的巨大应用潜力。因此,这项工作表明,Cs2PdBr6 MCs 的设计是解决包晶材料内在问题的一种高效方法,预示着在水环境中高性能 PEC 应用的一种有前途的策略。
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引用次数: 0
Label-free, background-free detection of nucleic acid with immobilization-free heterogeneous biosensor and one-pot hybridization chain reaction amplification 利用无固定化异质生物传感器和单锅杂交链反应扩增技术进行无标记、无背景的核酸检测
Pub Date : 2024-06-20 DOI: 10.1016/j.asems.2024.100115
Hongyan Yang , Zeyu Ma , Dan Zhang , Yi Wang , Lei Li , Guobao Zhou

Although immobilization-free and label-free electrochemical DNA (E-DNA) biosensors have engaged tremendous interest due to their superior properties, such as easy operation, time-saving and cost-saving, most of them are fabricated in homogeneous modes and usually produce high background current. In the present work, we proposed a new immobilization-free and label-free heterogeneous E-DNA assay based on a dual-blocker-aided multibranched hybridization chain reaction (HCR) for one-pot nucleic acid detection with zero background. The target nucleic acid triggers the HCR involving cascaded hybridization between two metastable hairpins, resulting in the generation of HCR products with multibranched arms, which can be captured onto the electrode via π-π stacking interactions between multibranched arms and reduced graphene oxide (rGO). Prior to the incubation process with an electrode, two blockers are designed to prohibit the nonspecific absorption of unreacted hairpin probes. Thus, an immobilization-free and label-free heterogeneous electrochemical assay for one-pot nucleic acid detection with zero background is readily realized. This strategy also presents additional merits of simplicity and cheap cost, since probe immobilization, signal tag labeling, and multiple incubation processes are avoided. Therefore, the as-proposed effective and versatile biosensor has great potential to be applied in nucleic acid-related practical biosensing.

虽然无固定化和无标记的电化学 DNA(E-DNA)生物传感器因其操作简便、省时、省钱等优越性能而备受关注,但它们大多采用均相模式制造,通常会产生较高的背景电流。在本研究中,我们提出了一种基于双阻断剂辅助多分支杂交链反应(HCR)的新型免固定、免标记异构 E-DNA 检测方法,可实现零背景的核酸检测。目标核酸触发的 HCR 涉及两个可转移发夹之间的级联杂交,从而产生具有多分支臂的 HCR 产物,这些产物可通过多分支臂与还原氧化石墨烯(rGO)之间的 π-π 堆叠相互作用被捕获到电极上。在与电极孵育之前,设计了两种阻断剂,以禁止未反应发夹探针的非特异性吸收。这样,一种无固定、无标记的异质电化学分析法就很容易实现了,它可以实现零背景的单次核酸检测。由于避免了探针固定、信号标签标记和多重孵育过程,这一策略还具有操作简单、成本低廉等优点。因此,这种高效、多功能的生物传感器在核酸相关的实用生物传感领域具有巨大的应用潜力。
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引用次数: 0
Optical sensor for BTEX detection: Integrating machine learning for enhanced sensing 用于检测 BTEX 的光学传感器:整合机器学习,增强传感能力
Pub Date : 2024-06-20 DOI: 10.1016/j.asems.2024.100114
Mary Hashemitaheri , Ebrahim Ebrahimi , Geethanga de Silva , Hamed Attariani

Optical sensors provide a fast and real-time approach to detect benzene, toluene, ethylbenzene, and xylenes (BTEX) in environmental monitoring and industrial safety. However, detecting the concentration of a particular gas in a mixture can be challenging. Here, we develop a machine-learning model that can precisely measure BTEX concentrations simultaneously based on an absorption spectroscopy gas sensing system. The convolutional neural network (CNN) is utilized to identify the absorbance spectra for each volatile, along with their concentrations in a mixture. A synthetic data set is generated using a series of physics-based simulations to create the predictive model. The data set consists of the overall absorbance of numerous random BTEX mixtures over time, based on various percentages of the permissible exposure limit (PEL). It is worth noting that benzene has a negligible absorbance (very low PEL, 1–5 ppm) compared to other volatile gases, which makes it difficult to detect. To address this challenge, we introduce a 3-stage solution to accurately discriminate between all BTEX species, regardless of their concentration levels. As a result, the R-squared above 0.99 for toluene, ethylbenzene, and o-xylene, and the R-squared above 0.96 for benzene, is achieved, indicating the model's capability to predict BTEX concentrations.

