molecular logic gate

分子逻辑门
  • 文章类型: Journal Article
    一种新型香豆素荧光传感器CHE,掺入2-肼基苯并噻唑和香豆素醛,已开发出在干扰存在下优先检测Hg2和Ag的方法。与以前流行的基于强度的荧光探针相比,CHE对Hg2+和Ag+表现出比率荧光响应,并使用EDTA与离子-CHE络合物相互作用时的差异提取能力进一步准确区分Hg2和Ag。研究并阐明了传感机理。化学传感器CHE已成功用于检测六个不同样品中的Hg2和Ag,结果令人满意。此外,组合逻辑电路是利用三个不同的逻辑门(NOT,OR,和INH)基于传感器响应Hg2+/Ag+和其他阳离子的差分输出信号。有趣的是,利用EDTA与Hg2+相互作用的可逆和可重复的开关行为,提出了具有多写功能的概念性“写-读-擦除-读”内存功能,为基于分子的记忆系统提供了新的视角。
    A novel coumarin-based fluorescent sensor CHE, incorporating 2-hydrazinylbenzothiazole and coumarin aldehyde, has been developed that demonstrated a preferential detection of Hg2+ and Ag+ in presence of interferences. Compared to previously prevalent intensity-based fluorescent probes, CHE exhibited a ratiometric fluorescence response to Hg2+ and Ag+, and further accurately differentiated Hg2+ and Ag + using the differential extractive ability of EDTA when interacting with ion-CHE complexes. Sensing mechanism was investigated and elucidated. The chemosensor CHE was successfully applied to detect Hg2+ and Ag+ in six distinct samples with satisfactory results. Additionally, combinatorial logic circuits were constructed utilizing three distinct logic gates (NOT, OR, and INH) based on the sensor\'s differential output signals in response to Hg2+/Ag+ and other cations. Interestingly, utilizing the reversible and reproducible switching behavior of the EDTA interaction with Hg2+, a conceptual \'Write-Read-Erase-Read\' memory function with multi-write capability was proposed, offering a novel perspective for molecular-based memory systems.
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  • 文章类型: Journal Article
    在本研究中,我们设计了一种分子逻辑门系统,采用Fe2离子和胆固醇作为生物分析物,用于创新的检测策略。我们利用绿色合成方法,使用芒果叶提取物来创建称为“mGQDs”的荧光石墨烯量子点。通过像HR-TEM这样的技术,即,高分辨率透射电子显微镜,拉曼光谱,XPS,即,X射线光电子能谱,mGQDs的成功形成得到证实。研究了mGQDs的光致发光(PL)特性在金属离子检测中的潜在应用,特别是水中的Fe2+痕迹,通过使用荧光技术。在425nm激发下,mGQD在其PL光谱中在495和677nm处表现出发射带。用2.5μMFe2离子,Fe2引起的mGQDsPL强度的显着猝灭降低了97%;但是,添加20mM胆固醇导致92%的回收率。在室温下通过线性Stern-Volmer(S-V)图确定检测限,Fe2+离子的值为4.07μM,胆固醇的值为1.8mM。此外,mGQD证明了生物相容性,水溶性,和无毒性,促进快速非酶胆固醇检测方法的创建。选择性和检测研究强调了mGQDs在胆固醇水平监测中的可靠性。此外,为了检测目的,建立了采用Fe2+金属离子和胆固醇作为生物分析物的分子逻辑门系统。总的来说,这项研究介绍了一种生态友好的方法来制作MGQDs,并强调了它们在检测金属离子和胆固醇方面的有效性,表明它们作为多种分析和生物医学应用的多功能纳米材料的潜力。
    In the present study, we have engineered a molecular logic gate system employing both Fe2+ ions and cholesterol as bioanalytes for innovative detection strategies. We utilized a green-synthesis method employing the mango leaves extract to create fluorescent graphene quantum dots termed \"mGQDs\". Through techniques like HR-TEM, i.e., high-resolution transmission electron microscopy, Raman spectroscopy, and XPS, i.e., X-ray photoelectron spectroscopy, the successful formation of mGQDs was confirmed. The photoluminescence (PL) characteristics of mGQDs were investigated for potential applications in metal ion detection, specifically Fe2+ traces in water, by using fluorescence techniques. Under 425 nm excitation, mGQDs exhibited emission bands at 495 and 677 nm in their PL spectrum. Fe2+-induced notable quenching of mGQDs\' PL intensity decreased by 97% with 2.5 μM Fe2+ ions; however, adding 20 mM cholesterol resulted in a 92% recovery. Detection limits were established through a linear Stern-Volmer (S-V) plot at room temperature, yielding values of 4.07 μM for Fe2+ ions and 1.8 mM for cholesterol. Moreover, mGQDs demonstrated biocompatibility, aqueous solubility, and nontoxicity, facilitating the creation of a rapid nonenzymatic cholesterol detection method. Selectivity and detection studies underscored mGQDs\' reliability in cholesterol level monitoring. Additionally, a molecular logic gate system employing Fe2+ metal ions and cholesterol as a bioanalyte was established for detection purposes. Overall, this research introduces an ecofriendly approach to craft mGQDs and highlights their effectiveness in detecting metal ions and cholesterol, suggesting their potential as versatile nanomaterials for diverse analytical and biomedical applications.
