Molecular logic gates

分子逻辑门
  • 文章类型: Journal Article
    纳米酶是一类具有生物催化功能和类酶活性的纳米材料,其优点包括高稳定性,低成本,和大规模生产。它们可以催化基于特定纳米结构的天然酶的底物,并作为天然酶的替代品。他们的应用研究涉及生物医学等广泛领域,环境治理,农业,和食物。分子逻辑门是一门新兴的交叉学科,可以在分子尺度上模拟硅电路的功能,执行单个或多个输入逻辑运算,并生成逻辑输出。分子逻辑门是一种二进制操作,根据布尔逻辑的规则将输入信号转换为输出信号,产生两个信号,高水平,和低水平。高电平和低电平表示逻辑门的“真”和“假”值,它们的输出对应于分子逻辑门的\"l\"和\"0\",分别。纳米酶和逻辑门的结合是一个新颖而有吸引力的研究方向,两者的交叉应用为各个领域带来了新的机遇和思路,比如建造高效的生物计算机,智能药物输送系统,和疾病的精确诊断。这篇综述描述了基于纳米酶的逻辑门的应用,这有望为研究人员的后续研究提供一定的理论基础。
    Nanozymes are a class of nanomaterials with biocatalytic function and enzyme-like activity, whose advantages include high stability, low cost, and mass production. They can catalyze the substrates of natural enzymes based on specific nanostructures and serve as substitutes for natural enzymes. Their applied research involves a wide range of fields such as biomedicine, environmental governance, agriculture, and food. Molecular logic gates are a new cross-disciplinary discipline, which can simulate the function of silicon circuits on a molecular scale, perform single or multiple input logic operations, and generate logic outputs. A molecular logic gate is a binary operation that converts an input signal into an output signal according to the rules of Boolean logic, generating two signals, a high level, and a low level. The high and low levels represent the \"true\" and \"false\" values of the logic gates, and their outputs correspond to \"l\" and \"0\" of the molecular logic gates, respectively. The combination of nanozymes and logic gates is a novel and attractive research direction, and the cross-application of the two brings new opportunities and ideas for various fields, such as the construction of efficient biocomputers, intelligent drug delivery systems, and the precise diagnosis of diseases. This review describes the application of logic gates based on nanozymes, which is expected to provide a certain theoretical foundation for researchers\' subsequent studies.
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  • 文章类型: Journal Article
    开发具有最高级荧光增强因子(F/F0)的可激活荧光探针以提高信噪比(S/N)仍然是一个紧迫的问题。“AND”分子逻辑门正在成为增强探针选择性和准确性的有用工具。这里,“AND”逻辑门被开发为超级增强器,用于设计具有巨大F/F0和S/N比的可激活探针。它利用脂滴(LD)作为可控背景输入,并将目标分析物设置为可变输入。由于双重锁定,荧光非常猝灭,因此获得目标分析物的极端F/F0比。重要的是,此探针可以在响应发生后转移到LD。目标分析物可以在没有对照组的情况下通过空间位置直接可视化。因此,从头设计过氧亚硝酸盐(ONOO-)可激活探针(CNP2-B)。CNP2-B与ONOO-反应后的F/F0达到2600。此外,CNP2-B在被激活后可以从线粒体转移到脂滴。在体外和体内,CNP2-B的选择性和S/N比高于市售探针3'-(对羟基苯基)荧光素(HPF)。因此,在用原位CNP2-B探针凝胶给药后,清楚地描绘了小鼠模型中的动脉粥样硬化斑块。设想这种输入可控的“与”逻辑门以执行更多的成像任务。
    Developing activatable fluorescent probes with superlative fluorescence enhancement factor (F/F0 ) to improve the signal-to-noise (S/N) ratio is still an urgent issue. \"AND\" molecular logic gates are emerging as a useful tool for enhanced probes selectivity and accuracy. Here, an \"AND\" logic gate is developed as super-enhancers for designing activatable probes with huge F/F0 and S/N ratio. It utilizes lipid-droplets (LDs) as controllable background input and sets the target analyte as variable input. The fluorescence is tremendously quenching due to double locking, thus an extreme F/F0 ratio of target analyte is obtained. Importantly, this probe can transfer to LDs after a response occurs. The target analyte can be directly visualized through the spatial location without a control group. Accordingly, a peroxynitrite (ONOO- ) activatable probe (CNP2-B) is de novo designed. The F/F0 of CNP2-B achieves 2600 after reacting with ONOO- . Furthermore, CNP2-B can transfer from mitochondria to lipid droplets after being activated. The higher selectivity and S/N ratio of CNP2-B are obtained than commercial probe 3\'-(p-hydroxyphenyl) fluorescein (HPFin vitro and in vivo. Therefore, the atherosclerotic plaques at mouse models are delineated clearly after administration with in situ CNP2-B probe gel. Such input controllable \"AND\" logic gate is envisioned to execute more imaging tasks.
