Pub Date : 2024-10-22DOI: 10.1021/acssensors.4c02060
Sebastian Freko, Marta Nikić, Dirk Mayer, Lennart J K Weiß, Friedrich C Simmel, Bernhard Wolfrum
The rapid and reliable detection and quantification of nucleic acids is crucial for various applications, including infectious disease and cancer diagnostics. While conventional methods, such as the quantitative polymerase chain reaction are widely used, they are limited to the laboratory environment due to their complexity and the requirement for sophisticated equipment. In this study, we present a novel amplification-free digital sensing strategy by combining the collateral cleavage activity of the Cas12a enzyme with single-impact electrochemistry. In doing so, we modified silver nanoparticles using a straightforward temperature-assisted cofunctionalization process to subsequently detect the collision events of particles released by the activated Cas12a as distinct current spikes on a microelectrode array. The functionalization resulted in stable DNA-AgNP conjugates, making them suitable for numerous biosensor applications. Thus, our study demonstrates the potential of clustered regularly interspaced short palindromic repeats-based diagnostics combined with impact-based digital sensing for a rapid and amplification-free quantification of nucleic acids.
{"title":"Digital Clustered Regularly Interspaced Short Palindromic Repeats-Powered Biosensor Concept without Target Amplification Using Single-Impact Electrochemistry.","authors":"Sebastian Freko, Marta Nikić, Dirk Mayer, Lennart J K Weiß, Friedrich C Simmel, Bernhard Wolfrum","doi":"10.1021/acssensors.4c02060","DOIUrl":"https://doi.org/10.1021/acssensors.4c02060","url":null,"abstract":"<p><p>The rapid and reliable detection and quantification of nucleic acids is crucial for various applications, including infectious disease and cancer diagnostics. While conventional methods, such as the quantitative polymerase chain reaction are widely used, they are limited to the laboratory environment due to their complexity and the requirement for sophisticated equipment. In this study, we present a novel amplification-free digital sensing strategy by combining the collateral cleavage activity of the Cas12a enzyme with single-impact electrochemistry. In doing so, we modified silver nanoparticles using a straightforward temperature-assisted cofunctionalization process to subsequently detect the collision events of particles released by the activated Cas12a as distinct current spikes on a microelectrode array. The functionalization resulted in stable DNA-AgNP conjugates, making them suitable for numerous biosensor applications. Thus, our study demonstrates the potential of clustered regularly interspaced short palindromic repeats-based diagnostics combined with impact-based digital sensing for a rapid and amplification-free quantification of nucleic acids.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":null,"pages":null},"PeriodicalIF":8.2,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142453359","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Combining wearable sensors with modern technologies such as internet of things and big data to monitor or intervene in obesity-induced chronic diseases, such as obstructive sleep apnea, type II diabetes, cardiovascular diseases, and Alzheimer's disease, is of great significance to the self-health management of human beings. This study designed a loofah-conducting graphite four friction layer enhanced triboelectric nanogenerator (LG-TENG) and developed a health management system for human motion recognition and early warning of sleep breathing abnormalities. By uniformly spraying and depositing conductive graphite on the surface of the loofah and the elastic film cross-interlocking bending structure design, the signal strength of the LG-TENG has been improved by 390%. The stable output signal is still maintained after 1500 s of continuous operation at a frequency of 2 Hz. LG-TENG can realize accurate motion analysis by muscle contraction state. Combining different deep learning models resulted in 98.1% accuracy in recognizing seven categories of displacement speeds for an individual and 96.46% accuracy in recognizing seven categories of displacement speeds for three individuals. In addition, the sleep breathing monitoring early warning system was developed by integrating Bluetooth wireless transmission and upper computer analysis technology. This system aims to analyze and provide real-time warnings for sleep-breathing abnormalities. This research promotes an innovation of TENG technology based on the advantages of natural materials, recyclability and low cost. It offers new ideas for self-health management and scientific exercise for obese people, showing a broad application prospect.
