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PHANTOM platform integrating photothermal PCR and swCNT-FET for rapid molecular diagnostics. 幻影平台集成光热PCR和swcnts - fet快速分子诊断。
IF 11.8 1区 生物学 Q1 BIOPHYSICS Pub Date : 2026-11-15 Epub Date: 2026-08-03 DOI: 10.1016/j.bios.2026.119088
Jingrui Wu, Da Eun Oh, Hyunju Cho, Jiwoong Son, Hua Mi, Hong-Seog Park, Yung-Kang Peng, Jwa-Min Nam, Tae Hyun Kim, Jung-Hoon Lee

Plasmonic photothermal polymerase chain reaction (PPT-PCR) is a nucleic acid amplification technique that utilizes the localized surface plasmon resonance effect of plasmonic nanomaterials under the irradiation of light with specific wavelengths to achieve rapid thermal cycling. PPT-PCR is considered as a next-generation PCR technique due to the potential to be applied to the development of point-of-care diagnostics and the fast, sensitive and accurate detection performance. In this study, we present PHANTOM, a proof-of-concept system that functionally integrates plasmonic photothermal PCR, magnetic nanoparticle removal, and swCNT-FET-based label-free electrical readout for rapid molecular diagnostics. The swCNT-FET sensor exhibits high sensitivity, capable of detecting low concentrations of target nucleic acids within minutes after PPT-PCR amplification. Besides, to improve the specificity of the assay, we introduce a hairpin structured primer to generate amplicons with an external single-strand tail that can hybridize with probes modified on the swCNT-FET sensor. With this design, an estimated limit of detection of 1.5 aM (experimentally validated down to 10 aM) was achieved within 20 min.

等离子体光热聚合酶链式反应(Plasmonic photothermal polymerase chain reaction, pt - pcr)是利用等离子体纳米材料在特定波长光照射下的局部表面等离子体共振效应,实现快速热循环的核酸扩增技术。由于具有快速、灵敏和准确的检测性能,pt -PCR被认为是下一代PCR技术的发展方向。在这项研究中,我们提出了PHANTOM,这是一种概念验证系统,功能集成了等离子光热PCR,磁性纳米颗粒去除和基于swcnts - fet的无标记电子读数,用于快速分子诊断。swcnts - fet传感器具有高灵敏度,能够在PPT-PCR扩增后几分钟内检测低浓度的靶核酸。此外,为了提高检测的特异性,我们引入了一个发夹结构的引物来产生带有外部单链尾部的扩增子,该扩增子可以与在swcnts - fet传感器上修饰的探针杂交。通过这种设计,在20 min内实现了1.5 aM(实验验证低至10 aM)的估计检测极限。
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引用次数: 0
Robust and reusable iridium oxide-modified FTO electrodes for long-term organ-on-a-chip monitoring. 稳健且可重复使用的氧化铱修饰FTO电极,用于长期器官芯片监测。
IF 11.8 1区 生物学 Q1 BIOPHYSICS Pub Date : 2026-11-01 Epub Date: 2026-07-02 DOI: 10.1016/j.bios.2026.118982
Kaige Chen, Fan Zhuo, Changling Lv, Zeyu Chen, Xiang Chen, Han Shan

Real-time monitoring in organ-on-a-chip (OoC) systems is critical for capturing dynamic drug responses, yet standard gold (Au) electrodes utilized in electrical cell-substrate impedance sensing (ECIS) suffer from opacity, high cost, and poor reusability. Here, we report a transparent, robust, and reusable sensing interface based on iridium oxide-modified fluorine-doped tin oxide (IrOx@FTO). By electrodepositing nanostructured IrOx onto FTO, we exploited its pseudocapacitive properties to significantly improve interfacial properties, enhancing sensitivity while preserving optical clarity. We integrated these electrodes into a 128-channel high-throughput platform to monitor HaCaT keratinocytes. The system successfully resolved acute surfactant-induced barrier disruption and differentiated dose-dependent cytotoxic responses to doxorubicin (DOX) with higher precision than bare FTO. Crucially, cycling tests involving repeated culture and cleaning revealed that IrOx@FTO maintains exceptional baseline stability, significantly outperforming gold electrodes which exhibited severe degradation and delamination. This work establishes a scalable, optically compatible, and cost-effective strategy for long-term, multi-modal monitoring in advanced microphysiological systems.