光学传感器为环境监测和工业安全提供了一种快速、实时检测苯、甲苯、乙苯和二甲苯(BTEX)的方法。然而,检测混合物中特定气体的浓度是一项挑战。在此,我们基于吸收光谱气体传感系统开发了一种机器学习模型,可同时精确测量 BTEX 的浓度。我们利用卷积神经网络(CNN)来识别每种挥发性物质的吸收光谱以及它们在混合物中的浓度。使用一系列基于物理的模拟生成合成数据集,以创建预测模型。该数据集包括大量随机 BTEX 混合物随着时间推移的总体吸光度,基于允许接触限值 (PEL) 的不同百分比。值得注意的是,与其他挥发性气体相比,苯的吸光度可以忽略不计(PEL 很低,1-5 ppm),因此很难检测。为了应对这一挑战,我们引入了一种三阶段解决方案,以准确区分所有 BTEX 种类,而不论其浓度水平如何。结果,甲苯、乙苯和邻二甲苯的 R 方均超过 0.99,苯的 R 方均超过 0.96,表明该模型具有预测 BTEX 浓度的能力。
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引用次数: 0
Mechanical properties modulation and biological applications of DNA hydrogels DNA 水凝胶的机械特性调制和生物应用
Pub Date : 2024-06-19 DOI: 10.1016/j.asems.2024.100113
Yiliu Wang , Yu Zhang , Qi Zhang , Xia Li , Qinglong Yan , Ying Zhu

DNA hydrogels are three-dimensional polymer networks constructed using DNA as the structural building block. Due to the tight binding between hydrophilic groups on DNA chains and water molecules, they exhibit outstanding plasticity and fluid thermodynamic properties, making them one of the best choices for mimicking natural biological tissues. By controlling the backbone building blocks, gelation conditions, and cross-linking methods of DNA hydrogels, hydrogels with different mechanical strengths can be obtained, thus expanding their applications in the field of biology. This review first introduces the relationship between the mechanical properties of DNA hydrogels and their structure, elucidates the approaches and strategies for mechanical property modulation, and focuses on the scheme of controllable design to modulate the mechanical properties of DNA hydrogels for applications in biosensing, cellular function regulation, and bone tissue engineering. Furthermore, this review outlines the future development directions and challenges faced in the mechanical property modulation of DNA hydrogels, providing useful information for the precise design of DNA hydrogels for biological research.

DNA 水凝胶是以 DNA 为结构单元构建的三维聚合物网络。由于 DNA 链上的亲水基团与水分子紧密结合,它们具有出色的可塑性和流体热力学特性,是模拟天然生物组织的最佳选择之一。通过控制 DNA 水凝胶的骨架构建模块、凝胶化条件和交联方法,可以获得不同机械强度的水凝胶,从而拓展其在生物学领域的应用。本综述首先介绍了 DNA 水凝胶的力学性能与其结构之间的关系,阐明了调控力学性能的方法和策略,并重点介绍了调控 DNA 水凝胶力学性能的可控设计方案,以应用于生物传感、细胞功能调控和骨组织工程等领域。此外,本综述还概述了 DNA 水凝胶机械性能调控的未来发展方向和面临的挑战,为生物研究中 DNA 水凝胶的精确设计提供了有用信息。
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引用次数: 0
Progress in ion detection and clinical diagnosis based on G-quadruplex combined with fluorescence properties 基于 G-四链路结合荧光特性的离子检测和临床诊断研究进展
Pub Date : 2024-06-17 DOI: 10.1016/j.asems.2024.100112
Ping Lu, Gerile Aodeng, Jun Ai

G-quadruplex is a high-level structure composed of folded DNA or RNA rich in tandem repeats of guanine (G). In recent years, G-quadruplex is widely used in various fields due to its unique structural properties. This article briefly introduces the structural properties of G-quadruplex, and provides a brief introduction to the research on DNA and RNA G-quadruplex in various detection and medical fields. It is hoped that this can provide some help to readers who want to understand G-quadruplex.