{"title":"Self-Powered, Flexible, Wireless and Intelligent Human Health Management System Based on Natural Recyclable Materials.","authors":"Dongsheng Liu, Yuzhang Wen, Zhenning Xie, Mengqi Zhang, Yunlu Wang, Qingyang Feng, Zihang Cheng, Zhuo Lu, Yupeng Mao, Haidong Yang","doi":"10.1021/acssensors.4c02186","DOIUrl":"https://doi.org/10.1021/acssensors.4c02186","url":null,"abstract":"<p><p>Combining wearable sensors with modern technologies such as internet of things and big data to monitor or intervene in obesity-induced chronic diseases, such as obstructive sleep apnea, type II diabetes, cardiovascular diseases, and Alzheimer's disease, is of great significance to the self-health management of human beings. This study designed a loofah-conducting graphite four friction layer enhanced triboelectric nanogenerator (LG-TENG) and developed a health management system for human motion recognition and early warning of sleep breathing abnormalities. By uniformly spraying and depositing conductive graphite on the surface of the loofah and the elastic film cross-interlocking bending structure design, the signal strength of the LG-TENG has been improved by 390%. The stable output signal is still maintained after 1500 s of continuous operation at a frequency of 2 Hz. LG-TENG can realize accurate motion analysis by muscle contraction state. Combining different deep learning models resulted in 98.1% accuracy in recognizing seven categories of displacement speeds for an individual and 96.46% accuracy in recognizing seven categories of displacement speeds for three individuals. In addition, the sleep breathing monitoring early warning system was developed by integrating Bluetooth wireless transmission and upper computer analysis technology. This system aims to analyze and provide real-time warnings for sleep-breathing abnormalities. This research promotes an innovation of TENG technology based on the advantages of natural materials, recyclability and low cost. It offers new ideas for self-health management and scientific exercise for obese people, showing a broad application prospect.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":null,"pages":null},"PeriodicalIF":8.2,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142453360","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-21DOI: 10.1021/acssensors.4c01097
Xingyu Ma, Da Chen, Quanlin Qu, Shengmei Liao, Menghan Wang, Hanning Wang, Ziyue Chen, Tong Zhang, Fei Wang, Yijian Liu
An omnidirectional stretchable strain sensor with high resolution is a critical component for motion detection and human–machine interaction. It is the current dominant solution to integrate several consistent units into the omnidirectional sensor based on a certain geometric structure. However, the excessive similarity in orientation characteristics among sensing units restricts orientation recognition due to their closely matched strain sensitivity. In this study, based on strain partition modulation (SPM), a sensitivity anisotropic amplification strategy is proposed for resistive strain sensors. The stress distribution of a sensitive conductive network is modulated by structural parameters of the customized periodic hole array introduced underneath the elastomer substrate. Meanwhile, the strain isolation structures are designed on both sides of the sensing unit for stress interference immune. The optimized sensors exhibit excellent sensitivity (19 for 0–80%; 109 for 80%–140%; 368 for 140%–200%), with nearly a 7-fold improvement in the 140%–200% interval compared to bare elastomer sensors. More importantly, a sensing array composed of multiple units with different hole configurations can highlight orientation characteristics with amplitude difference between channels reaching up to 29 times. For the 48-class strain-orientation decoupling task, the recognition rate of the sensitivity-differentiated layout sensor with the lightweight deep learning network is as high as 96.01%, superior to that of 85.7% for the sensitivity-consistent layout. Furthermore, the application of the sensor to the fitness field demonstrates an accurate recognition of the wrist flexion direction (98.4%) and spinal bending angle (83.4%). Looking forward, this methodology provides unique prospects for broader applications such as tactile sensors, soft robotics, and health monitoring technologies.
