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Self-confined catalytic DNA circuit for on-site nonenzymatic amplified microRNA imaging 用于现场非酶扩增microRNA成像的自限制催化DNA电路。
IF 10.5 1区 生物学 Q1 BIOPHYSICS Pub Date : 2025-11-25 DOI: 10.1016/j.bios.2025.118265
Xue Hu , Mingmeng Xie , Yuxiang Lang , Jieyuan Zhang , Lin He , Xinhui Jiang , Hecun Zou , Zhengwei Zhang , Siqiao Li
MicroRNAs (miRNAs) are critical regulators in cancer biology, yet their low abundance and high sequence similarity pose significant challenges for accurate intracellular detection. Herein, we present a metal-organic frameworks (MOFs) with self-confined catalytic DNA circuit (designated as MSCDC) integrated within a pH-responsive MIL-53(Fe) framework for on-site, nonenzymatic amplified imaging of miRNA-9 in hepatocellular carcinoma (HCC) cells. The MSCDC was synthesized by anchoring double-stemmed DNA hairpin probes onto MIL-53(Fe) through π–π stacking and electrostatic interactions, achieving high probe density and nuclease resistance. The pH-triggered degradation of MIL-53(Fe) facilitated efficient intracellular release of DNA probes, while the self-confined catalytic DNA circuit enabled autonomous, enzyme-free amplification, converting weak miRNA-9 inputs into strong fluorescence outputs. Compared with conventional carriers, the MSCDC exhibited superior probe loading capacity, enhanced serum stability, excellent biocompatibility, and a femtomolar detection limit (0.32 fM). Importantly, the nanoplatform enabled reliable, real-time visualization of oncogenic miRNA-9 in diverse HCC cell lines, yielding results that were highly consistent with qRT-PCR. This work highlights a generalizable self-confined, nonenzymatic nucleic acid amplification strategy for precise intracellular biosensing, thereby opening avenues for early cancer diagnosis and molecular imaging.
MicroRNAs (miRNAs)是癌症生物学中的重要调控因子,但它们的低丰度和高序列相似性给准确的细胞内检测带来了重大挑战。在此,我们提出了一种金属有机框架(mof),其具有自我限制的催化DNA电路(称为MSCDC),集成在ph响应MIL-53(Fe)框架中,用于肝细胞癌(HCC)细胞中miRNA-9的现场非酶扩增成像。通过π-π堆叠和静电相互作用,将双柄DNA发夹探针固定在MIL-53(Fe)上,合成了高探针密度和耐核酸酶能力的MSCDC。ph触发的MIL-53(Fe)降解促进了DNA探针在细胞内的有效释放,而自我限制的催化DNA电路实现了自主的无酶扩增,将弱miRNA-9输入转化为强荧光输出。与传统载体相比,MSCDC具有更好的探针负载能力,增强的血清稳定性,良好的生物相容性和飞摩尔检出限(0.32 fM)。重要的是,纳米平台能够可靠、实时地可视化不同HCC细胞系中的致癌miRNA-9,产生的结果与qRT-PCR高度一致。这项工作强调了一种可推广的自我限制、非酶核酸扩增策略,用于精确的细胞内生物传感,从而为早期癌症诊断和分子成像开辟了道路。
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引用次数: 0
Synergistic modulation of oxidation state of Pt nanozymes via Pd doping and ZIF-67 support enhances the catalytic efficiency for immunoassay detection 通过Pd掺杂和ZIF-67载体协同调节Pt纳米酶的氧化态,提高了免疫检测的催化效率
IF 10.5 1区 生物学 Q1 BIOPHYSICS Pub Date : 2025-11-25 DOI: 10.1016/j.bios.2025.118264
Zhenjiang Liu , Ying Yang , Weiguo Yu , Jiankun Feng , Hailong Chen , Runan Li , Longhua Li , Yuan Xue
Modulating the oxidation state of active sites presents a promising strategy for enhancing catalytic performance. However, the intrinsic electronic properties of a single regulatory strategy make it difficult to accurately control the oxidation state of nanozymes. Herein, we design high-efficiency PtXPd1@ZIF-67 nanozymes by integrating two modulation strategies (Pd doping and ZIF-67 support) to effectively regulate the oxidation state of the Pt active center. The results demonstrate that Pt4Pd1@ZIF-67 nanozyme with a moderate oxidation state exhibits the best catalytic activity, which is 1.97- and 3.87-fold higher than that of Pt@ZIF-67 and Pt@ZIF-67-S (S represents the removal of ZIF-67 support), respectively. Theoretical calculations indicate that the moderate oxidation state of Pt enhances the adsorption of OH, thereby reducing the energy barrier of the key reaction step (2∗OH → ∗O + H2O) and ultimately improving the catalytic activity of nanozyme. Crucially, Pt4Pd1@ZIF-67 nanozyme was successfully employed to develop a novel indirect competitive immunoassay for the detection of zearalenone, with a limit of detection of 0.534 ng L−1. This work provides a potential strategy for the rational design of high catalytic performance nanozymes for immunoassay detection.