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  • 文章类型: Journal Article
    本工作代表了一种基于荧光共振能量转移(FRET)的传感方法,用于检测枪弹残留物(GSR)成分。两种激光染料Acf和RhB已分别用作FRET对中的供体和受体。真实样本是在法医科学实验室进行测试射击后收集的。另一方面,已在实验室制备了标准GSR溶液。对于标准GSR溶液的制备,我们使用盐BaCl2,SbCl3和Pb(NO3)2的水溶液。通过在水溶液中混合盐,在Acf和RhB之间测量FRET效率,以检测实际样品和标准溶液中GSR成分(Pb2,Ba2和Sb3)的存在。已经观察到,FRET效率在GSR组分存在下系统地降低。为了放大染料对的FRET效率,使用无机粘土分散体(锂皂石)。FRET效率的提高代表了所提出的传感器的更好的灵敏度。电流传感器可用于量化真实样品中GSR组分的浓度。
    The present work represents a Fluorescence Resonance Energy Transfer (FRET) based sensing method for detecting Gunshot Residue (GSR) components. Two laser dyes Acf and RhB have been used as donor and acceptor respectively in the FRET pair. The real sample was collected after test firing in a forensic science laboratory. On the other hand, a standard GSR solution has been prepared in the laboratory. For the preparation of standard GSR solutions, we used the water solutions of the salts BaCl2, SbCl3, and Pb(NO3)2. The FRET efficiency was measured between Acf and RhB to sense the presence of GSR components (Pb+2, Ba+2, and Sb+3) in both real sample and standard solution by mixing the salts in aqueous solution. It has been observed that the FRET efficiency systematically decreases in the presence of GSR components. To amplify the FRET efficiency of the dye pair, inorganic clay dispersion (laponite) was used. The enhancement in FRET efficiency represents a better sensitivity of the proposed sensor. The current sensor is useful for the quantification of concentrations of the GSR components in a real sample.
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  • 文章类型: Journal Article
    反阴离子触发的金属离子检测很少用荧光法报道。为了解决这个具有挑战性的问题,以溴代水杨醛和水合肼为原料合成了一种荧光探针(H2L),并通过单晶X射线衍射进行结构表征。探针本身显示非常弱的荧光。然而,与其他金属离子相比,在Zn2存在下,其发射强度增加。令人惊讶的是,在Zn2+的存在下,该探针的发射曲线仅在乙酸根阴离子(OAc)作为抗衡阴离子存在时增强,可以通过光谱研究进行精确的定量分析。探针之间的组成和络合,Zn2+离子,和OAc'由ESI-MS支持,1H-NMR,和约伯的阴谋。基于这些研究,确认探针:金属之间的结合比为1:2,Zn2的检测限(LOD)为2.18µM。该探针能够在pH〜6.5-9.5的宽范围内识别Zn2离子,并且可以被EDTA有效回收。此外,从H2L与Zn2+的荧光行为出发,构建了组合分子逻辑门和存储器件,OAc,和EDTA输入基于NOT和AND门。有趣的是,聚集诱导的排放(AIEE)现象也被认为与大于50%的水含量的有机水混合物,然后用于检测通常用作炸药的苦味酸。
    Counter anion-triggered metal ion detection has been rarely reported by fluorimetric method. To address this challenging issue, a fluorescent probe (H2L) has been synthesized from bromo-salicylaldehyde and hydrazine hydrate, and structurally characterized by single crystal X-ray diffraction. The probe shows very weak fluorescence itself. However, its emission intensity increases in the presence of Zn2+ over other metal ions. Surprisingly, the emission profile of this probe in presence of Zn2+ is augmented only when acetate anion (OAc¯) is present as counter anion, that allows for precise quantitative analysis by spectroscopic studies. The compositions and complexation among the probe, Zn2+ ion, and OAc¯ are supported by ESI-MS, 1H-NMR, and Job\'s plot. Based on these studies, it is confirmed that the binding ratio between probe: metal is 1:2 and the detection limit (LOD) for the Zn2+ is 2.18 µM. The probe is capable of recognizing Zn2+ ion in the wide range of pH∼6.5-9.5, and it could be efficiently recycled by EDTA. Furthermore, the combinatorial molecular logic gate and memory device have been constructed from the fluorescent behavior of H2L with Zn2+, OAc¯, and EDTA input as based on NOT and AND gates. Interestingly, the aggregation-induced emission (AIEE) phenomenon is also perceived with greater than 50% water content in organic water mixtures, which are then useful for the detection of picric acid often used as explosive.