器官芯片(OoC)系统的实时监测对于捕获动态药物反应至关重要,但用于电池-衬底阻抗传感(ECIS)的标准金(Au)电极存在不透明、成本高和可重用性差的问题。在这里,我们报告了一种基于氧化铱修饰的氟掺杂氧化锡的透明、健壮和可重复使用的传感接口(IrOx@FTO)。通过在FTO上电沉积纳米结构IrOx,我们利用其赝电容特性显著改善了界面特性,提高了灵敏度,同时保持了光学清晰度。我们将这些电极集成到128通道高通量平台中,以监测HaCaT角化细胞。该系统成功地解决了表面活性剂诱导的急性屏障破坏,并区分了对阿霉素(DOX)的剂量依赖性细胞毒性反应,其精度高于裸FTO。至关重要的是,涉及重复培养和清洗的循环测试表明,IrOx@FTO保持了卓越的基线稳定性,显著优于表现出严重降解和分层的金电极。这项工作为先进微生理系统的长期、多模态监测建立了一种可扩展、光学兼容且具有成本效益的策略。
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引用次数: 0
Corrigendum to "Fully-printed microneedles meet plants: a pathway towards easy-to-use NFC monitoring of total ionic conductivity in precision agriculture" [Biosens. Bioelectron. 306 (2026) 118667]. “完全打印的微针与植物相遇:在精准农业中实现易于使用的近距离通信(NFC)监测总离子电导率的途径”[Biosens]的勘误表。生物电子学学报,2016(5):387 - 398。
IF 11.8 1区 生物学 Q1 BIOPHYSICS Pub Date : 2026-11-01 Epub Date: 2026-06-04 DOI: 10.1016/j.bios.2026.118865
Dominik Baraniecki, Giulio Rosati, Amelia Miarka, Jakub Krzeminski, Carme Martínez-Domingo, Malgorzata Jakubowska, Eloi Ramon, Arben Merkoçi
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引用次数: 0
Reliable biomarker monitoring at microneedle aptamer biosensors using a dual-frequency ratiometric approach: Overcoming signal drifts. 可靠的生物标志物监测微针适体生物传感器使用双频比率法:克服信号漂移。
IF 11.8 1区 生物学 Q1 BIOPHYSICS Pub Date : 2026-11-01 Epub Date: 2026-07-03 DOI: 10.1016/j.bios.2026.118989
Gyeongho Kim, Ponnusamy Nandhakumar, Maria Reynoso, Qinyu Yu, Muhammad Inam Khan, Barak Sabbagh, Ga-Eun Kim, Beatrice Acot, Rhea Park, Stacey Surace, Joseph Wang

Electrochemical aptamer-based (E-AB) microneedle (MN) sensors offer a promising route for continuous monitoring of endogenous biomarkers. However, long-term operation is often limited by signal attenuation arising from surface biofouling, aptamer detachment, and redox label degradation. Here, we investigated the origin of signal drift by monitoring changes in the peak current (IP) of the redox label during prolonged square-wave voltammetry (SWV) operation in PBS, serum, and artificial ISF. To address this drift, we introduced a dual-frequency ratiometric approach based on the ratio between the IP measured at frequencies showing maximum (Fmax) and minimum (Fmin) responses. Prolonged SWV measurements in PBS, where biofouling is negligible, showed a gradual decrease in IP, and cyclic voltammetry measurements obtained before and after SWV operation confirmed a decrease in the MB faradaic current. These results suggest that SWV-induced aptamer detachment and/or MB degradation are major source of intrinsic signal drift. In serum and artificial ISF, this drift was further exacerbated by biofouling, resulting in an approximately 30% decrease in IP measured at Fmax and Fmin (IFmax and IFmin) over 48 h. In contrast, the ratiometric signal (IR = IFmax/IFmin), remained stable because similar signal drift in IFmax and IFmin was effectively compensated. In addition, the ratiometric approach reduced sensor-to-sensor variation, enabling reliable continuous cortisol monitoring with quantified concentrations that closely matched the applied levels, whereas IFmax-based quantification resulted in large deviations. These findings establish dual-frequency ratiometric E-AB MN sensors as a reliable platform for stable and accurate continuous biomarker monitoring in complex biological fluids.