调节活性位点的氧化态是提高催化性能的一种很有前途的策略。然而,单一调控策略的固有电子特性使得精确控制纳米酶的氧化状态变得困难。在此,我们设计了高效的PtXPd1@ZIF-67纳米酶,通过整合两种调制策略(Pd掺杂和ZIF-67支持)来有效调节Pt活性中心的氧化状态。结果表明,中等氧化态的Pt4Pd1@ZIF-67纳米酶表现出最好的催化活性,分别比Pt@ZIF-67和Pt@ZIF-67-S (S表示ZIF-67载体的去除)高1.97倍和3.87倍。理论计算表明,Pt的中等氧化态增强了对OH的吸附,从而降低了关键反应步骤(2 * OH→∗O + H2O)的能垒,最终提高了纳米酶的催化活性。至关重要的是,Pt4Pd1@ZIF-67纳米酶成功地开发了一种新的间接竞争免疫分析法,用于检测玉米赤霉烯酮,检测限为0.534 ng L−1。这项工作为合理设计高催化性能的纳米酶用于免疫分析检测提供了潜在的策略。
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引用次数: 0
Creating a novel halotolerant whole-cell biosensor for efficient degradation and precise quantification of p-nitrophenol-substituted organophosphate pesticides in hypersaline ecosystems 创建一种新型耐盐全细胞生物传感器,用于高盐生态系统中对硝基苯酚取代的有机磷农药的有效降解和精确定量。
IF 10.5 1区 生物学 Q1 BIOPHYSICS Pub Date : 2025-11-24 DOI: 10.1016/j.bios.2025.118240
Yujie Liu , Xinyu Zhang , Haomin Chen , Ziling Yuan , Xiujuan Tian , Nan Xu , Ruihua Liu , Chao Yang
The previously constructed biosensors for organophosphate pesticides (OPs) detection cannot be used to measure OPs concentrations under high salt conditions. In this study, a novel halotolerant whole-cell biosensor J9U-pBBR-pobRA-gfp, which consisted of a p-nitrophenol (pNP)-responsive transcription regulator PobR and its cognate promoter fused to a reporter GFP, was constructed from a salt-tolerant chassis Halomonas cupida J9 for pNP-substituted OPs detection in high-salinity environments. Through dynamic regulation of PobR expression levels, the leaky fluorescence was significantly reduced. Furthermore, the optimized biosensing circuits were introduced into an OP-degrading chassis J9U-mpd, to generate dual-functional biosensors that could degrade 40 μM methyl parathion (MP) within 80 min in high-salinity media. The biosensors exhibited broad specificity towards pNP-substituted OPs (e.g., MP and fenitrothion), while showing no response to non-pNP-substituted OPs like chlorpyrifos. Dose-response curves indicated that the three biosensors J9U-mpd-pBBR-P3 (P15 or P17) pobRA-gfp maintained a linear detection range of 0.1–60 μM for pNP and 0.1–20 μM for MP in high-saline media. Biosensors J9U-mpd-pBBR-P3 (or P17) pobRA-gfp achieved a low detection limit (LOD) of 0.1 μM for both pNP and MP in seawater and high-salinity river water, and showed a LOD of 0.019 mg/kg for pNP and 0.026 mg/kg for MP in saline-alkali soil. pNP and MP concentrations estimated by the biosensors J9U-mpd-pBBR-P3 (or P17) pobRA-gfp matched well with pollutant concentrations measured by HPLC analysis, demonstrating the reliability of the biosensor detection results. The halotolerant biosensor can be applied to efficient degradation and precise quantification of OPs in hypersaline aquatic and terrestrial ecosystems. Our strategy of combining synthetic biology with extremophile chassis may be utilized to create novel biosensors for pollutant detection in extreme environments.