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  • 文章类型: Journal Article
    分子实验室的概念,这是短短二十年前提出的,吸引了科学家的想象力。从最初被提议作为由三个化学输入驱动的AND逻辑门,作为检测化学物质聚集的直接方法,构成实验室分子的定义多年来已经扩大。在这次审查中,可以通过荧光检测多种分析物的分子,在其他技术中,进行审查和讨论,在分子逻辑和多分析物传感的背景下。该评论强调了将该领域的研究前沿移至下一个维度的挑战和建议。
    The concept of a lab-on-a-molecule, which was proposed just short of two decades ago, has captured the imagination of scientists. From originally being proposed as an AND logic gate driven by three chemical inputs as a direct way of detecting congregations of chemical species, the definition of what constitutes a lab-on-a-molecule has broadened over the years. In this review, molecules that can detect multiple analytes by fluorescence, among other techniques, are reviewed and discussed, in the context of molecular logic and multi-analyte sensing. The review highlights challenges and suggestions for moving the frontiers of research in this field to the next dimension.
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  • 文章类型: Journal Article
    FDA(食品和药物管理局,(美国))将ZnO列为被广泛认为是安全的材料。使用沉淀法制备了具有一系列微小粒径的ZnONP。ZnO纳米颗粒表面装饰有含有萘酚单元的三足传感器。具有修饰在ZnONP上的相同受体的组装体与纯化的三足受体的阳离子检测能力形成对比。进行紫外可见分光光度分析以研究受体和修饰的ZnO受体的状态转变。在理想情况下通过荧光研究确定对Al3阳离子的正选择性。通过DLS和SEM分析确定相同受体-TP1的粒度和表面形态,并用三足受体TP2修饰。使用荧光开关光诱导电子转移(PET)机制,涂覆在ZnO上的受体特异性地检测Al3+离子的存在。使用B-H图方程确定结合常数值。[TP1-Al3+的结合化学计量,TP2-Al3+]显示1:1的比例。用三足受体TP1修饰的ZnO表面的荧光开关ON-OFF过程用于创建分子逻辑门,它可以作为传感器和分子开关的模块。在[TP1;TP2-Al3+]络合物溶液中加入Na2EDTA导致荧光发射显著减少。这一发现为化学传感器的可逆性提供了令人信服的支持。为了使这种传感器能够实际应用,我们已经开发了含有受体TP1和TP2的盒。成功,它可以检测Al3+金属离子。我们对测量重要工业程序产生的废水中Al3离子浓度的方法的可靠性和适当性进行了全面评估。
    The FDA (Food and Drug Administration, (USA)) lists ZnO as a material that is widely acknowledged to be safe. ZnO NPs with a range of tiny particle sizes were made using the precipitation process. ZnO nanoparticles\' surface is embellished with a tripodal sensor containing naphthol units. The assembly with the same receptor decorated on ZnO NPs is contrasted with the cation detection capabilities of the purified tripodal receptor. The UV-visible spectrophotometric analysis was conducted to study the state transitions of the receptor and the decorated ZnO receptor. A positive selectivity to Al3+ cations is determined by the fluorescence study under ideal circumstances. The particle size and surface morphologies are determined by DLS and SEM analysis for the same receptor - TP1 and embellished with a tripodal receptor TP2. Using a fluorescence switch-on Photoinduced Electron Transfer (PET) mechanism, the receptor coated on ZnO detects the presence of Al3+ ions with specificity. The binding constant value was determined using the B-H plot equation. Binding stoichiometry for [TP1-Al3+, TP2-Al3+] showed a 1:1 ratio. The fluorescence switches ON-OFF process of the ZnO surface adorned - TP2 with Tripodal receptor- TP1 was used to create molecular logic gates, which can function as a module for sensors and molecular switches. The addition of Na2EDTA in the solution of the [TP1; TP2 - Al3+] complex resulted in a noticeable reduction in the emission of fluorescence. This finding offers compelling support for the reversibility of the chemosensor. To enable the practical application of this sensor, we have developed a cassette containing receptors TP1 and TP2. Successfully, it can detect Al3+ metal ions. We performed a comprehensive assessment of the dependability and appropriateness of our approach in measuring the concentration of Al3+ ions in wastewater produced by important industrial procedures.