{"title":"Directional Characteristic Enhancement of an Omnidirectional Detection Sensor Enabled by Strain Partitioning Effects in a Periodic Composite Hole Substrate","authors":"Xingyu Ma, Da Chen, Quanlin Qu, Shengmei Liao, Menghan Wang, Hanning Wang, Ziyue Chen, Tong Zhang, Fei Wang, Yijian Liu","doi":"10.1021/acssensors.4c01097","DOIUrl":"https://doi.org/10.1021/acssensors.4c01097","url":null,"abstract":"An omnidirectional stretchable strain sensor with high resolution is a critical component for motion detection and human–machine interaction. It is the current dominant solution to integrate several consistent units into the omnidirectional sensor based on a certain geometric structure. However, the excessive similarity in orientation characteristics among sensing units restricts orientation recognition due to their closely matched strain sensitivity. In this study, based on strain partition modulation (SPM), a sensitivity anisotropic amplification strategy is proposed for resistive strain sensors. The stress distribution of a sensitive conductive network is modulated by structural parameters of the customized periodic hole array introduced underneath the elastomer substrate. Meanwhile, the strain isolation structures are designed on both sides of the sensing unit for stress interference immune. The optimized sensors exhibit excellent sensitivity (19 for 0–80%; 109 for 80%–140%; 368 for 140%–200%), with nearly a 7-fold improvement in the 140%–200% interval compared to bare elastomer sensors. More importantly, a sensing array composed of multiple units with different hole configurations can highlight orientation characteristics with amplitude difference between channels reaching up to 29 times. For the 48-class strain-orientation decoupling task, the recognition rate of the sensitivity-differentiated layout sensor with the lightweight deep learning network is as high as 96.01%, superior to that of 85.7% for the sensitivity-consistent layout. Furthermore, the application of the sensor to the fitness field demonstrates an accurate recognition of the wrist flexion direction (98.4%) and spinal bending angle (83.4%). Looking forward, this methodology provides unique prospects for broader applications such as tactile sensors, soft robotics, and health monitoring technologies.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":null,"pages":null},"PeriodicalIF":8.9,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452415","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-18DOI: 10.1021/acssensors.4c02585
Er-Chi Zhou, Hang Fu, Hao-Ze Wang, Ya-Jun Yang, Xing-Hua Zhang
S-DNA is a double-stranded DNA that forms under tensions of >65 pN. Here, we report that S-DNA resists the cleavage of Cas12a and the restriction endonuclease SmaI. Taking advantage of this resistance, in magnetic tweezer experiments, we developed an assay to convert multiple-DNA-tethered beads into single-DNA-tethered beads and remove the only-one-end-tethered DNA molecule by cleaving the DNA that does not transition to S-DNA at about 80 pN. When multiple DNA molecules are tethered to a single bead, they share the tension, exist in the B-form, and allow the cleavage. Only-one-end-tethered DNA molecules, free of tension, are also cleaved. In versatile types of experiments, we proved the broad applications of this assay: measuring the correct DNA elasticity and DNA condensation dynamics by avoiding the false results due to interference of only-one-end-tethered DNA molecules and quantifying the accurate cleavage rates of Cas12a and the restriction endonucleases by eliminating the error caused by multiple-DNA-tethered beads. This convenient assay ensures correct and accurate results in high-throughput DNA stretching experiments.
S-DNA 是一种在 65 pN 张力下形成的双链 DNA。在这里，我们报告了 S-DNA 能抵抗 Cas12a 和限制性内切酶 SmaI 的裂解。利用这种抗性，在磁镊实验中，我们开发了一种检测方法，将多DNA系留珠转化为单DNA系留珠，并通过在约80 pN时裂解未转化为S-DNA的DNA来移除仅一端系留的DNA分子。当多个 DNA 分子系在一个珠子上时，它们共享张力，以 B-形式存在，并允许裂解。只有一端系在一起的 DNA 分子在没有张力的情况下也会被裂解。在多种类型的实验中，我们证明了这种检测方法的广泛应用：通过避免仅一端系链 DNA 分子的干扰而得出错误结果，从而测量正确的 DNA 弹性和 DNA 凝聚动力学；通过消除多 DNA 系链珠造成的误差而量化 Cas12a 和限制性内切酶的准确裂解率。这种便捷的检测方法可确保在高通量 DNA 拉伸实验中得到正确、准确的结果。
{"title":"Converting Multiple- to Single-DNA-Tethered Beads and Removing Only-One-End-Tethered DNA in High-Throughput Stretching","authors":"Er-Chi Zhou, Hang Fu, Hao-Ze Wang, Ya-Jun Yang, Xing-Hua Zhang","doi":"10.1021/acssensors.4c02585","DOIUrl":"https://doi.org/10.1021/acssensors.4c02585","url":null,"abstract":"S-DNA is a double-stranded DNA that forms under tensions of >65 pN. Here, we report that S-DNA resists the cleavage of Cas12a and the restriction endonuclease <i>Sma</i>I. Taking advantage of this resistance, in magnetic tweezer experiments, we developed an assay to convert multiple-DNA-tethered beads into single-DNA-tethered beads and remove the only-one-end-tethered DNA molecule by cleaving the DNA that does not transition to S-DNA at about 80 pN. When multiple DNA molecules are tethered to a single bead, they share the tension, exist in the B-form, and allow the cleavage. Only-one-end-tethered DNA molecules, free of tension, are also cleaved. In versatile types of experiments, we proved the broad applications of this assay: measuring the correct DNA elasticity and DNA condensation dynamics by avoiding the false results due to interference of only-one-end-tethered DNA molecules and quantifying the accurate cleavage rates of Cas12a and the restriction endonucleases by eliminating the error caused by multiple-DNA-tethered beads. This convenient assay ensures correct and accurate results in high-throughput DNA stretching experiments.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":null,"pages":null},"PeriodicalIF":8.9,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142449712","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-18DOI: 10.1021/acssensors.4c02251