以往构建的有机磷农药检测生物传感器不能用于高盐条件下有机磷农药浓度的检测。在本研究中,我们以耐盐型铜盐单胞菌J9为基础,构建了一种新型耐盐全细胞生物传感器J9U-pBBR-pobRA-gfp,该传感器由对硝基酚(pNP)应答转录调控因子PobR及其同源启动子融合到报告基因GFP中,用于在高盐度环境中检测pNP取代的OPs。通过动态调控PobR的表达水平,显著降低了漏荧光。此外,将优化后的生物传感电路引入到op降解底盘J9U-mpd中,生成的双功能生物传感器可以在80 min内降解高盐度介质中40 μM的甲基对硫磷(MP)。生物传感器对pnp取代的OPs(如MP和杀虫硫磷)表现出广泛的特异性,而对非pnp取代的OPs(如毒死蜱)没有反应。剂量响应曲线表明,J9U-mpd-pBBR-P3 (P15或P17) pobRA-gfp对高盐介质中pNP和MP的线性检测范围分别为0.1 ~ 60 μM和0.1 ~ 20 μM。J9U-mpd-pBBR-P3(或P17) pobRA-gfp生物传感器在海水和高盐度河水中对pNP和MP的检出限均为0.1 μM,在盐碱地中对pNP和MP的检出限分别为0.019 mg/kg和0.026 mg/kg。生物传感器J9U-mpd-pBBR-P3(或P17) pobRA-gfp测定的pNP和MP浓度与HPLC测定的污染物浓度吻合较好,证明了生物传感器检测结果的可靠性。耐盐生物传感器可用于高盐水生和陆地生态系统中有机磷的高效降解和精确定量。我们将合成生物学与极端微生物底盘相结合的策略可用于创建用于极端环境中污染物检测的新型生物传感器。
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引用次数: 0
CRISPR-Cas12a-integrated pregnancy test strip biosensors: Visual detection of telomerase and miRNA let-7a in cervical cancer diagnostics crispr - cas12a集成妊娠试验试纸生物传感器:端粒酶和miRNA let-7a在宫颈癌诊断中的视觉检测
IF 10.5 1区 生物学 Q1 BIOPHYSICS Pub Date : 2025-11-24 DOI: 10.1016/j.bios.2025.118241
Xiaoya Gu , Tong Zhang , Haoyan Yao , Fenglan Guo , Chenqing Yang , Huiqiu Xu , Xinyi He , Zhe Ma , Xiyuan Zhang , Shijiang Yu , Ruifang An , Fu Wang
Cervical cancer is a leading cause of female cancer-related mortality globally, and early screening based on reliable biomarkers is critical for improving prognosis. Telomerase (a key driver of cellular immortalization) and microRNA let-7a (a tumor suppressor with downregulated expression in cervical cancer) are well-validated diagnostic targets, but existing detection methods are hindered by complex procedures, high instrumentation costs, and reliance on specialized technical expertise—limiting their accessibility in resource-constrained settings. To address these limitations, we developed two novel CRISPR-Cas12a-integrated biosensors using commercially available pregnancy test strips (PTS) for instrument-free, visual readout. Both biosensors leverage a core signal mediator, probe 1 (“MB-ssDNA1-hCG”), which links CRISPR-Cas12a activation to visible color development on the PTS. The first Biosensor CRISPR-PTS-Telo detects telomerase activity in one-step without PCR: telomerase-generated (TTAGGG)n repeats activate Cas12a-crRNA1 complex, cleaving the probe 1 to release hCG, achieving a detection limit of 18 HeLa cells—comparable to sensitive laboratory assays. The second Biosensor CRISPR-PTS-let7a detects miRNA let-7a by first converting miRNA signals to Trigger DNA via Assister DNA and probe 2 (“MB-ssDNA2+Trigger”), activating Cas12a-crRNA2 complex, cleaving the probe 1 and inducing PTS coloration. This achieves a detection limit of 25.1 fM for let-7a. Validation with clinical samples (24 cervical tissues and 26 blood samples) confirmed their concordance with gold-standard methods (ELISA for telomerase, RT-qPCR for let-7a). These versatile tools hold significant potential as point-of-care testing (POCT) solutions to facilitate early, accessible cervical cancer screening.
