Pub Date : 2024-10-02DOI: 10.1021/acssensors.4c01482
Dongmin Shi, Yilin Yin, Xiaoyuan Li, Jie Yuan
The early diagnosis of cancer in a point-of-need manner is of great significance, yet it remains challenging to achieve the necessary sensitivity and speed. Traditional lateral flow immunoassay (LFIA) methods are limited in accuracy and quantification, restricting their suitability for home-based applications. Thus, we explored a new and user-friendly electrochemical LFIA (e-LFIA) test strip to detect α-fetoprotein (AFP), a diagnostic marker for liver cancer. The specific electrochemical immunoprobe utilized in this e-LFIA test strip is characterized by significant signal boosting, resulted from the loading Ag shell into a gold nanoparticle (AuNP)-coated dendritic mesoporous silica nanoscaffold (DMSN). Leveraging the distinct electrochemical characteristics of Ag anodic stripping and the high volume-to-surface area ratio of DMSNs, the developed DMSNs/AuNPs@Ag-based e-LFIA test strip is capable of detecting AFP at a low concentration of 0.85 ng/mL within a rapid 20 min timespan, both of these values are smaller than those in current clinical testing. Furthermore, we utilized homemade screen-printed electrodes in this sensing prototype and demonstrated the high versatility and reliability of this e-LFIA device. We envision that this DMSNs/AuNPs@Ag-based e-LFIA holds substantial potential for the early diagnosis of liver cancer and household health monitoring.
{"title":"Signal-Boosted Electrochemical Lateral Flow Immunoassay for Early Point-of-Care Detection of Liver Cancer Biomarker.","authors":"Dongmin Shi, Yilin Yin, Xiaoyuan Li, Jie Yuan","doi":"10.1021/acssensors.4c01482","DOIUrl":"https://doi.org/10.1021/acssensors.4c01482","url":null,"abstract":"<p><p>The early diagnosis of cancer in a point-of-need manner is of great significance, yet it remains challenging to achieve the necessary sensitivity and speed. Traditional lateral flow immunoassay (LFIA) methods are limited in accuracy and quantification, restricting their suitability for home-based applications. Thus, we explored a new and user-friendly electrochemical LFIA (e-LFIA) test strip to detect α-fetoprotein (AFP), a diagnostic marker for liver cancer. The specific electrochemical immunoprobe utilized in this e-LFIA test strip is characterized by significant signal boosting, resulted from the loading Ag shell into a gold nanoparticle (AuNP)-coated dendritic mesoporous silica nanoscaffold (DMSN). Leveraging the distinct electrochemical characteristics of Ag anodic stripping and the high volume-to-surface area ratio of DMSNs, the developed DMSNs/AuNPs@Ag-based e-LFIA test strip is capable of detecting AFP at a low concentration of 0.85 ng/mL within a rapid 20 min timespan, both of these values are smaller than those in current clinical testing. Furthermore, we utilized homemade screen-printed electrodes in this sensing prototype and demonstrated the high versatility and reliability of this e-LFIA device. We envision that this DMSNs/AuNPs@Ag-based e-LFIA holds substantial potential for the early diagnosis of liver cancer and household health monitoring.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":null,"pages":null},"PeriodicalIF":8.2,"publicationDate":"2024-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142363416","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 : 2024-10-01DOI: 10.1021/acssensors.4c01406
Alix Thomas, Kapil Upadhyaya, Daniel Bejan, Hayden Adoff, Michael Cohen, Carsten Schultz
ADP-ribosylation, the transfer of ADP-ribose (ADPr) from nicotinamide adenine dinucleotide (NAD+) groups to proteins, is a conserved post-translational modification (PTM) that occurs most prominently in response to DNA damage. ADP-ribosylation is a dynamic PTM regulated by writers (PARPs), erasers (ADPr hydrolases), and readers (ADPR binders). PARP1 is the primary DNA damage-response writer responsible for adding a polymer of ADPR to proteins (PARylation). Real-time monitoring of PARP1-mediated PARylation, especially in live cells, is critical for understanding the spatial and temporal regulation of this unique PTM. Here, we describe a genetically encoded FRET probe (pARS) for semiquantitative monitoring of PARylation dynamics. pARS feature a PAR-binding WWE domain flanked with turquoise and Venus. With a ratiometric readout and excellent signal-to-noise characteristics, we show that pARS can monitor PARP1-dependent PARylation temporally and spatially in real-time. pARS provided unique insights into PARP1-mediated PARylation kinetics in vitro and high-sensitivity detection of PARylation in live cells, even under mild DNA damage. We also show that pARS can be used to determine the potency of PARP inhibitors in vitro and, for the first time, in live cells in response to DNA damage. The robustness and ease of use of pARS make it an important tool for the PARP field.