基于电化学适配体(E-AB)的微针(MN)传感器为内源性生物标志物的连续监测提供了一条很有前途的途径。然而,由于表面生物污垢、适体分离和氧化还原标签降解引起的信号衰减,长期操作往往受到限制。在这里,我们通过监测PBS、血清和人工ISF在长时间方波伏安法(SWV)操作期间氧化还原标签的峰值电流(IP)的变化来研究信号漂移的起源。为了解决这种漂移,我们引入了一种双频比率法,该方法基于在显示最大(Fmax)和最小(Fmin)响应的频率下测量的IP之间的比率。在PBS中进行长时间的SWV测量,其中生物污垢可以忽略不计,显示出IP逐渐降低,并且在SWV操作前后进行的循环伏安测量证实了MB法拉第电流的降低。这些结果表明,swv诱导的适体分离和/或MB降解是本征信号漂移的主要来源。在血清和人工ISF中,生物污垢进一步加剧了这种漂移,导致在48 h内Fmax和Fmin (IFmax和IFmin)测量的IP下降约30%。相比之下,比值信号(IR = IFmax/IFmin)保持稳定,因为IFmax和IFmin中类似的信号漂移得到了有效补偿。此外,比率法减少了传感器间的差异,实现了与应用水平密切匹配的量化浓度的可靠连续皮质醇监测,而基于ifmax的量化导致了很大的偏差。这些发现建立了双频比率E-AB MN传感器作为稳定、准确、连续监测复杂生物流体中生物标志物的可靠平台。
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引用次数: 0
One-Tube RPA-CRISPR-Cas13a assay with rational design for single-molecule detection of waterborne viruses in drinking water treatment. 合理设计的单管rna - crispr - cas13a方法用于饮用水处理中水传播病毒的单分子检测
IF 11.8 1区 生物学 Q1 BIOPHYSICS Pub Date : 2026-11-01 Epub Date: 2026-07-02 DOI: 10.1016/j.bios.2026.118983
Fan Wang, Changhua He, Yingzi Lin, Xiaohong Zhou

The global rise in waterborne viral infections has created an urgent need for portable, highly efficient environmental virus detection technologies. CRISPR-based nucleic acid detection coupled with isothermal amplification (e.g., Recombinase Polymerase Amplification, RPA) shows great promise for field applications. However, most reported designs fail to achieve the single-molecule sensitivity, which significantly limits their practical applications. To bridge the gap, we proposed a rational design strategy for the RPA primer and the CRISPR-Cas13a crRNA, suggesting that sensitivity can be enhanced by simplifying the secondary structure of the crRNA spacer region. Subsequently, we established a portable, one-tube CRISPR-Cas13a bioassay to detect two major waterborne viruses, achieving ultrasensitive detection limits of 5/8 aM for norovirus and 2/3 aM for rotavirus within 40 min. Thereafter, seasonal sampling across different treatment stages of a drinking water treatment plant was conducted, and water samples were analyzed using the one-tube CRISPR-Cas13a bioassay in comparison with qPCR and dPCR, revealing a positive detection rate of 15.79% (6/38) for the one-tube CRISPR-Cas13a bioassay, 18.42% (7/38) for qPCR, and 15.79% (6/38) for dPCR. The assay's modular design allows for broad applicability to other pathogens by simply modifying the target nucleic acid sequence, offering high sensitivity and specificity. This innovation paves the way for deployable point-of-care testing and large-scale spatiotemporal virus monitoring.