宫颈癌是全球女性癌症相关死亡的主要原因,基于可靠生物标志物的早期筛查对于改善预后至关重要。端粒酶(细胞永生化的关键驱动因素)和microRNA let-7a(宫颈癌中表达下调的肿瘤抑制因子)是经过充分验证的诊断靶点,但现有的检测方法受到复杂的程序、高昂的仪器成本和对专业技术知识的依赖的阻碍,限制了它们在资源有限的环境下的可及性。为了解决这些限制,我们开发了两种新型的crispr - cas12a集成生物传感器,使用市售的妊娠试纸(PTS)进行无仪器的视觉读数。这两种生物传感器都利用了核心信号介质探针1(“MB-ssDNA1-hCG”),它将CRISPR-Cas12a激活与PTS上的可见颜色发展联系起来。第一种生物传感器crispr - ts - telo无需PCR即可一步检测端粒酶活性:端粒酶生成(TTAGGG)n重复序列激活Cas12a-crRNA1复合物,切割探针1以释放hCG,达到18个HeLa细胞的检测限-与敏感的实验室分析相当。第二种生物传感器CRISPR-PTS-let7a首先通过辅助DNA和探针2(“MB-ssDNA2+Trigger”)将miRNA信号转化为触发DNA,激活Cas12a-crRNA2复合物,切割探针1并诱导PTS着色,从而检测miRNA let-7a。这使得let-7a的检测极限为25.1 fM。临床样本(24份宫颈组织和26份血液样本)的验证证实了它们与金标准方法(端粒酶ELISA, let-7a RT-qPCR)的一致性。这些多功能工具具有作为即时检测(POCT)解决方案的巨大潜力,可促进早期、可获得的宫颈癌筛查。
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引用次数: 0
rGO-based porous structure modified by PPy/β-CD for 3D electrochemical chiral sensor 三维电化学手性传感器用PPy/β-CD修饰rgo基多孔结构
IF 10.5 1区 生物学 Q1 BIOPHYSICS Pub Date : 2025-11-24 DOI: 10.1016/j.bios.2025.118263
Yingyi Ma , Yu Si , Shun Yao , Xinran Li , Xinzheng Li , Jingfang Li
Chiral discrimination is crucial in medicine, food, and materials science. Herein, we report a novel electrochemical chiral sensor with a three-dimensional (3D) porous interface integrating chirality, conductivity, and porosity for efficient discrimination of tryptophan (Trp) enantiomers. The 3D porous reduced graphene oxide (p-rGO) film with enhanced nanosheet d-spacing and surface area is fabricated via a low-cost, adjustable self-assembly process, followed by electrochemical reduction. Polypyrrole (PPy) and β-cyclodextrin (β-CD) are co-deposited onto the p-rGO framework to construct the chiral sensing interface. The resulting p-rGO/PPy/β-CD electrode exhibits high enantioselectivity, enabling separate detection of D- and L-Trp and quantification of L-Trp in racemic mixtures. The superior recognition performance is attributed to the synergistic effects of the components: β-CD provides chiral cavities and hydrogen-bonding sites, PPy enhances π–π interactions and charge transfer, and p-rGO promotes electron transport and molecular adsorption. Theoretical simulations further reveal stronger hydrogen-bonding and binding energies between β-CD-PPy and L-Trp compared to D-Trp, confirming the experimentally observed selectivity. The sensor also demonstrates excellent reproducibility, stability, anti-interference ability, and applicability to real sample analysis. This work presents a general strategy for designing 3D-structured chiral sensors with high sensitivity and selectivity, highlighting the potential of integrating conductive, porous, and chiral materials for advanced electrochemical sensing platforms.