ADP-ribosylation 是指从烟酰胺腺嘌呤二核苷酸(NAD+)基团向蛋白质转移 ADP-ribose (ADPr),它是一种保守的翻译后修饰 (PTM),主要发生在 DNA 损伤时。ADP-ribosylation 是一种动态的 PTM,由写入者(PARPs)、擦除者(ADPr 水解酶)和读取者(ADPR 结合者)调控。PARP1 是主要的 DNA 损伤反应写入器,负责将 ADPR 聚合物添加到蛋白质中(PARylation)。实时监测 PARP1 介导的 PARylation,尤其是活细胞中的 PARylation,对于了解这种独特 PTM 的空间和时间调控至关重要。在这里,我们描述了一种用于半定量监测 PARylation 动态的基因编码 FRET 探针(pARS)。通过比率读数和出色的信噪比特性,我们发现 pARS 可以在时间和空间上实时监测 PARP1 依赖性 PARylation。pARS 为体外 PARP1 介导的 PARylation 动力学提供了独特的见解,并能在活细胞中高灵敏度地检测 PARylation,即使在轻微 DNA 损伤的情况下也是如此。我们还表明,pARS 可用于确定 PARP 抑制剂在体外的效力,并首次用于活细胞中对 DNA 损伤的反应。pARS 的稳健性和易用性使其成为 PARP 领域的重要工具。
{"title":"A Genetically Encoded Sensor for Real-Time Monitoring of Poly-ADP-Ribosylation Dynamics In Vitro and in Cells.","authors":"Alix Thomas, Kapil Upadhyaya, Daniel Bejan, Hayden Adoff, Michael Cohen, Carsten Schultz","doi":"10.1021/acssensors.4c01406","DOIUrl":"10.1021/acssensors.4c01406","url":null,"abstract":"<p><p>ADP-ribosylation, the transfer of ADP-ribose (ADPr) from nicotinamide adenine dinucleotide (NAD<sup>+</sup>) groups to proteins, is a conserved post-translational modification (PTM) that occurs most prominently in response to DNA damage. ADP-ribosylation is a dynamic PTM regulated by writers (PARPs), erasers (ADPr hydrolases), and readers (ADPR binders). PARP1 is the primary DNA damage-response writer responsible for adding a polymer of ADPR to proteins (PARylation). Real-time monitoring of PARP1-mediated PARylation, especially in live cells, is critical for understanding the spatial and temporal regulation of this unique PTM. Here, we describe a genetically encoded FRET probe (pARS) for semiquantitative monitoring of PARylation dynamics. pARS feature a PAR-binding WWE domain flanked with turquoise and Venus. With a ratiometric readout and excellent signal-to-noise characteristics, we show that pARS can monitor PARP1-dependent PARylation temporally and spatially in real-time. pARS provided unique insights into PARP1-mediated PARylation kinetics in vitro and high-sensitivity detection of PARylation in live cells, even under mild DNA damage. We also show that pARS can be used to determine the potency of PARP inhibitors in vitro and, for the first time, in live cells in response to DNA damage. The robustness and ease of use of pARS make it an important tool for the PARP field.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":null,"pages":null},"PeriodicalIF":8.2,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142337270","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 : 2024-10-01DOI: 10.1021/acssensors.4c01568
Yi Zhang, Hengtuo Xing, Jin Li, Fang Han, Suna Fan, Yaopeng Zhang
With the advancement of modern medical and brain–computer interface devices, flexible artificial nociceptors with tactile perception hold significant scientific importance and exhibit great potential in the fields of wearable electronic devices and biomimetic robots. Here, a bioinspired artificial intelligent nociceptive alarm system integrating sensing monitoring and transmission functions is constructed using a silk fibroin (SF) fibrous memristor. This memristor demonstrates high stability, low operating power, and the capability to simulate synaptic plasticity. As a result, an artificial pressure nociceptor based on the SF fibrous memristor can detect both fast and chronic pain and provide a timely alarm in the event of a fall or prolonged immobility of the carrier. Further, an array of artificial pressure nociceptors not only monitors the pressure distribution across various parts of the carrier but also provides direct feedback on the extent of long-term pressure to the carrier. This work holds significant implications for medical support in biological carriers or targeted maintenance of electronic carriers.