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  • 文章类型: Journal Article
    探索具有高可靠性和高精度的智能荧光材料来诊断疾病具有重要意义,但仍然是巨大的挑战。在这里,基于配位合成后改性,制备了Tb3+官能化的ME-PA(Tb@1),它可以通过LMCT-ET过程从ME-PA到Tb3+离子发出明亮的绿色荧光。Tb@1可以同时区分色氨酸(Try)及其代谢产物5-羟基吲哚-3-乙酸(5-HIAA),两个有效的抑郁症指标,在比率和比色模式。这种传感器具有效率高、灵敏度高的优点,以及出色的可重用性和抗干扰性。从ME到Try和5-HIAA的PET工艺,分析物与Tb@1之间的竞争吸收可能与传感机理有关。在现实的血清或尿液环境中,Tb@1对Try和5-HIAA的检出限分别为0.0183和0.0149mg/L。此外,结合反向传播神经网络(BPNN),进一步设计了两个可循环计算的双输出分子逻辑门,实现了对电子元器件的智能控制,以识别两种生物标志物的存在,并从荧光图像中判断其浓度。这项工作提供了一种新颖的方法来调制基于ML辅助HOF荧光传感器的逻辑电路,具有很好的应用于精确和图像的抑郁症诊断。本文受版权保护。保留所有权利。
    Exploring intelligent fluorescent materials with high reliability and precision to diagnose diseases is significant but remains a great challenge. Herein, based on coordination post-synthetic modification, a Tb3+ functionalized ME-PA (Tb@1) is prepared, which can emit brilliant green fluorescence through ligand-to-mental charge transfer-assisted energy transfer (LMCT-ET) process from ME-PA to Tb3+ ions. Tb@1 can simultaneously distinguish Tryptophan (Try) and its metabolite 5-hydroxyindole-3-acetic acid (5-HIAA), two effective indicators for depression, in ratio and colorimetric mode. And this sensor behaves the advantages of high efficiency and sensitivity, as well as excellent reusability and anti-interference. The PET process from ME to Try and 5-HIAA, and the competitive absorption between analytes and Tb@1 may be relevant to sensing mechanism. In realistic serum or urine environment, the detection limits of Tb@1 for Try and 5-HIAA are 0.0183 and 0.0149 mg L-1 respectively. Moreover, in conjunction with back propagation neural network (BPNN), two dual-output molecular logic gates that can be calculated circularly are further designed, which realizes intelligent control of the electronic component to identify the existence of two biomarkers and judge their concentrations from fluorescence images. This work offers a novel approach to modulate logic circuits based on ML-assisted HOF fluorescent sensor, with promising application for a precise and pictorial depression diagnosis.