全球水传播病毒感染的增加,迫切需要便携式、高效的环境病毒检测技术。基于crispr的核酸检测与等温扩增(如重组酶聚合酶扩增,RPA)相结合,在现场应用中具有很大的前景。然而,大多数报道的设计未能达到单分子灵敏度,这极大地限制了它们的实际应用。为了弥补这一差距,我们提出了RPA引物和CRISPR-Cas13a crRNA的合理设计策略,表明可以通过简化crRNA间隔区的二级结构来提高灵敏度。随后,我们建立了一种便携式单管CRISPR-Cas13a生物检测方法,检测两种主要的水媒病毒,在40 min内,对诺如病毒和轮状病毒的超灵敏检测限分别为5/8 aM和2/3 aM。随后,对某饮用水处理厂的不同处理阶段进行季节性采样,采用单管CRISPR-Cas13a生物测定法对水样进行分析,并与qPCR和dPCR进行比较,单管CRISPR-Cas13a生物测定法的阳性检出率为15.79% (6/38),qPCR为18.42% (7/38),dPCR为15.79%(6/38)。该检测的模块化设计允许广泛适用于其他病原体,只需修改目标核酸序列,提供高灵敏度和特异性。这一创新为可部署的即时检测和大规模时空病毒监测铺平了道路。
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引用次数: 0
A real-time 5-hydroxytryptamine monitoring system applicable both in vitro and in vivo. 一种适用于体内体外的5-羟色胺实时监测系统。
IF 11.8 1区 生物学 Q1 BIOPHYSICS Pub Date : 2026-11-01 Epub Date: 2026-07-02 DOI: 10.1016/j.bios.2026.118954
Liu-Hong Yang, Shi-Chun Ren, Jia-Feng Wang, Ge Dai, Feng-Feng Mo

This research addresses the challenge of real-time monitoring of the neurotransmitter serotonin (5-HT), a key chemical messenger in the brain whose dynamics are important for understanding neurological disorders. While electrochemical methods are promising for such real-time detection, existing approaches face limitations in maintaining stable performance in physiological settings and achieving precise spatiotemporal measurements. To overcome these barriers, two electrochemical systems were developed: one for monitoring 5-HT secretion from cells and another for tracking 5-HT in the mouse brain. By enhancing electrodes with specific nanocomposites to improve sensitivity and selectivity, the cell system successfully analyzed real-time 5-HT secretion dynamics from rat insulinoma cells with performance comparable to standard methods. The neural interface system effectively tracked 5-HT fluctuations across multiple brain regions in living mice and detected changes induced by external interventions. These platforms enable real-time tracking of 5-HT dynamics both in cells and in living organisms, demonstrating significant potential for studies requiring real-time neurotransmitter monitoring.

这项研究解决了实时监测神经递质5-羟色胺(5-HT)的挑战,5-羟色胺是大脑中关键的化学信使,其动力学对理解神经系统疾病很重要。虽然电化学方法有望实现这种实时检测,但现有方法在保持生理环境下的稳定性能和实现精确的时空测量方面存在局限性。为了克服这些障碍,研究人员开发了两种电化学系统:一种用于监测细胞分泌的5-羟色胺,另一种用于追踪小鼠大脑中的5-羟色胺。通过使用特定纳米复合材料增强电极以提高灵敏度和选择性,该细胞系统成功分析了大鼠胰岛素瘤细胞的实时5-羟色胺分泌动态,其性能与标准方法相当。神经接口系统有效地追踪了活体小鼠多个脑区的5-羟色胺波动,并检测了外部干预引起的变化。这些平台能够实时跟踪细胞和生物体中的5-羟色胺动态,显示出需要实时神经递质监测的研究的巨大潜力。
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引用次数: 0
Propylene carbonate-PVDF-HFP/MXene-based self-powered biosensor for auxiliary detection of salivary exosomal miRNA-155 in pediatric asthma. 基于碳酸丙烯酯- pvdf - hfp / mxene的自供电生物传感器辅助检测儿童哮喘唾液外泌体miRNA-155
IF 11.8 1区 生物学 Q1 BIOPHYSICS Pub Date : 2026-11-01 Epub Date: 2026-07-05 DOI: 10.1016/j.bios.2026.118984
Tiantian Sun, Fangyan Ji, Zhenrun Li, Qiang Ma