{"title":"Bioinspired Artificial Intelligent Nociceptive Alarm System Based on Fibrous Biomemristors","authors":"Yi Zhang, Hengtuo Xing, Jin Li, Fang Han, Suna Fan, Yaopeng Zhang","doi":"10.1021/acssensors.4c01568","DOIUrl":"https://doi.org/10.1021/acssensors.4c01568","url":null,"abstract":"With the advancement of modern medical and brain–computer interface devices, flexible artificial nociceptors with tactile perception hold significant scientific importance and exhibit great potential in the fields of wearable electronic devices and biomimetic robots. Here, a bioinspired artificial intelligent nociceptive alarm system integrating sensing monitoring and transmission functions is constructed using a silk fibroin (SF) fibrous memristor. This memristor demonstrates high stability, low operating power, and the capability to simulate synaptic plasticity. As a result, an artificial pressure nociceptor based on the SF fibrous memristor can detect both fast and chronic pain and provide a timely alarm in the event of a fall or prolonged immobility of the carrier. Further, an array of artificial pressure nociceptors not only monitors the pressure distribution across various parts of the carrier but also provides direct feedback on the extent of long-term pressure to the carrier. This work holds significant implications for medical support in biological carriers or targeted maintenance of electronic carriers.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":null,"pages":null},"PeriodicalIF":8.9,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142360616","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 : 2024-09-30DOI: 10.1021/acssensors.4c01027
Trung-Anh Le, Tan-Phat Huynh
Hemicelluloses (HCs) are promising sustainable biopolymers with a great natural abundance, excellent biocompatibility, and biodegradability. Yet, their potential sensing applications remain limited due to intrinsic challenges in their heterogeneous chemical composition, structure, and physicochemical properties. Herein, recent advances in the development of HC-based sensors for different chemical analytes and physical stimuli using different transduction mechanisms are reviewed and discussed. HCs can be utilized as carbonaceous precursors, reducing, capping, and stabilizing agents, binders, and active components for sensing applications. In addition, different strategies to develop and improve the sensing capacity of HC-based sensors are also highlighted.