手性鉴别在医学、食品和材料科学中至关重要。在此,我们报道了一种新的电化学手性传感器,该传感器具有三维(3D)多孔界面,集成了手性,电导率和孔隙率,用于有效识别色氨酸(Trp)对映体。3D多孔还原氧化石墨烯(p-rGO)薄膜具有增强的纳米片间距和表面积,通过低成本,可调节的自组装工艺制备,然后进行电化学还原。聚吡咯(PPy)和β-环糊精(β-CD)共沉积在p-还原氧化石墨烯框架上,构建手性传感界面。所得的p-rGO/PPy/β-CD电极具有高对映选择性,可以在消旋混合物中分别检测D-和l -色氨酸,并对l -色氨酸进行定量。优异的识别性能归功于各组分的协同作用:β-CD提供手性空腔和氢键位点,PPy增强π -π相互作用和电荷转移,p-rGO促进电子传递和分子吸附。理论模拟进一步揭示了β-CD-PPy和l -色氨酸之间的氢键和结合能比d -色氨酸更强,证实了实验观察到的选择性。该传感器还具有良好的再现性、稳定性、抗干扰能力和对实际样品分析的适用性。这项工作提出了设计具有高灵敏度和选择性的3d结构手性传感器的一般策略,突出了集成导电,多孔和手性材料用于先进电化学传感平台的潜力。
{"title":"rGO-based porous structure modified by PPy/β-CD for 3D electrochemical chiral sensor","authors":"Yingyi Ma ,&nbsp;Yu Si ,&nbsp;Shun Yao ,&nbsp;Xinran Li ,&nbsp;Xinzheng Li ,&nbsp;Jingfang Li","doi":"10.1016/j.bios.2025.118263","DOIUrl":"10.1016/j.bios.2025.118263","url":null,"abstract":"<div><div>Chiral discrimination is crucial in medicine, food, and materials science. Herein, we report a novel electrochemical chiral sensor with a three-dimensional (3D) porous interface integrating chirality, conductivity, and porosity for efficient discrimination of tryptophan (Trp) enantiomers. The 3D porous reduced graphene oxide (p-rGO) film with enhanced nanosheet d-spacing and surface area is fabricated via a low-cost, adjustable self-assembly process, followed by electrochemical reduction. Polypyrrole (PPy) and <em>β</em>-cyclodextrin (<em>β</em>-CD) are co-deposited onto the p-rGO framework to construct the chiral sensing interface. The resulting p-rGO/PPy/<em>β</em>-CD electrode exhibits high enantioselectivity, enabling separate detection of D- and L-Trp and quantification of L-Trp in racemic mixtures. The superior recognition performance is attributed to the synergistic effects of the components: <em>β</em>-CD provides chiral cavities and hydrogen-bonding sites, PPy enhances π–π interactions and charge transfer, and p-rGO promotes electron transport and molecular adsorption. Theoretical simulations further reveal stronger hydrogen-bonding and binding energies between <em>β</em>-CD-PPy and L-Trp compared to D-Trp, confirming the experimentally observed selectivity. The sensor also demonstrates excellent reproducibility, stability, anti-interference ability, and applicability to real sample analysis. This work presents a general strategy for designing 3D-structured chiral sensors with high sensitivity and selectivity, highlighting the potential of integrating conductive, porous, and chiral materials for advanced electrochemical sensing platforms.</div></div>","PeriodicalId":259,"journal":{"name":"Biosensors and Bioelectronics","volume":"295 ","pages":"Article 118263"},"PeriodicalIF":10.5,"publicationDate":"2025-11-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145622262","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
DNAzyme walker–triggered HCR dual amplification mediated by MOF-derived bimetallic Fe-Ni–doped porous carbon nanozyme for homogeneous dual-mode aptasensor detection of profenofos mof衍生的双金属fe - ni掺杂多孔碳纳米酶介导的DNAzyme步行者触发HCR双扩增用于均匀双模适体传感器检测丙烯诺威。
IF 10.5 1区 生物学 Q1 BIOPHYSICS Pub Date : 2025-11-22 DOI: 10.1016/j.bios.2025.118261
Yifan Xu , Baoshan He , Ming Lu , Zhengyong Liang , Longdi Wang , Wenhong Zhao , Ligen Wu , Dongdong Xie
Profenofos (PFF), a widely utilized organophosphorus pesticide, readily accumulates in crops and poses neurotoxic risks to humans. However, rapid and precise detection of PFF in complex matrices remains challenging. Herein, we report a homogeneous dual-mode aptasensor integrating a DNAzyme walker and hybridization chain reaction (HCR) cascade, mediated by a MOF-derived bimetallic Fe–Ni–doped porous carbon nanozyme (FeNi-C). We synthesized a porous Fe-Ni–doped carbon material (FeNi-C) derived from Fe-Ni metal–organic frameworks (FeNi-MOFs) by carefully tuning carbonization conditions, resulting in exceptional peroxidase-like (POD-like) catalytic activity. Subsequently, FeNi-C immobilized with platinum nanoparticles (Pt@FeNi-C) served as nanozyme probes. The synergistic interaction among the bimetallic composition, porous structure, and high specific surface area was found to endow FeNi-C with superior catalytic and kinetic properties, while the platinum deposited on its surface further enhanced the catalytic activity and served as a stable site for DNA. Additionally, the DNAzyme–driven walker enhanced the efficiency of PFF recognition, with the hybridization chain reaction (HCR) cascade simultaneously reducing steric hindrance and introducing additional Pt@FeNi-C probes, thereby amplifying the detection signals. Pt@FeNi-C efficiently catalyzed TMB redox reactions in the presence of H2O2, simultaneously generating electrochemical and colorimetric signals. Using TMB as substrate enabled homogeneous detection for PFF, avoiding the complex electrode construction process. In addition, the dual-mode signal output detection effectively minimized background interference and enhanced analytical reliability. The aptasensor achieved detection limits of 4.32 fg/mL (electrochemical mode) and 20.80 fg/mL (colorimetric mode), showing promise for environmental monitoring and food safety.