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  • 文章类型: Journal Article
    土壤样品中的有效重金属会对生态系统造成直接毒性,植物,和人类健康。用于可用重金属测定的传统化学提取和重组细菌方法通常存在不准确和特异性差的问题。在这项工作中,我们构造了具有分子级生物计算能力的半加法器和半减法器分子逻辑门,以智能感测可用的铅(Pb)和镉(Cd)。可用的Pb和Cd可以切割DNA酶序列以释放触发DNA,可以激活逻辑系统中的发夹式探头组件。该多功能逻辑系统不仅可以根据真值表实现对可用Pb和Cd的智能识别,还可以实现高灵敏度的同时定量,检出限为2.8pM和25.6pM,分别。逻辑生物传感器具有良好的鲁棒性,已用于测定土壤样品中的有效Pb和Cd,具有良好的准确性和可靠性。逻辑生物传感器与DTPA+ICP-MS方法之间的相对误差(Re)为-8.1%至7.9%。具有可编程性的优点,可扩展性,和多计算能力,分子逻辑系统可以提供一个简单的,快速,智能监测环境样品中有效Pb和Cd的方法。
    The available heavy metals in soil samples can cause the direct toxicity on ecosystems, plants, and human health. Traditional chemical extraction and recombinant bacterial methods for the available heavy metals assay often suffer from inaccuracy and poor specificity. In this work, we construct half adder and half subtractor molecular logic gates with molecular-level biocomputation capabilities for the intelligent sensing of the available lead (Pb) and cadmium (Cd). The available Pb and Cd can cleave DNAzyme sequences to release the trigger DNA, which can activate the hairpin probe assembly in the logic system. This multifunctional logic system can not only achieve the intelligent recognition of the available Pb and Cd according to the truth tables, but also can realize the simultaneous quantification with high sensitivity, with the detection limits of 2.8 pM and 25.6 pM, respectively. The logic biosensor is robust and has been applied to determination of the available Pb and Cd in soil samples with good accuracy and reliability. The relative error (Re) between the logic biosensor and the DTPA + ICP-MS method was from -8.1 % to 7.9 %. With the advantages of programmability, scalability, and multicomputing capacity, the molecular logic system can provide a simple, rapid, and smart method for intelligent monitoring of the available Pb and Cd in environmental samples.
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  • 文章类型: Journal Article
    我们成功合成了稳定的阴离子微孔金属-有机骨架(MOF)HDU-1([Me2NH2]2In2[(TATAB)4(DMF)4](DMF)4(H2O)4),并通过交换策略构建了荧光探针Tb@HDU-1。因为其悬浮的Tb(Ⅲ)特征跃迁和配体发射的荧光响应明显,Tb@HDU-1可以用作荧光探针,用于检测Fe3和Cu2离子。令人惊讶的是,Tb@HDU-1被用作Cu2+离子的比率荧光探针,而对Fe3+离子仅有单峰检测,其中描述了基于Ln-MOF的传感器的特定罕见示例,以区分猝灭的Fe3和Cu2离子。因此,我们设计了一种分子逻辑门器件,以使Fe3和Cu2离子的区分更加清晰和适当。此外,Fe3和Cu2离子之间的不同猝灭作用可能归因于骨架与金属离子之间的竞争吸收和相互作用的差异。
    We successfully synthesized a stable anionic microporous metal-organic framework (MOF) HDU-1 ([Me2NH2]2In2[(TATAB)4(DMF)4](DMF)4(H2O)4) and constructed a fluorescent probe Tb@HDU-1 by an exchange strategy. Because of its suspension distinct fluorescent response of Tb(III) characteristic transition and ligand emission, the Tb@HDU-1 can be used as fluorescent probe for sensing towards Fe3+ and Cu2+ ions. It is surprising that Tb@HDU-1 is used as a ratiometric fluorescent probe for Cu2+ ions while only single peak detection for Fe3+ ions, which describes a particular rare example of a sensor based on Ln-MOFs to distinguish quenching Fe3+ and Cu2+ ions. Hence we designed a molecular logic gate device for making the distinction of Fe3+ and Cu2+ ions more clearly and appropriately. In addition, the different quenching effect between Fe3+ and Cu2+ ions may be ascribed to the differences of competitive absorption and interaction between frameworks and metal ions.