{"title":"Hemicellulose-Based Sensors: When Sustainability Meets Complexity","authors":"Trung-Anh Le, Tan-Phat Huynh","doi":"10.1021/acssensors.4c01027","DOIUrl":"https://doi.org/10.1021/acssensors.4c01027","url":null,"abstract":"Hemicelluloses (HCs) are promising sustainable biopolymers with a great natural abundance, excellent biocompatibility, and biodegradability. Yet, their potential sensing applications remain limited due to intrinsic challenges in their heterogeneous chemical composition, structure, and physicochemical properties. Herein, recent advances in the development of HC-based sensors for different chemical analytes and physical stimuli using different transduction mechanisms are reviewed and discussed. HCs can be utilized as carbonaceous precursors, reducing, capping, and stabilizing agents, binders, and active components for sensing applications. In addition, different strategies to develop and improve the sensing capacity of HC-based sensors are also highlighted.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":null,"pages":null},"PeriodicalIF":8.9,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329909","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}
Transition metal oxide semiconductors have great potential for use in H2 sensors, but in recent years, the strange phenomena about gas-sensitive performance associated with their special properties have been more widely discussed in research. In some cases, the resistance of transition metal oxide gas sensors will emerge with some changes contrary to their intrinsic semiconductor characteristics, especially in gas sensor research of WO3. Based on the hydrothermal synthesis of WO3, our work focuses on the abnormal change of tungsten oxide resistance to different gases at low temperature (80–200 °C) and high temperature (above 200 °C). Through in situ FT-IR and in situ XPS, combined with density functional theory calculations, a new reasonable explanation of WO3 is proposed for the abnormal resistance change caused by temperature and the strange response due to gas concentration. The occurrence of these findings can be attributed to the synergistic effect resulting from the presence of two contributing factors. One of them is attributed to the alteration in the surface valence state of WO3 induced by gas, resulting in the reduction of W6+. The other one is due to the reaction between gas and adsorbed oxygen on the surface of WO3. This work presents a novel and rational concept for addressing the reaction mechanism between gas and transition metal oxide semiconductors, thereby paving the way for the development of highly efficient gas sensors based on transition metal oxide semiconductors.
{"title":"Observation on Switching Properties of WO3-Based H2 Sensor Regulated by Temperature and Gas Concentration","authors":"Beixi An, Yifan Yang, Yanrong Wang, Ruixia Li, Zhengkun Wu, Peizhe Wang, Tingyu Zhang, Ruiqi Han, Erqing Xie","doi":"10.1021/acssensors.4c01212","DOIUrl":"https://doi.org/10.1021/acssensors.4c01212","url":null,"abstract":"Transition metal oxide semiconductors have great potential for use in H<sub>2</sub> sensors, but in recent years, the strange phenomena about gas-sensitive performance associated with their special properties have been more widely discussed in research. In some cases, the resistance of transition metal oxide gas sensors will emerge with some changes contrary to their intrinsic semiconductor characteristics, especially in gas sensor research of WO<sub>3</sub>. Based on the hydrothermal synthesis of WO<sub>3</sub>, our work focuses on the abnormal change of tungsten oxide resistance to different gases at low temperature (80–200 °C) and high temperature (above 200 °C). Through in situ FT-IR and in situ XPS, combined with density functional theory calculations, a new reasonable explanation of WO<sub>3</sub> is proposed for the abnormal resistance change caused by temperature and the strange response due to gas concentration. The occurrence of these findings can be attributed to the synergistic effect resulting from the presence of two contributing factors. One of them is attributed to the alteration in the surface valence state of WO<sub>3</sub> induced by gas, resulting in the reduction of W<sup>6+</sup>. The other one is due to the reaction between gas and adsorbed oxygen on the surface of WO<sub>3</sub>. This work presents a novel and rational concept for addressing the reaction mechanism between gas and transition metal oxide semiconductors, thereby paving the way for the development of highly efficient gas sensors based on transition metal oxide semiconductors.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":null,"pages":null},"PeriodicalIF":8.9,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142330370","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 : 2024-09-30DOI: 10.1021/acssensors.4c00539
Jeffrey W. Beard, Samuel L. Hunt, Alexander Evans, Coleman Goenner, Benjamin L. Miller
Point of care (PoC) nucleic acid amplification tests (NAATs) are a cornerstone of public health, providing the earliest and most accurate diagnostic method for many communicable diseases in the same location where the patient receives treatment. Communicable diseases, such as human immunodeficiency virus (HIV), disproportionately impact low-resource communities where NAATs are often unobtainable due to the resource-intensive enzymes that drive the tests. Enzyme-free nucleic acid detection methods, such as hybridization chain reaction (HCR), use DNA secondary structures for self-driven amplification schemes, producing large DNA nanostructures, capable of single-molecule detection in cellulo. These thermodynamically driven DNA-based tests have struggled to penetrate the PoC diagnostic field due to their inadequate limits of detection or complex workflows. Here, we present a proof-of-concept NAAT that combines HCR-based amplification of a target nucleic acid sequence with paper-based nucleic acid filtration and enrichment capable of detecting sub-pM levels of synthetic DNA. We reconstruct the favorable hybridization conditions of an in cellulo reaction in vitro by incubating HCR in an evaporating, microvolume environment containing poly(ethylene glycol) as a crowding agent. We demonstrate that the kinetics and thermodynamics of DNA–DNA and DNA–RNA hybridization is enhanced by the dynamic evaporating environment and inclusion of crowding agents, bringing HCR closer to meeting PoC NAAT needs.