G-quadruplex 是一种由富含串联重复鸟嘌呤(G)的折叠 DNA 或 RNA 组成的高级结构。近年来,G-四叠体因其独特的结构特性被广泛应用于各个领域。本文简要介绍了 G 型四叠体的结构特性,并简要介绍了 DNA 和 RNA G 型四叠体在各种检测和医学领域的研究情况。希望能为想要了解 G-四叠体的读者提供一些帮助。
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引用次数: 0
Development of ratiometric DNA biosensors with improved accuracy, precision, and signal-to-noise ratio 开发具有更高精度、准确性和信噪比的比率 DNA 生物传感器
Pub Date : 2024-05-16 DOI: 10.1016/j.asems.2024.100106
Qing Tao , Yanli Wen , Wen Liang , Lele Wang , Ruiyan Guo , Min Ding , Ming Luo , Juan Yan , Feiyan Gong , Chengming Cao , Lanying Li , Gang Liu

Ratiometric DNA biosensors, which utilize DNA as the recognition element and integrate dual signals from diverse sensing platforms including fluorescence, electrochemistry, and surface-enhanced Raman scattering (SERS), have demonstrated remarkable proficiency in detecting a wide range of targets. In this review, we showcase the significant progress achieved by ratiometric biosensors. Firstly, ratiometric biosensors have made notable advancements in analyzing real samples. These include the analysis of pH values near cancer cells, quantification of miRNA in human cell lysates, detection of human telomerase RNA in cell extracts, and performing DNA logic-gated in situ bioimaging on cell membranes. Secondly, excellent sensitivity has been attained through the utilization of effective amplification methods such as RCA, HCR, and CHA, among others. Thirdly, the construction of stable reference signals has resulted in significantly improved precision for ratiometric biosensors. This breakthrough has overcome matrix effects, enabling reliable detection in real samples with high selectivity. This review provides a comprehensive overview of recent advancements in strategies employed by ratiometric DNA biosensors. We present three types of biosensors based on distinct sensing platforms: fluorescent, electrochemical, and SERS biosensors. Additionally, we discuss future directions and primary challenges in the development of ratiometric DNA biosensors.

DNA 比率生物传感器利用 DNA 作为识别元件,整合了来自荧光、电化学和表面增强拉曼散射(SERS)等不同传感平台的双重信号,在检测各种目标物方面表现出了非凡的能力。在本综述中,我们将展示比率计量生物传感器所取得的重大进展。首先,比率测量生物传感器在分析真实样品方面取得了显著进步。其中包括分析癌细胞附近的 pH 值、定量人类细胞裂解液中的 miRNA、检测细胞提取物中的人类端粒酶 RNA 以及在细胞膜上进行 DNA 逻辑门控原位生物成像。其次,通过使用 RCA、HCR 和 CHA 等有效的扩增方法,实现了极高的灵敏度。第三,稳定参考信号的构建大大提高了比率测量生物传感器的精度。这一突破克服了基质效应,实现了对真实样品的可靠检测和高选择性。本综述全面概述了比率测量 DNA 生物传感器所采用策略的最新进展。我们介绍了基于不同传感平台的三种生物传感器:荧光、电化学和 SERS 生物传感器。此外,我们还讨论了比率测量 DNA 生物传感器的未来发展方向和主要挑战。
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引用次数: 0
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Advanced Sensor and Energy Materials
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