This study developed a novel integrated self-powered biosensor for non-invasive auxiliary detection of pediatric asthma-associated miRNA-155. A flexible self-supporting electrode based on a propylene carbonate-PVDF-HFP/MXene composite was developed and implemented in an enzymatic biofuel cell self-powered sensing system. PVDF-HFP displayed excellent chemical stability and strong film-forming ability and MXene worked as electroactive materials in the self-supporting electrode substrate. The anode of the self-powered biosensor was prepared with Au NPs-decorated cobalt-nickel layered double hydroxide, which effectively enhanced electron transfer between enzymes and electrode to improve power output. Meanwhile, the cathode was designed based on [Ru(NH3)6]3+ as efficient electron acceptors. As a result, the glucose oxidation reaction at the anode and the reduction of [Ru(NH3)6]3+ at the cathode generated a measurable open-circuit voltage (EOCV), which was real-time recorded through smartphone integration. The development of self-powered biosensor overcame the limitations of the low power output, functional layer detachment, and active site deactivation. The established integrated self-powered biosensing system successfully quantified salivary exosomal miRNA-155 across a broad concentration range (0.001-10,000 pM) with a detection limit of 0.21 fM. This work constructed a robust and portable platform suitable for non-invasive auxiliary detection of pediatric asthma, demonstrating promising applications in liquid biopsy.

本研究开发了一种新型集成自供电生物传感器,用于无创辅助检测儿童哮喘相关miRNA-155。开发了一种基于碳酸丙烯酯- pvdf - hfp /MXene复合材料的柔性自支撑电极,并将其应用于酶生物燃料电池自供电传感系统中。PVDF-HFP表现出优异的化学稳定性和较强的成膜能力,MXene作为电活性材料作为自支撑电极衬底。采用金纳米粒子修饰钴镍层状双氢氧化物制备自供电生物传感器的阳极,有效增强了酶与电极之间的电子传递,提高了功率输出。同时,设计了以[Ru(NH3)6]3+为高效电子受体的阴极。结果,阳极的葡萄糖氧化反应和阴极的[Ru(NH3)6]3+的还原产生了可测量的开路电压(EOCV),通过智能手机集成实时记录。自供电生物传感器的发展克服了低功率输出、功能层脱离和活性位点失活的限制。建立的集成自供电生物传感系统成功地定量唾液外泌体miRNA-155在很宽的浓度范围内(0.001-10,000 pM),检测限为0.21 fM。本工作构建了一个强大的便携式平台,适用于儿童哮喘的无创辅助检测,在液体活检中具有广阔的应用前景。
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引用次数: 0
Interfacial structure-modified nanozyme drives single-receptor-single-reaction-unit multichannel sensor array for pesticide discrimination. 界面结构修饰的纳米酶驱动单受体-单反应单元多通道传感器阵列用于农药识别。
IF 11.8 1区 生物学 Q1 BIOPHYSICS Pub Date : 2026-11-01 Epub Date: 2026-07-04 DOI: 10.1016/j.bios.2026.118993
Jin Liu, Jiyue Zhao, Hongxiang Chen, Yu Zhou, Yifei Chen, Chengzhou Zhu, Hongye Yan