医疗点核酸扩增检测(NAATs)是公共卫生的基石,可在患者接受治疗的同一地点为许多传染病提供最早、最准确的诊断方法。人类免疫缺陷病毒(HIV)等传染病对资源匮乏的社区造成了极大的影响,而在这些社区,由于需要使用耗费大量资源的酶来进行检测,因此往往无法获得 NAAT。无酶核酸检测方法,如杂交链反应(HCR),利用 DNA 二级结构进行自驱动扩增,产生大型 DNA 纳米结构,能够在细胞内进行单分子检测。这些基于热力学驱动的 DNA 检测方法由于检测极限不足或工作流程复杂,一直难以渗透到 PoC 诊断领域。在这里,我们介绍一种概念验证型 NAAT,它将基于 HCR 的目标核酸序列扩增与基于纸的核酸过滤和富集相结合,能够检测亚 pM 水平的合成 DNA。我们通过在含有聚乙二醇(poly(ethylene glycol)作为拥挤剂的蒸发微体积环境中培养 HCR,重建了体外细胞内反应的有利杂交条件。我们证明,DNA-DNA 和 DNA-RNA 杂交的动力学和热力学在动态蒸发环境和加入拥挤剂后得到增强,从而使 HCR 更接近于满足 PoC NAAT 的需求。
{"title":"Mimicking a Cellular Crowding Environment for Enzyme-Free Paper-Based Nucleic Acid Tests at the Point of Care","authors":"Jeffrey W. Beard, Samuel L. Hunt, Alexander Evans, Coleman Goenner, Benjamin L. Miller","doi":"10.1021/acssensors.4c00539","DOIUrl":"https://doi.org/10.1021/acssensors.4c00539","url":null,"abstract":"Point of care (PoC) nucleic acid amplification tests (NAATs) are a cornerstone of public health, providing the earliest and most accurate diagnostic method for many communicable diseases in the same location where the patient receives treatment. Communicable diseases, such as human immunodeficiency virus (HIV), disproportionately impact low-resource communities where NAATs are often unobtainable due to the resource-intensive enzymes that drive the tests. Enzyme-free nucleic acid detection methods, such as hybridization chain reaction (HCR), use DNA secondary structures for self-driven amplification schemes, producing large DNA nanostructures, capable of single-molecule detection <i>in cellulo</i>. These thermodynamically driven DNA-based tests have struggled to penetrate the PoC diagnostic field due to their inadequate limits of detection or complex workflows. Here, we present a proof-of-concept NAAT that combines HCR-based amplification of a target nucleic acid sequence with paper-based nucleic acid filtration and enrichment capable of detecting sub-pM levels of synthetic DNA. We reconstruct the favorable hybridization conditions of an <i>in cellulo</i> reaction <i>in vitro</i> by incubating HCR in an evaporating, microvolume environment containing poly(ethylene glycol) as a crowding agent. We demonstrate that the kinetics and thermodynamics of DNA–DNA and DNA–RNA hybridization is enhanced by the dynamic evaporating environment and inclusion of crowding agents, bringing HCR closer to meeting PoC NAAT needs.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":null,"pages":null},"PeriodicalIF":8.9,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142330288","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 : 2024-09-29DOI: 10.1021/acssensors.4c01791
Xuefei Zhao, Shan Jiang, Zhaorui Zhang, Xiaohui Yan, Zhihang Xu, Huashuai Hu, Ye Zhu, J. Paul Attfield, Minghui Yang
Detecting H2S in oxygen-deficient conditions is vital for identifying leaks in SF6-insulated electrical equipment. Current infrared-based detection methods are expensive and sensitive to environmental conditions, highlighting the necessity for cost-effective and stable gas sensors. Existing gas sensors based on semiconducting metal oxides (SMOXs) are limited by redox reactions with oxygen and require high operating temperatures. Here, we introduce a room-temperature (RT) H2S sensor for oxygen-deficient environments using the intrinsic conducting two-dimensional (2D) metal–organic framework (MOF), Co1.8Ni1.2(hexaiminotriphenylene)2 [Co1.8Ni1.2(HITP)2], overcoming the limitations of SMOX gas sensors. Remarkably, Co1.8Ni1.2(HITP)2 sensors exhibit exceptional selectivity for H2S with negligible cross-responses and a sensitivity drift of less than 4.13% in an SF6 atmosphere over 60 days. The Co1.8Ni1.2(HITP)2 gas sensor shows significant promise for real-time and stable monitoring of H2S gas in oxygen-deficient environments.