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  • 文章类型: Journal Article
    在目前的工作中,精心设计了包含“Y”结结构的G-四链体,我们演示了几个新的和无标签的电化学逻辑门操作(OR,AND,NOR,和NAND)通过定义两个不同的生物分子,人8-氧代-7,8-二氢鸟嘌呤DNA糖基化酶1(hOGG1)和microRNA-141(miRNA-141),作为输入。\"Y\"连接结构固定在金电极表面作为信号转导平台。具有不同组合的输入分子的存在可以改变\“Y\”连接结构,从而通过8-oxoG位点特异性裂解和miRNA-141触发的\“Y\”置换破坏完整G-四链体的形成连接。因此,血红素与G-四链体序列的随后结合在电极上的血红素的电化学还原后产生了显着的电流变化输出。导致不同逻辑运算的成功功能,而无需用电活性物质标记DNA序列。具有具有不同输入和无标签电化学格式的多种逻辑运算的优点,这种分子逻辑门可以潜在地为开发用于各种应用的简单和强大的生物逻辑门提供有希望的机会。
    In current work, with elaborate designs of G-quadruplex containing \"Y\" junction structures, we demonstrate the construction of several new and label-free electrochemical logic gate operations (OR, AND, NOR, and NAND) by defining two distinct biomolecules, human 8-oxo-7,8-dihydroguanine DNA glycosylase 1 (hOGG1) and microRNA-141 (miRNA-141), as the inputs. The \"Y\" junction structures are immobilized onto the surface of gold electrode as the signal transduction platform. The presence of the input molecules with different combinations can alter the \"Y\" junction structures to disrupt the formation of the complete G-quadruplexes via 8-oxoG-site specific cleavage and miRNA-141-triggered displacement of the \"Y\" junctions. Subsequent association of hemin with the G-quadruplex sequences thus yields significant current variation outputs upon electrochemical reduction of hemin on the electrode, leading to the successful function of different logic operations without the involvement of labeling the DNA sequences with electro-active species. Featured with the advantages of multiple logic operations with distinct inputs and the label-free electrochemical format, such molecular logic gates can potentially provide promising opportunities for the development of simple and robust biological logic gates for various applications.
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  • 文章类型: Journal Article
    对大规模集成逻辑系统的需求不断增长,促使多读出分子逻辑门的发展。尤其是,探索同时具有荧光(FL)和磁共振(MR)信号作为可测量输出的双读出逻辑器件具有重要意义,因为FL/MR的信号组合可能使分子逻辑设备在生物医学应用中具有更好的实用性。在这项研究中,掺钬(III)的碳纳米点(Ho-CD),在FL和MR信号中均表现出pH响应行为,通过简单的一锅热解法合成。当被H+触发时,Fe3+,或Fe2+,Ho-CD用作FL和MR信号的开关,导致双读出和多寻址逻辑门。一系列基本布尔运算,包括YES,NOT,OR,NOR,XOR,通过改变H+/Fe3+/Fe2+的化学输入,已经成功地证明了PASS0和INH。更重要的是,具有更高函数(NOR-INH和MR(XOR+INH)-OR)的多级积分布尔运算,实现不同逻辑门的串联,也得到了成功的证明。这项研究可能为多层次设计铺平道路,双读出分子逻辑系统具有更好的操作稳定性,这在未来的生物医学应用中具有巨大的潜力。
    The increasing demand for large-scale integrated logic systems urges the development of multireadout molecular logic gates. Especially, it is of great significance to explore dual-readout logic devices with both fluorescence (FL) and magnetic resonance (MR) signals as measurable outputs, since the signal combination of FL/MR might render molecular logic devices better practicality in biomedical applications. In this study, holmium(III)-doped carbon nanodots (Ho-CDs), which exhibited pH-responsive behaviors in both FL and MR signals, were synthesized by a facile one-pot pyrolysis method. When triggered by H+, Fe3+, or Fe2+, the Ho-CDs served as a switch for both FL and MR signals, leading to dual-readout and multiaddressable logic gates. A series of elementary Boolean operations including YES, NOT, OR, NOR, XOR, PASS 0, and INH have been successfully demonstrated by varying the chemical inputs of H+/Fe3+/Fe2+. More importantly, multilevel integrative Boolean operations with higher functions (NOR-INH and MR (XOR + INH)-OR), which realize the concatenation of different logic gates, have also been successfully demonstrated. This study may pave an avenue to design multilevel, dual-readout molecular logic systems with better operation stability, which hold great potential for biomedical applications in the future.