丙烯磷农药(Profenofos, PFF)是一种广泛使用的有机磷农药,极易在农作物中积累,对人体具有神经毒性风险。然而,快速准确地检测复杂矩阵中的PFF仍然具有挑战性。在此,我们报道了一种均匀的双模式感应传感器,集成了DNAzyme助行器和杂交链反应(HCR)级联,由mof衍生的双金属fe - ni掺杂多孔碳纳米酶(FeNi-C)介导。我们通过精心调整碳化条件,合成了Fe-Ni金属有机骨架(FeNi-MOFs)衍生的多孔Fe-Ni掺杂碳材料(FeNi-C),从而获得了优异的过氧化物酶(POD-like)催化活性。随后,用铂纳米颗粒(Pt@FeNi-C)固定FeNi-C作为纳米酶探针。双金属组成、多孔结构和高比表面积之间的协同作用赋予了FeNi-C优越的催化和动力学性能,而沉积在其表面的铂进一步增强了催化活性,并作为DNA的稳定位点。此外,dnazyme驱动的助行器提高了PFF识别的效率,其杂交链反应(HCR)级联同时降低了位阻并引入了额外的Pt@FeNi-C探针,从而放大了检测信号。Pt@FeNi-C在H2O2存在下有效催化TMB氧化还原反应,同时产生电化学和比色信号。使用TMB作为衬底可以实现PFF的均匀检测,避免了复杂的电极构建过程。此外,双模信号输出检测有效地减少了背景干扰,提高了分析可靠性。该传感器的检出限分别为4.32 fg/mL(电化学模式)和20.80 fg/mL(比色模式),有望用于环境监测和食品安全。
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引用次数: 0
An intelligent molecularly imprinted sensing platform augmented by interval partial least squares for specific detection of mycophenolic acid in agricultural silage 基于区间偏最小二乘增强的智能分子印迹检测平台用于青贮饲料中霉酚酸的特异性检测
IF 10.5 1区 生物学 Q1 BIOPHYSICS Pub Date : 2025-11-21 DOI: 10.1016/j.bios.2025.118254
Qiang Zhu , Shuyu Jiang , Jiaxiong Zou , Peng Liu , Zuo Wang , Weijun Shen , Xinyi Lan , Tingting Chu , Qianglin Liu , Yangping Wen , Fachun Wan , Yu Ge
Mycophenolic acid (MPA), a prevalent mycotoxin, presents significant analytical challenges in complex silage matrices due to limited selectivity and pronounced electrochemical baseline drift. To address this, we developed an intelligent molecularly imprinted sensor (Fe3O4-MGO/MIP/GCE) for the sensitive and selective detection of MPA. This sensing platform incorporates Fe3O4 modified magnetic graphene oxide (Fe3O4-MGO) as a highly conductive nanocomposite substrate, with pyrrole-3-carboxylic acid (Py3C) serving as a dual-functional monomer. Py3C was electropolymerized in the presence of MPA to form recognition sites that also function as signal transducers. Furthermore, to overcome signal instability and subjective interpretation, we integrated a machine learning-assisted approach using a small-window moving average algorithm for automated baseline correction, coupled with interval partial least squares (iPLS) for precise peak identification. This data-driven strategy eliminates manual intervention, enhances signal fidelity, and improves analytical robustness in complex environments. The sensor demonstrated a wide linear range from 7.5 nmol L-1 to 5 μmol L-1, with a low detection limit of 2.1 nmol L-1 (S/N = 3). Recovery rates in real silage samples ranged from 91.5 % to 102.4 %, confirming high accuracy and strong anti-interference capability. This work successfully merges biomimetic molecular recognition with intelligent signal processing, offering a reliable and objective platform for the on-site monitoring of mycotoxins in agricultural systems.