{"title":"High-Performance H2S Sensors to Detect SF6 Leakage","authors":"Xuefei Zhao, Shan Jiang, Zhaorui Zhang, Xiaohui Yan, Zhihang Xu, Huashuai Hu, Ye Zhu, J. Paul Attfield, Minghui Yang","doi":"10.1021/acssensors.4c01791","DOIUrl":"https://doi.org/10.1021/acssensors.4c01791","url":null,"abstract":"Detecting H<sub>2</sub>S in oxygen-deficient conditions is vital for identifying leaks in SF<sub>6</sub>-insulated electrical equipment. Current infrared-based detection methods are expensive and sensitive to environmental conditions, highlighting the necessity for cost-effective and stable gas sensors. Existing gas sensors based on semiconducting metal oxides (SMOXs) are limited by redox reactions with oxygen and require high operating temperatures. Here, we introduce a room-temperature (RT) H<sub>2</sub>S sensor for oxygen-deficient environments using the intrinsic conducting two-dimensional (2D) metal–organic framework (MOF), Co<sub>1.8</sub>Ni<sub>1.2</sub>(hexaiminotriphenylene)<sub>2</sub> [Co<sub>1.8</sub>Ni<sub>1.2</sub>(HITP)<sub>2</sub>], overcoming the limitations of SMOX gas sensors. Remarkably, Co<sub>1.8</sub>Ni<sub>1.2</sub>(HITP)<sub>2</sub> sensors exhibit exceptional selectivity for H<sub>2</sub>S with negligible cross-responses and a sensitivity drift of less than 4.13% in an SF<sub>6</sub> atmosphere over 60 days. The Co<sub>1.8</sub>Ni<sub>1.2</sub>(HITP)<sub>2</sub> gas sensor shows significant promise for real-time and stable monitoring of H<sub>2</sub>S gas in oxygen-deficient environments.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":null,"pages":null},"PeriodicalIF":8.9,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142330291","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 : 2024-09-28DOI: 10.1021/acssensors.4c01444
Wenjing Wang, Jie Yang
Although several imaging strategies for dual fluorescence (or Förster) resonance energy transfer (FRET) biosensors have been reported, their implementation is challenging because of the limited performance of fluorescent proteins and the spectral overlap of FRET biosensors. These processes often require additional data calibration to eliminate artifacts. Many CFP/YFP FRET biosensors have been developed. In this study, we introduced the mKate3/HT7(JFX650) FRET pair, which effectively formed two pairs of FRET pairs for dual-FRET imaging when combined with the CFP/YFP FRET pair. The FRET donor mKate3 exhibited higher brightness than its predecessor mKate. The FRET acceptor, HT7(JFX650), is a HaloTag7 protein covalently conjugated with a far-red JFX650-THL ligand. The pair comprising mKate3 and HT7(JFX650) represents an excellent FRET dyad, exhibiting a high FRET efficiency ratio. To use the FRET pair for dual FRET biosensor imaging, we constructed PKA and K+ biosensors based on the mKate3/HT7(JFX650) FRET pair. These biosensors can be used along with CFP/YFP biosensors to simultaneously detect the responses of intracellular PKA/Src, PKA/Ca2+, and K+/Ca2+ under different stimuli. The findings revealed that dual FRET biosensors, which are based on the combination of CFP/YFP and mKate3/HT7 (JFX650), exhibit adequate compatibility and can be used to visualize multiple molecular activities in a live cell.