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  • 文章类型: Journal Article
    The widespread use of antibiotics caused severe problems of antibiotic residues in foodstuffs and water, posing a serious threat to public health and thus urging the development of sensitive, selective, and rapid detection methods for antibiotics. In this study, a fluorescence resonance energy transfer (FRET)-based system is developed for the multiplexed analysis of chloramphenicol (CAP) and streptomycin (Strep) with detection limits of 2.51 and 8.69μg l-1, respectively. The FRET-based system consists of Cy3-tagged anti-CAP aptamer-conjugated gold nanoparticles (AuNPs) (referred to as AuNPs-AptCAP) and Cy5-tagged anti-Strep aptamer-conjugated AuNPs (referred to as AuNPs-AptStrep). In addition, AuNPs-AptCAP and AuNPs-AptStrep have been demonstrated to serve as signal transducers for implementing a series of logic operations such as YES, NOT, INH, OR, (2-4)-Decoder and even more complicated multi-level logic gates (OR-INH). Based on the outputs of logic operations, it could be figured out whether targeted analytes were present or not, thus enabling multiplex sensing and evaluation of pollution status. This proof of concept study might provide a new route for the enhanced sensing performance to distinguish different pollution status as well as the design of molecular mimics of logic elements to demonstrate better applicability.
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  • 文章类型: Journal Article
    Molecular switching memories have gained great importance in recent years because of the current sharp increase in the production of consumer electronics. Herein, 3D-printed nanocomposite carbon electrodes (3D-nCEs) have been explored as unconventional responsive interfaces to electrically readout bistable molecular switches via electrochemical impedance spectroscopy as the output system. As a proof-of-concept, two different 3D-printed responsive interfaces have been devised using surface engineering for covalently anchoring (supra)molecular components that well-define two electrical states (on/off) driven by either electrical or optical stimuli. Accordingly, this work paves the way for the functionalization of 3D-nCEs through fundamental chemistry, opening up new horizons in unprecedented tailored 3D-printed responsive interfaces which could be utilized as potential (bio)sensors, (opto)electronic devices, or molecular logic gates.
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    Due to structual polymorphism, excellent binding activity and functional significances in biological regulation, G-quadruplex has become the focus of research as an innovated module for analytical chemistry and biomedicine. Meanwhile, in the biosensor fields, new nanomaterial graphene oxide (GO) has also received extensive attention due to its brilliant physical and chemical properties. Herein, we propose a non-label and enzyme-free logic operation platform based on G-quadruplex structure and GO instead of any expensive modification. Taking advantage of the quenching ability of GO to AgNCs and the fluorescence enhancement of NMM (N-methylmesoporphyrin IX) mediated by the split G-quadruplex, a series of binary logic gates (AND, OR, INHIBIT, XOR) have been constructed and verified by biological experiments. Subsequently, two combinatorial logic gates were successfully realized conceptually on the basis of the same BGG platform, including half adder and half subtractor. Taken together, such a universal platform has great potential in applications, such as biocomputing, bio-imaging and disease diagnosis, which cultivate a new view for future biological research.
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    A novel near-infrared fluorescent chemosensor based on BODIPY (Py-1) has been synthesized and characterized. Py-1 displays high selectivity and sensitivity for sensing Cu(2+) over other metal ions in acetonitrile. Upon addition of Cu(2+) ions, the maximum absorption band of Py-1 in CH3CN displays a red shift from 603 to 608 nm, which results in a visual color change from pink to blue. When Py-1 is excited at 600 nm in the presence of Cu(2+), the fluorescent emission intensity of Py-1 at 617 nm is quenched over 86%. Notably, the complex of Py-1-Cu(2+) can be restored with the introduction of EDTA or S(2-). Consequently, an IMPLICATION logic gate at molecular level operating in fluorescence mode with Cu(2+) and S(2-) as chemical inputs can be constructed. Finally, based on the reversible and reproducible system, a nanoscale sequential memory unit displaying \"Writing-Reading-Erasing-Reading\" functions can be integrated.
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