霉酚酸(MPA)是一种常见的霉菌毒素,由于选择性有限和电化学基线漂移明显,在复杂的青贮基质中提出了重大的分析挑战。为了解决这一问题,我们开发了一种智能分子印迹传感器(Fe3O4-MGO/MIP/GCE),用于灵敏和选择性地检测MPA。该传感平台采用Fe3O4修饰磁性氧化石墨烯(Fe3O4- mgo)作为高导电性纳米复合衬底,并以吡咯-3羧酸(Py3C)作为双功能单体。Py3C在MPA存在下电聚合,形成识别位点,也起到信号换能器的作用。此外,为了克服信号不稳定性和主观解释,我们集成了一种机器学习辅助方法,使用小窗口移动平均算法进行自动基线校正,并结合区间偏最小二乘(iPLS)进行精确的峰值识别。这种数据驱动策略消除了人工干预,增强了信号保真度,并提高了复杂环境中的分析鲁棒性。该传感器线性范围为7.5 ~ 5 μmol L-1,检出限低至2.1 nmol L-1 (S/N = 3)。在实际青贮样品中的回收率为91.5% ~ 102.4%,准确度高,抗干扰能力强。本研究成功地将仿生分子识别与智能信号处理相结合,为农业系统真菌毒素的现场监测提供了可靠、客观的平台。
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引用次数: 0
MOFs-on-MOFs modified wearable electrochemical microneedle array for uric acid detection 用于尿酸检测的MOFs-on-MOFs修饰的可穿戴电化学微针阵列。
IF 10.5 1区 生物学 Q1 BIOPHYSICS Pub Date : 2025-11-21 DOI: 10.1016/j.bios.2025.118246
Tayyaba Iftikhar , Tahir Imran , Jinhua He , Chuangjie Zhang , Yuanting Xie , Haitao Ye , Lei Su
Conventional UA detection relies on invasive blood or urine tests, limiting convenience and real-time monitoring. In this study, we have designed a novel microneedle array-based wearable electrochemical sensor to detect UA in skin interstitial fluid (ISF), which consists of a bi-metal-organic framework (bi-MOF) modified screen-printed electrode (SPE) and 3D-printed hollow microneedle array patch (HMNsAP). To this end, a “MOFs on MOFs” strategy was applied by combining HKUST-1 and Eu-MOF nanocomposites on an SPE, enhancing electrode surface area, electrode material porosity, and electron transfer efficiency. The HMNsAP was equipped with a microvalve and connected to a vacuum tube to facilitate efficient ISF extraction while preventing backflow to mitigate biosafety risk. The sensor showed outstanding analytical performance, with a low limit of detection of 20 nM and high recovery rates ranging from 98.6% to 100.4% across various UA concentrations in ex-vivo rat skin tests, along with strong selectivity and reproducibility, indicated by a relative standard deviation (RSD = 1.68%). These findings underscore the synergistic advantages of combining advanced MOF materials with an innovative microneedle system for precise UA monitoring in ISF, enhancing its role in personalized diagnostics and beyond.
传统的UA检测依赖于侵入性血液或尿液检测,限制了便利性和实时监测。在这项研究中,我们设计了一种新型的基于微针阵列的可穿戴电化学传感器,用于检测皮肤间质液(ISF)中的UA,该传感器由双金属有机框架(bi-MOF)修饰的丝网印刷电极(SPE)和3d打印空心微针阵列贴片(HMNsAP)组成。为此,通过在SPE上结合HKUST-1和Eu-MOF纳米复合材料,采用“mof上mof”策略,提高了电极表面积、电极材料孔隙率和电子传递效率。HMNsAP配备了一个微阀,并连接到真空管,以促进有效的ISF提取,同时防止回流,降低生物安全风险。该传感器具有出色的分析性能,在不同UA浓度的离体大鼠皮肤试验中,低检出限为20 nM,回收率为98.6% ~ 100.4%,具有较强的选择性和重复性,相对标准偏差(RSD = 1.68%)。这些发现强调了将先进的MOF材料与创新的微针系统相结合的协同优势,可以在ISF中进行精确的UA监测,增强其在个性化诊断等方面的作用。
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引用次数: 0
Bio-hybrid Photovoltaic devices operated on living photosynthetic bacteria 生物混合光电装置以活的光合细菌为动力
IF 10.5 1区 生物学 Q1 BIOPHYSICS Pub Date : 2025-11-21 DOI: 10.1016/j.bios.2025.118260
Rossella Labarile , Anna De Salvo , Federico Rondelli , Maria Michela Giangregorio , Michele Di Lauro , Massimo Trotta , Gianluca Maria Farinola , Fabio Biscarini
The use of the abundant and easily available solar energy is central towards a carbon-free society and represents the most sustainable strategy for the increasing energy demand. Rhodobacter (R.) sphaeroides is a versatile photosynthetic purple non sulfur bacteria able to harvest sunlight, particularly in the Near InfraRed (NIR) region, and to efficiently transform it into photochemical energy. In this work, whole wild-type, metabolically-active photosynthetic bacterial cells of R. sphaeroides, and their carotenoid-less mutant strain, were integrated in a two-electrode architecture, to output a positive photovoltage upon illumination. The photovoltage amplitude of the mutant strain is almost three times higher than that obtained with wild-type cells. Photosynthetic bacteria were also integrated in a light-electrolyte-gated organic transistor to produce a photomodulated electronic current, as well as in a biophotonic power cell working on direct sunlight. This proves that bio-organic hybrid optoelectronic devices may enable environmentally safe and cost-effective energy production.