Xiuyuan Yao, Linyao Wang, Jie Luo, Chuyan Zhang, Yongxin Li
With the continuous development of DNA nanotechnology, DNA walkers have attracted increased attention because of their autonomous and progressive walking along predesigned tracks. Compared with the traditional DNA walkers, the emerged multipedal DNA walkers showed their special charm with sustainable walking capability, higher reaction efficiency, expanded walking region, and improved amplification capability. Consequently, multipedal DNA walkers have developed rapidly and shown potential in biosensing applications. Hence, in this review, we make a comprehensive representation of the engineering strategy of multipedal DNA walkers, which focused on the design of multiple walking strands as well as the construction of tracks and driving forces. Meanwhile, the application of multipedal DNA walkers in biosensors has been thoroughly described according to the type of biosensing signal readout. By illustrating some representative works, we also summarized the merits and challenges of multipedal DNA walker-based biosensors and offered a deep discussion of the latest progress and future.
随着DNA纳米技术的不断发展，DNA步行器因其可沿着预先设计的轨道自主、渐进地行走而受到越来越多的关注。与传统的 DNA 步行器相比，新出现的多级 DNA 步行器显示出其独特的魅力，具有可持续行走能力、更高的反应效率、更大的行走区域和更强的扩增能力。因此，多极 DNA 步行器得到了快速发展，并在生物传感应用中展现出巨大潜力。因此，在这篇综述中，我们全面介绍了多足 DNA 步行器的工程设计策略，主要集中在多条步行链的设计以及轨道和驱动力的构建上。同时，根据生物传感信号读出的类型，全面阐述了多向DNA步行器在生物传感器中的应用。通过展示一些代表性的作品，我们还总结了基于多极DNA步行器的生物传感器的优点和挑战，并对最新进展和未来进行了深入探讨。
{"title":"Multipedal DNA Walker: Engineering Strategy, Biosensing Application and Future Perspectives","authors":"Xiuyuan Yao, Linyao Wang, Jie Luo, Chuyan Zhang, Yongxin Li","doi":"10.1021/acssensors.4c02251","DOIUrl":"https://doi.org/10.1021/acssensors.4c02251","url":null,"abstract":"With the continuous development of DNA nanotechnology, DNA walkers have attracted increased attention because of their autonomous and progressive walking along predesigned tracks. Compared with the traditional DNA walkers, the emerged multipedal DNA walkers showed their special charm with sustainable walking capability, higher reaction efficiency, expanded walking region, and improved amplification capability. Consequently, multipedal DNA walkers have developed rapidly and shown potential in biosensing applications. Hence, in this review, we make a comprehensive representation of the engineering strategy of multipedal DNA walkers, which focused on the design of multiple walking strands as well as the construction of tracks and driving forces. Meanwhile, the application of multipedal DNA walkers in biosensors has been thoroughly described according to the type of biosensing signal readout. By illustrating some representative works, we also summarized the merits and challenges of multipedal DNA walker-based biosensors and offered a deep discussion of the latest progress and future.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":null,"pages":null},"PeriodicalIF":8.9,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142448877","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-18DOI: 10.1021/acssensors.4c01198
Eric R Westphal,Kenneth M Plackowski,Michael J Holzmann,Alexandra M Outka,Dongchang Chen,Koushik Ghosh,John K Grey
Carbon dots have attracted widespread interest for sensing applications based on their low cost, ease of synthesis, and robust optical properties. We investigate structure-function evolution on multiemitter fluorescence patterns for model carbon-nitride dots (CNDs) and their implications on trace-level sensing. Hydrothermally synthesized CNDs with different reaction times were used to determine how specific functionalities and their corresponding fluorescence signatures respond upon the addition of trace-level analytes. Archetype explosives molecules were chosen as a testbed due to similarities in substituent groups or inductive properties (i.e., electron withdrawing), and solution-based assays were performed using ratiometric fluorescence excitation-emission mapping (EEM). Analyte-specific quenching and enhancement responses were observed in EEM landscapes that varied with the CND reaction time. We then used self-organizing map models to examine EEM feature clustering with specific analytes. The results reveal that interactions between carbon-nitride frameworks and molecular-like species dictate response characteristics that may be harnessed to tailor sensor development for specific applications.