{"title":"Development of mKate3/HaloTag7 (JFX650) and CFP/YFP Dual-Fluorescence (or Förster) Resonance Energy Transfer Pairs for Visualizing Dual-Molecular Activity","authors":"Wenjing Wang, Jie Yang","doi":"10.1021/acssensors.4c01444","DOIUrl":"https://doi.org/10.1021/acssensors.4c01444","url":null,"abstract":"Although several imaging strategies for dual fluorescence (or Förster) resonance energy transfer (FRET) biosensors have been reported, their implementation is challenging because of the limited performance of fluorescent proteins and the spectral overlap of FRET biosensors. These processes often require additional data calibration to eliminate artifacts. Many CFP/YFP FRET biosensors have been developed. In this study, we introduced the mKate3/HT7(JFX650) FRET pair, which effectively formed two pairs of FRET pairs for dual-FRET imaging when combined with the CFP/YFP FRET pair. The FRET donor mKate3 exhibited higher brightness than its predecessor mKate. The FRET acceptor, HT7(JFX650), is a HaloTag7 protein covalently conjugated with a far-red JFX650-THL ligand. The pair comprising mKate3 and HT7(JFX650) represents an excellent FRET dyad, exhibiting a high FRET efficiency ratio. To use the FRET pair for dual FRET biosensor imaging, we constructed PKA and K<sup>+</sup> biosensors based on the mKate3/HT7(JFX650) FRET pair. These biosensors can be used along with CFP/YFP biosensors to simultaneously detect the responses of intracellular PKA/Src, PKA/Ca<sup>2+</sup>, and K<sup>+</sup>/Ca<sup>2+</sup> under different stimuli. The findings revealed that dual FRET biosensors, which are based on the combination of CFP/YFP and mKate3/HT7 (JFX650), exhibit adequate compatibility and can be used to visualize multiple molecular activities in a live cell.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":null,"pages":null},"PeriodicalIF":8.9,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329104","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}
The metastasis of cancer cells is a principal cause of morbidity and mortality in cancer. The combination of a cytosensor and photothermal therapy (PTT) cannot completely eliminate cancer cells at one time. Hence, this study aimed to design a localized surface plasmonic resonance (LSPR)-based aptasensor for a circuit of cytosensing-PTT (COCP). This was achieved by coating a novel sandwich layer of polydopamine/gold nanoparticles/polydopamine (PDA/AuNPs/PDA) around the Ω-shaped fiber-optic (Ω-FO). The short-wavelength peak of the sandwich layer with strong resonance exhibited a high refractive index sensitivity (RIS). The modification with the T-shaped aptamer endowed FO-LSPR with unique characteristics of time-dependent sensitivity enhancement behavior for a sensitive cytosensor with the lowest limit of detection (LOD) of 13 cells/mL. The long-wavelength resonance peak in the sandwich layer appears in the near-infrared region. Hence, the rate of increased localized temperature of FO-LSPR was 160 and 30-fold higher than that of the bare and PDA-coated FO, indicating strong photothermal conversion efficiency. After considering the localized temperature distribution around the FO under the flow environment, the FO-LSPR-enabled aptasensor killed 77.6% of cancer cells in simulated blood circulation after five cycles of COCP. The FO-LSPR-enabled aptasensor improved the efficiency of the cytosensor and PTT to effectively kill cancer cells, showing significant potential for application in inhibiting cancer metastasis.