利用丰富且容易获得的太阳能是实现无碳社会的核心,也是应对不断增长的能源需求的最可持续战略。球形红杆菌(R.)是一种多功能的光合紫色无硫细菌,能够收集阳光,特别是在近红外(NIR)区域,并有效地将其转化为光化学能。在这项工作中,整个野生型,具有代谢活性的光合细菌细胞,以及它们不含类胡萝卜素的突变株,被整合在一个双电极结构中,在光照下输出正光电压。突变株的光电压振幅几乎是野生型细胞的三倍。光合细菌也被集成在光电解质门控有机晶体管中,以产生光电调制电流,以及在阳光直射下工作的生物光子电池中。这证明了生物有机混合光电器件可以实现环境安全且具有成本效益的能源生产。
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引用次数: 0
A modular platform for surface-bound biosensing: SpyCatcher-Mediated functionalization of antifouling polypeptide brushes on gold and polystyrene 表面结合生物传感的模块化平台:spycatch介导的黄金和聚苯乙烯防污多肽刷的功能化
IF 10.5 1区 生物学 Q1 BIOPHYSICS Pub Date : 2025-11-21 DOI: 10.1016/j.bios.2025.118251
Chuanbao Zheng , Zohaib Hussain , Amanda de Souza , Chang Chen , Walter van Slooten , Siddharth Deshpande , Zhisen Zhang , Han Zuilhof , Renko de Vries
Precise molecular engineering of surfaces is critical for advancing biosensing, antifouling technologies, and smart material interfaces, yet current methods often suffer from uncontrolled orientation or require complex surface chemical modifications. Here, we report a modular protein-based platform that combines two key elements: (1) self-assembling B-M-E protein antifouling brushes composed of a solid-binding peptide (B), a multimerization domain (M), and an antifouling polypeptide (E). (2) Bioorthogonal SpyCatcher/SpyTag chemistry for precise post-assembly covalent immobilization of target molecules with site-specific control. We demonstrate high-efficiency conjugation on both gold and polystyrene surfaces using quartz crystal microbalance with dissipation (QCM-D) and fluorescence assays. This bioorthogonal strategy offers one-step surface coating without complex chemical modifications, tunable and stable protein immobilization, and universal substrate compatibility. Our post-assembly functionalization platform provides a versatile toolbox for creating functional protein coatings by suppressing non-specific binding, which minimizes background interference and improves detection sensitivity and specificity. This approach holds significant potential for applications such as point-of-care diagnostics and continuous monitoring devices.
精确的表面分子工程对于推进生物传感、防污技术和智能材料界面至关重要,但目前的方法往往受到不受控制的方向或需要复杂的表面化学修饰的影响。在这里,我们报道了一个模块化的基于蛋白质的平台,它结合了两个关键要素:(1)由固体结合肽(B)、多聚结构域(M)和防污多肽(E)组成的自组装B-M-E蛋白防污刷。(2)生物orthogonal SpyCatcher/SpyTag化学用于精确的组装后共价固定目标分子,具有位点特异性控制。我们展示了在金和聚苯乙烯表面的高效共轭使用石英晶体微天平耗散(QCM-D)和荧光分析。这种生物正交策略提供了无需复杂化学修饰的一步表面涂层,可调和稳定的蛋白质固定,以及普遍的底物兼容性。我们的装配后功能化平台提供了一个多功能工具箱,通过抑制非特异性结合来创建功能性蛋白质涂层,从而最大限度地减少背景干扰,提高检测灵敏度和特异性。这种方法对于即时诊断和连续监测设备等应用具有巨大的潜力。
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Biosensors and Bioelectronics
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