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  • 文章类型: Journal Article
    农药的同时和高性能检测仍然是一个相当大的挑战和迫切需要。在这里,已经开发了基于双发射碳点(CD)的非酶荧光传感平台,在同时检测对硫磷(MP)和草甘膦方面显示出优异的灵敏度和选择性。通过对桑叶和氢氧化钠进行水热处理,制备了具有440nm(bCD)和660nm(rCD)发射的CD。bCDs通过内部过滤效应对水解MP的反应,而rCDs通过静态猝灭作用在Cu2+的辅助下感知草甘膦。发现MP(0.3-65.0μM)和草甘膦(1.0-110.0μM)具有良好的线性相关性,检出限为0.14和0.60μM。值得注意的是,提出的双通道策略成功地应用于同时检测MP和草甘膦在食品/草药样品与可接受的回收率,精度好,和高选择性。此外,实现了对食物的估计,草药,或环境安全。
    Simultaneous and high-performance detection of pesticides is still a considerable challenge and urgent need. Herein, a dual-emission carbon dots (CDs)-based nonenzymatic fluorescent sensing platform has been developed, which shows excellent sensitivity and selectivity in simultaneously detecting parathion-methyl (MP) and glyphosate. CDs with emissions at 440 nm (bCDs) and 660 nm (rCDs) were prepared by hydrothermal treatment of mulberry leaves and sodium hydroxide. bCDs response to hydrolyzed MP via inner filter effect, while rCDs sense glyphosate with the aid of Cu2+ by static quenching effect. Excellent linear correlations were found for MP (0.3-65.0 μM) and glyphosate (1.0-110.0 μM) with limits of detection at 0.14 and 0.60 μM. Notably, the presented dual-channel strategy was successfully applied in simultaneously detecting MP and glyphosate in food/herbal samples with acceptable recoveries, good precision, and high selectivity. Moreover, an ORlogicgatewas achieved for estimating food, herbal, or environmental safety.
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  • 文章类型: Journal Article
    通过自由基聚合形成的聚丙烯酰胺水凝胶是通过基于光诱导电子转移(PET)和/或内部电荷转移(ICT)捕获蒽和4-氨基-1,8-萘酰亚胺荧光逻辑门而形成的。分子在水凝胶中的非共价固定导致半固体YES,NOT,和逻辑门。两个分子与门,Pourbaix传感器的例子,用过硫酸铵在酸性甲醇水溶液中测试,一种强氧化剂,并显示出比以前报道的更大的荧光量子产率。将逻辑水凝胶暴露于具有化学输入的水溶液中,在365nm紫外光下观察荧光输出响应。当置于溶液中时,所有的分子逻辑门都在一定程度上扩散出水凝胶,特别是那些具有二级碱性胺的。该研究举例说明了将分子逻辑门从均质溶液带入固溶体环境领域的努力。我们展示了使用Pourbaix传感器作为pE-pH指标来监测氧化和酸性条件,特别是过量的过硫酸铵,一种用于SDS-聚丙烯酰胺凝胶聚合的试剂。
    Polyacrylamide hydrogels formed by free radical polymerisation were formed by entrapping anthracene and 4-amino-1,8-naphthalimide fluorescent logic gates based on photoinduced electron transfer (PET) and/or internal charge transfer (ICT). The non-covalent immobilisation of the molecules in the hydrogels resulted in semi-solid YES, NOT, and AND logic gates. Two molecular AND gates, examples of Pourbaix sensors, were tested in acidic aqueous methanol with ammonium persulfate, a strong oxidant, and displayed greater fluorescence quantum yields than previously reported. The logic hydrogels were exposed to aqueous solutions with chemical inputs, and the fluorescence output response was viewed under 365 nm UV light. All of the molecular logic gates diffuse out of the hydrogels to some extent when placed in solution, particularly those with secondary basic amines. The study exemplifies an effort of taking molecular logic gates from homogeneous solutions into the realm of solid-solution environments. We demonstrate the use of Pourbaix sensors as pE-pH indicators for monitoring oxidative and acidic conditions, notably for excess ammonium persulfate, a reagent used in the polymerisation of SDS-polyacrylamide gels.
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