Sensor arrays perform well in distinguishing subtle changes induced by structurally similar multi-target analytes in complex systems. However, the construction of most sensor arrays requires multiple receptors and sensing units, increasing detection complexity. Here, we developed Co3O4@Bi nanozymes with a Co-O-Bi interfacial structure, which is devoted to the construction of a single-receptor-single-reaction-unit multichannel sensor array. The Co-O-Bi interfaces facilitate electron transfer from Co to O and then to Bi and weaken the oxygen adsorption capacity. Compared to the Co3O4 nanozymes with repetitive metal Co-O-Co structural units, the resultant Co3O4@Bi nanozymes show a 3.6-fold enhancement in peroxidase-like activity, of which the oxidase-like performance exhibits a decline. As a result, the catalytic activity and selectivity of the Co3O4@Bi nanozymes were improved by introducing Co-O-Bi interfacial structures. Taking Co3O4@Bi as a single receptor and a typical chromogenic reaction as the single reaction unit, the sensor array was established and displayed three distinct characteristic peaks. Based on the different inhibition effects of various pesticides on the activity of Co3O4@Bi nanozyme, the characteristic peaks act as multiple signal channels, enabling the 100% discrimination of five pesticides during the combined use of multiple pesticides. In addition, the colorimetric sensor array can accurately identify the target pesticides with good selectivity and anti-interference capability. This work not only offers a new feasible strategy for the design of nanozymes with an interfacial structure but also addresses the reliance of traditional sensor arrays on multiple receptors and units.

传感器阵列可以很好地识别复杂系统中结构相似的多目标分析物引起的细微变化。然而,大多数传感器阵列的构建需要多个受体和传感单元,增加了检测的复杂性。在这里,我们开发了具有Co-O-Bi界面结构的Co3O4@Bi纳米酶,用于构建单受体-单反应单元多通道传感器阵列。Co-O-Bi界面有利于电子从Co到O再到Bi的转移,并削弱了氧吸附能力。与具有重复金属Co-O-Co结构单元的Co3O4纳米酶相比,所得Co3O4@Bi纳米酶的类过氧化物酶活性提高3.6倍,类氧化酶性能下降。结果表明,引入Co-O-Bi界面结构可提高Co3O4@Bi纳米酶的催化活性和选择性。以Co3O4@Bi为单一受体,以典型显色反应为单一反应单元,建立传感器阵列,并显示出三个明显的特征峰。基于不同农药对Co3O4@Bi纳米酶活性的不同抑制作用,特征峰作为多个信号通道,实现了多种农药联合使用时对5种农药的100%识别。此外,该比色传感器阵列能够准确识别目标农药,具有良好的选择性和抗干扰能力。这项工作不仅为设计具有界面结构的纳米酶提供了一种新的可行策略,而且解决了传统传感器阵列对多个受体和单元的依赖。
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引用次数: 0
Discreet wearable biopotential interfaces based on water-soluble biodegradable thermoplastics. 基于水溶性可生物降解热塑性塑料的可穿戴生物电位界面。
IF 11.8 1区 生物学 Q1 BIOPHYSICS Pub Date : 2026-10-15 DOI: 10.1016/j.bios.2026.119338
Shaghayegh Mesforush, Narges Pourjafarian, Yichen Wan, Tara Arjomandbigdeli, Ruobing Bai, Canek Fuentes-Hernandez

Non-invasive wearable biopotential interfaces (WBIs), devices that enable recording of electrical signals from the body's surface, depend on electrodes that form a low impedance interface with the skin. Existing electrodes are often bulky, uncomfortable, slow to stabilize, and socially unacceptable due to their conspicuous appearance, or require complex conductive materials and fabrication processes. Here, we show that thin films of poly(vinyl alcohol) (PVA), a low-cost, transparent, electronically insulating biodegradable thermoplastic, can be used as a discreet, high-performance electrode when exposed to a water-based ionic gel. Water plasticizes PVA and makes it mechanically skin-like. Plasticized PVA also becomes ionically conductive to serve as an electrode that conforms to the skin to enable efficient ion transport at the skin's interface upon application, yielding 13× lower resistance than when the same gel is used with a plastic backing. This eliminates the stabilization delay of conventional wet or semi-wet electrodes, leading to a similar level of performance when compared to benchmark Ag/AgCl semi-wet electrodes for electrocardiography and electromyography, enabling the implementation of a wireless gesture recognition interface. Signal quality is maintained or improved over multi-hour recordings, and artificial sweat can replace the ionic gel to yield a comparable skin-electrode impedance. These results establish biodegradable thermoplastics as a scalable path towards socially acceptable, high-performance WBIs.