{"title":"Influence of Carbon-Nitride Dot-Emitting Species and Evolution on Fluorescence-Based Sensing and Differentiation.","authors":"Eric R Westphal,Kenneth M Plackowski,Michael J Holzmann,Alexandra M Outka,Dongchang Chen,Koushik Ghosh,John K Grey","doi":"10.1021/acssensors.4c01198","DOIUrl":"https://doi.org/10.1021/acssensors.4c01198","url":null,"abstract":"Carbon dots have attracted widespread interest for sensing applications based on their low cost, ease of synthesis, and robust optical properties. We investigate structure-function evolution on multiemitter fluorescence patterns for model carbon-nitride dots (CNDs) and their implications on trace-level sensing. Hydrothermally synthesized CNDs with different reaction times were used to determine how specific functionalities and their corresponding fluorescence signatures respond upon the addition of trace-level analytes. Archetype explosives molecules were chosen as a testbed due to similarities in substituent groups or inductive properties (i.e., electron withdrawing), and solution-based assays were performed using ratiometric fluorescence excitation-emission mapping (EEM). Analyte-specific quenching and enhancement responses were observed in EEM landscapes that varied with the CND reaction time. We then used self-organizing map models to examine EEM feature clustering with specific analytes. The results reveal that interactions between carbon-nitride frameworks and molecular-like species dictate response characteristics that may be harnessed to tailor sensor development for specific applications.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":null,"pages":null},"PeriodicalIF":8.9,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142449246","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-17DOI: 10.1021/acssensors.4c02425
Yang Li, Rui Han, Baoping Zhu, Wenqing Wang, Zhen Song, Xiliang Luo
Developing antifouling biosensors capable of performing robustly in complex human body fluids is crucial for biomarker diagnosis and health monitoring. Herein, an antifouling and highly sensitive and stable biosensor was constructed through the self-assembly of the designed conjugates composed of a multifunctional peptide (MP) and PEGylated distearoylphosphatidylethanolamine (DSPE-PEG). The self-assembly capability of the DSPE-PEG-MP was demonstrated clearly through coarse-grained molecular dynamics simulation and transmission electron microscopy, and it can be effectively self-assembled onto the electrode surface modified with gold nanoparticles. The MP was designed to be antifouling and contained a peptide sequence that can specifically bind the target protein Annexin A1 (ANXA1), and the D-type amino acid composition of MP can enhance its resistance to enzymatic hydrolysis. The unique design of MP, in conjugation with the self-assembly capability of the PEGylated phospholipid DSPE-PEG, enabled the biosensor to exhibit excellent antifouling capability and stability in various complex human body fluids. The biosensor was capable of sensitively and selectively quantifying ANXA1 and achieved a limit of detection down to 0.12 pg mL–1. More importantly, the biosensor demonstrated satisfactory accuracy for ANXA1 detection in clinical serum samples, as verified by the enzyme linked immunosorbent assay (ELISA) kits. It is expected that various antifouling biosensors suitable for application in complex biological environments can be constructed by utilizing the strategy of designing similar DSPE-PEG-MP conjugates.