非侵入式可穿戴生物电位接口(wbi)是一种能够记录体表电信号的设备,它依赖于与皮肤形成低阻抗接口的电极。现有的电极通常体积庞大,不舒服,稳定缓慢,并且由于其显眼的外观而不被社会接受,或者需要复杂的导电材料和制造工艺。在这里,我们展示了聚乙烯醇(PVA)薄膜,一种低成本、透明、电子绝缘、可生物降解的热塑性塑料,当暴露在水基离子凝胶中时,可以用作谨慎的高性能电极。水使PVA塑化,使其机械上像皮肤一样。塑化的PVA还具有离子导电性,可以作为符合皮肤的电极,在应用时在皮肤界面上实现有效的离子传输,其电阻比使用塑料衬底时低13倍。这消除了传统湿电极或半湿电极的稳定延迟,与用于心电图和肌电图的基准Ag/AgCl半湿电极相比,具有相似的性能水平,从而实现无线手势识别界面。信号质量在数小时的记录中保持或改善,人工汗液可以代替离子凝胶产生类似的皮肤电极阻抗。这些结果确立了可生物降解热塑性塑料作为社会可接受的高性能wbi的可扩展路径。
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引用次数: 0
Curvature-Engineered Carbon Supports Dramatically Boost Electrocatalytic Activity of Ni Single Atoms for Glucose Sensing 曲率工程碳支持显著提高镍单原子的电催化活性,用于葡萄糖传感。
IF 11.8 1区 生物学 Q1 BIOPHYSICS Pub Date : 2026-10-14 DOI: 10.1016/j.bios.2026.119347
Ziyin Yang, Luyao Wang, Yaqi Kong, Chengcheng Qi
Although the local microenvironment exerts a profound influence on the catalytic activity of single-atom nanozymes, the role of support curvature has remained poorly understood. Herein, we construct a high-curvature onion-like carbon support via a template-free process, in which Ni nanoparticles act simultaneously as metal source, hard template, and carbon reconstructing agent. This curved architecture not only anchors Ni single atoms but also modulates their electronic structure, as confirmed by HAADF-STEM, X-ray absorption fine structure, and TEM, which reveal isolated bright spots, Ni–N coordination, and hollow curved shells, respectively. Experimental and theoretical analyses reveal that the curvature reduces the Ni valence state and upshifts the d-band center, thereby optimizing glucose adsorption and accelerating dehydrogenation kinetics. The curved support substantially enhances the catalytic activity of Ni single atoms toward glucose oxidation compared with planar carbon, achieving a sensitivity of 1739.43 μA·mM-1·cm-2, a detection limit of 0.6 μM, and excellent selectivity. Overall, our findings establish a clear structure–activity relationship and highlight curvature engineering as a powerful strategy for designing highly sensitive electrochemical sensors, opening new possibilities for microenvironmental tuning in practical bioanalysis.
虽然局部微环境对单原子纳米酶的催化活性有深远的影响,但对支撑曲率的作用仍知之甚少。在此,我们通过无模板工艺构建了高曲率洋葱状碳载体,其中Ni纳米颗粒同时作为金属源、硬模板和碳重构剂。HAADF-STEM、x射线吸收精细结构和TEM证实,这种弯曲结构不仅锚定了Ni单原子,而且调节了它们的电子结构,分别显示出孤立的亮点、Ni- n配位和空心弯曲壳层。实验和理论分析表明,曲率降低了Ni价态,使d带中心上移,从而优化了葡萄糖的吸附,加速了脱氢动力学。与平面碳相比,弯曲载体显著提高了Ni单原子对葡萄糖氧化的催化活性,灵敏度为1739.43 μA mM-1·cm-2,检出限为0.6 μM,选择性良好。总的来说,我们的研究结果建立了明确的结构-活性关系,并突出了曲率工程作为设计高灵敏度电化学传感器的有力策略,为实际生物分析中的微环境调谐开辟了新的可能性。
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引用次数: 0
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Biosensors and Bioelectronics
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