{"title":"A Nonfouling Electrochemical Biosensor for Protein Analysis in Complex Body Fluids Based on Multifunctional Peptide Conjugated with PEGlyated Phospholipid","authors":"Yang Li, Rui Han, Baoping Zhu, Wenqing Wang, Zhen Song, Xiliang Luo","doi":"10.1021/acssensors.4c02425","DOIUrl":"https://doi.org/10.1021/acssensors.4c02425","url":null,"abstract":"Developing antifouling biosensors capable of performing robustly in complex human body fluids is crucial for biomarker diagnosis and health monitoring. Herein, an antifouling and highly sensitive and stable biosensor was constructed through the self-assembly of the designed conjugates composed of a multifunctional peptide (MP) and PEGylated distearoylphosphatidylethanolamine (DSPE-PEG). The self-assembly capability of the DSPE-PEG-MP was demonstrated clearly through coarse-grained molecular dynamics simulation and transmission electron microscopy, and it can be effectively self-assembled onto the electrode surface modified with gold nanoparticles. The MP was designed to be antifouling and contained a peptide sequence that can specifically bind the target protein Annexin A1 (ANXA1), and the D-type amino acid composition of MP can enhance its resistance to enzymatic hydrolysis. The unique design of MP, in conjugation with the self-assembly capability of the PEGylated phospholipid DSPE-PEG, enabled the biosensor to exhibit excellent antifouling capability and stability in various complex human body fluids. The biosensor was capable of sensitively and selectively quantifying ANXA1 and achieved a limit of detection down to 0.12 pg mL<sup>–1</sup>. More importantly, the biosensor demonstrated satisfactory accuracy for ANXA1 detection in clinical serum samples, as verified by the enzyme linked immunosorbent assay (ELISA) kits. It is expected that various antifouling biosensors suitable for application in complex biological environments can be constructed by utilizing the strategy of designing similar DSPE-PEG-MP conjugates.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":null,"pages":null},"PeriodicalIF":8.9,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142444277","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-17DOI: 10.1021/acssensors.4c01873
Yuqing Gu, Jiayi Wang, Zhewen Luo, Xingyi Luo, Linley Li Lin, Shuang Ni, Cong Wang, Haoran Chen, Zehou Su, Yao Lu, Li-Yong Gan, Zhou Chen, Jian Ye
Label-free surface-enhanced Raman spectroscopy (SERS) is capable of capturing rich compositional information from complex biosamples by providing vibrational spectra that are crucial for biosample identification. However, increasing complexity and subtle variations in biological media can diminish the discrimination accuracy of traditional SERS excited by a single laser wavelength. Herein, we introduce a multiwavelength SERS approach combined with machine learning (ML)-based classification to improve the discrimination accuracy of human urine specimens for bladder cancer (BCa) diagnosis. This strategy leverages the excitation-wavelength-dependent SERS spectral profiles of complex matrices, which are mainly attributed to wavelength-related vibrational changes in individual analytes and differences in the variation ratios of SERS intensity across different wavelengths among various analytes. By capturing SERS fingerprints under multiple excitation wavelengths, we can acquire more comprehensive and unique chemical information on complex samples. Further experimental examinations with clinical urine specimens, supported by ML algorithms, demonstrate the effectiveness of this multiwavelength strategy and improve the diagnostic accuracy of BCa and staging of its invasion with SERS spectra from increasing numbers of wavelengths. The multiwavelength SERS holds promise as a convenient, cost-effective, and broadly applicable technique for the precise identification of complex matrices and diagnosis of diseases based on body fluids.
{"title":"Multiwavelength Surface-Enhanced Raman Scattering Fingerprints of Human Urine for Cancer Diagnosis","authors":"Yuqing Gu, Jiayi Wang, Zhewen Luo, Xingyi Luo, Linley Li Lin, Shuang Ni, Cong Wang, Haoran Chen, Zehou Su, Yao Lu, Li-Yong Gan, Zhou Chen, Jian Ye","doi":"10.1021/acssensors.4c01873","DOIUrl":"https://doi.org/10.1021/acssensors.4c01873","url":null,"abstract":"Label-free surface-enhanced Raman spectroscopy (SERS) is capable of capturing rich compositional information from complex biosamples by providing vibrational spectra that are crucial for biosample identification. However, increasing complexity and subtle variations in biological media can diminish the discrimination accuracy of traditional SERS excited by a single laser wavelength. Herein, we introduce a multiwavelength SERS approach combined with machine learning (ML)-based classification to improve the discrimination accuracy of human urine specimens for bladder cancer (BCa) diagnosis. This strategy leverages the excitation-wavelength-dependent SERS spectral profiles of complex matrices, which are mainly attributed to wavelength-related vibrational changes in individual analytes and differences in the variation ratios of SERS intensity across different wavelengths among various analytes. By capturing SERS fingerprints under multiple excitation wavelengths, we can acquire more comprehensive and unique chemical information on complex samples. Further experimental examinations with clinical urine specimens, supported by ML algorithms, demonstrate the effectiveness of this multiwavelength strategy and improve the diagnostic accuracy of BCa and staging of its invasion with SERS spectra from increasing numbers of wavelengths. The multiwavelength SERS holds promise as a convenient, cost-effective, and broadly applicable technique for the precise identification of complex matrices and diagnosis of diseases based on body fluids.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":null,"pages":null},"PeriodicalIF":8.9,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142448895","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Monitoring biomarkers secreted by cardiomyocytes is critical to evaluate anticancer drug-induced myocardial injury (MI). Cardiac troponin I (cTnI) is considered the gold standard biomarker for MI. Herein, an electrochemical aptasensor is engineered for cTnI detection based on lanthanide europium metal–organic frameworks (Eu-MOFs) and a hybridization chain reaction-directed DNAzyme strategy. Three types of Eu-MOF morphologies were easily synthesized by changing the solvent, and the Eu-MOF modulated by mixing the solvent of dimethylformamide and H2O (D-Eu-MOF) exhibited the best performance compared to other morphologies of the Eu-MOFs. Multifunctional nanoprobes were constructed from D-Eu-MOF@Pt loaded with natural horseradish peroxidase and combined with an aptamer-initiated nuclear acid hybridization chain reaction to form G-quadruplex/hemin DNAzymes for signal amplification. A novel capture probe is constructed on the basis of DNA nanotetrahedrons modified on screen-printed gold electrodes to enhance the capture of the target and multifunctional nanoprobes for signal amplification. It exhibits a detection limit of 0.17 pg mL–1 and a linear range from 0.5 pg mL–1 to 15 ng mL–1. The practicality of the platform is evaluated by measuring cTnI in real samples and secreted by cardiomyocytes after drug treatment, which provides great potential in drug-induced MI evaluation for clinical application.
监测心肌细胞分泌的生物标志物对于评估抗癌药物诱发的心肌损伤（MI）至关重要。心肌肌钙蛋白 I（cTnI）被认为是心肌梗死的金标准生物标志物。本文基于镧系元素铕金属有机框架（Eu-MOFs）和杂交链反应引导的 DNA 酶策略，设计了一种用于检测 cTnI 的电化学传感器。与其他形态的 Eu-MOF 相比，二甲基甲酰胺和 H2O 混合溶剂调制的 Eu-MOF（D-Eu-MOF）表现出最佳性能。由装载天然辣根过氧化物酶的 D-Eu-MOF@Pt 构建了多功能纳米探针，并将其与适配体引发的核酸杂交链反应相结合，形成用于信号放大的 G-四链/hemin DNA 酶。一种新型捕获探针是在丝网印刷金电极上修饰的 DNA 纳米四面体的基础上构建的，以增强对目标的捕获，并利用多功能纳米探针进行信号放大。其检测限为 0.17 pg mL-1，线性范围为 0.5 pg mL-1 至 15 ng mL-1。通过测量真实样本中的 cTnI 和药物治疗后心肌细胞分泌的 cTnI，评估了该平台的实用性，为药物诱导的心肌缺血评估提供了巨大的临床应用潜力。
{"title":"Aptamer-Based Electrochemical Biosensing Platform for Analysis of Cardiac Biomarkers","authors":"Mengjie Chen, Zelin Yang, Zhuoliang Hu, Yudan Hao, Jing Lu, Duanping Sun","doi":"10.1021/acssensors.4c01594","DOIUrl":"https://doi.org/10.1021/acssensors.4c01594","url":null,"abstract":"Monitoring biomarkers secreted by cardiomyocytes is critical to evaluate anticancer drug-induced myocardial injury (MI). Cardiac troponin I (cTnI) is considered the gold standard biomarker for MI. Herein, an electrochemical aptasensor is engineered for cTnI detection based on lanthanide europium metal–organic frameworks (Eu-MOFs) and a hybridization chain reaction-directed DNAzyme strategy. Three types of Eu-MOF morphologies were easily synthesized by changing the solvent, and the Eu-MOF modulated by mixing the solvent of dimethylformamide and H<sub>2</sub>O (D-Eu-MOF) exhibited the best performance compared to other morphologies of the Eu-MOFs. Multifunctional nanoprobes were constructed from D-Eu-MOF@Pt loaded with natural horseradish peroxidase and combined with an aptamer-initiated nuclear acid hybridization chain reaction to form G-quadruplex/hemin DNAzymes for signal amplification. A novel capture probe is constructed on the basis of DNA nanotetrahedrons modified on screen-printed gold electrodes to enhance the capture of the target and multifunctional nanoprobes for signal amplification. It exhibits a detection limit of 0.17 pg mL<sup>–1</sup> and a linear range from 0.5 pg mL<sup>–1</sup> to 15 ng mL<sup>–1</sup>. The practicality of the platform is evaluated by measuring cTnI in real samples and secreted by cardiomyocytes after drug treatment, which provides great potential in drug-induced MI evaluation for clinical application.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":null,"pages":null},"PeriodicalIF":8.9,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142444276","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Semiconductor gas sensors were confirmed to perform high linearity and a stable baseline under alternating current (AC) impedance measurements. However, a procedure to determine the optimal parameters of AC impedance measurements is still lacking. Taking the detection of SF6 decomposition gas as an example, this work has established a model of semiconductor gas sensors under AC impedance measurement. Employing four types of sensors to detect three gases (H2S, SO2, and CO), the effectiveness of the optimization method has been validated, as well. With the high linearity and stable baseline obtained from AC impedance measurement, it enables rapid correction of temperature drift within environmental temperatures ranging from 10 to 30 °C. Overall, the proposed method can provide a novel approach to inhibit the drift failure of semiconductor gas sensors.
经证实，半导体气体传感器在交流阻抗测量中具有较高的线性度和稳定的基线。然而，目前仍缺乏确定交流阻抗测量最佳参数的程序。本研究以检测 SF6 分解气体为例，建立了交流阻抗测量下的半导体气体传感器模型。采用四种传感器检测三种气体（H2S、SO2 和 CO），验证了优化方法的有效性。交流阻抗测量法具有线性度高、基线稳定的特点，可在 10 至 30 °C 的环境温度范围内快速修正温度漂移。总之，所提出的方法为抑制半导体气体传感器的漂移失效提供了一种新方法。
{"title":"Parameter Optimization of Semiconductor Gas Sensor under AC Impedance Measurement","authors":"Jifeng Chu, Zhuoli Deng, Jianbin Pan, Aijun Yang, Qiongyuan Wang, Hongye Yuan, Huan Yuan, Feng Xin, Mingzhe Rong, Xiaohua Wang","doi":"10.1021/acssensors.4c01903","DOIUrl":"https://doi.org/10.1021/acssensors.4c01903","url":null,"abstract":"Semiconductor gas sensors were confirmed to perform high linearity and a stable baseline under alternating current (AC) impedance measurements. However, a procedure to determine the optimal parameters of AC impedance measurements is still lacking. Taking the detection of SF<sub>6</sub> decomposition gas as an example, this work has established a model of semiconductor gas sensors under AC impedance measurement. Employing four types of sensors to detect three gases (H<sub>2</sub>S, SO<sub>2</sub>, and CO), the effectiveness of the optimization method has been validated, as well. With the high linearity and stable baseline obtained from AC impedance measurement, it enables rapid correction of temperature drift within environmental temperatures ranging from 10 to 30 °C. Overall, the proposed method can provide a novel approach to inhibit the drift failure of semiconductor gas sensors.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":null,"pages":null},"PeriodicalIF":8.9,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142440461","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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