{"title":"Sandwich Layer-Modified Ω-Shaped Fiber-Optic LSPR Enables the Development of an Aptasensor for a Cytosensing-Photothermal Therapy Circuit.","authors":"Xinyu Kong, Xingliang He, Fan He, Yu Li, Yanting Feng, Yongxin Li, Zewei Luo, Ji-Wei Shen, Yixiang Duan","doi":"10.1021/acssensors.4c00841","DOIUrl":"10.1021/acssensors.4c00841","url":null,"abstract":"<p><p>The metastasis of cancer cells is a principal cause of morbidity and mortality in cancer. The combination of a cytosensor and photothermal therapy (PTT) cannot completely eliminate cancer cells at one time. Hence, this study aimed to design a localized surface plasmonic resonance (LSPR)-based aptasensor for a circuit of cytosensing-PTT (COCP). This was achieved by coating a novel sandwich layer of polydopamine/gold nanoparticles/polydopamine (PDA/AuNPs/PDA) around the Ω-shaped fiber-optic (Ω-FO). The short-wavelength peak of the sandwich layer with strong resonance exhibited a high refractive index sensitivity (RIS). The modification with the T-shaped aptamer endowed FO-LSPR with unique characteristics of time-dependent sensitivity enhancement behavior for a sensitive cytosensor with the lowest limit of detection (LOD) of 13 cells/mL. The long-wavelength resonance peak in the sandwich layer appears in the near-infrared region. Hence, the rate of increased localized temperature of FO-LSPR was 160 and 30-fold higher than that of the bare and PDA-coated FO, indicating strong photothermal conversion efficiency. After considering the localized temperature distribution around the FO under the flow environment, the FO-LSPR-enabled aptasensor killed 77.6% of cancer cells in simulated blood circulation after five cycles of COCP. The FO-LSPR-enabled aptasensor improved the efficiency of the cytosensor and PTT to effectively kill cancer cells, showing significant potential for application in inhibiting cancer metastasis.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":null,"pages":null},"PeriodicalIF":8.2,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141904930","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 : 2024-09-27Epub Date: 2024-08-12DOI: 10.1021/acssensors.4c00957
Haoxin Ye, Xinzhe Zheng, Haoming Yang, Matthew D Kowal, Teresa M Seifried, Gurvendra Pal Singh, Krishna Aayush, Guang Gao, Edward Grant, David Kitts, Rickey Y Yada, Tianxi Yang
The accumulation of micro/nanoplastics (MNPs) in ecosystems poses tremendous environmental risks for terrestrial and aquatic organisms. Designing rapid, field-deployable, and sensitive devices for assessing the potential risks of MNPs pollution is critical. However, current techniques for MNPs detection have limited effectiveness. Here, we design a wireless portable device that allows rapid, sensitive, and on-site detection of MNPs, followed by remote data processing via machine learning algorithms for quantitative fluorescence imaging. We utilized a supramolecular labeling strategy, employing luminescent metal-phenolic networks composed of zirconium ions, tannic acid, and rhodamine B, to efficiently label various sizes of MNPs (e.g., 50 nm-10 μm). Results showed that our device can quantify MNPs as low as 330 microplastics and 3.08 × 106 nanoplastics in less than 20 min. We demonstrated the applicability of the device to real-world samples through determination of MNPs released from plastic cups after hot water and flow induction and nanoplastics in tap water. Moreover, the device is user-friendly and operative by untrained personnel to conduct data processing on the APP remotely. The analytical platform integrating quantitative imaging, customized data processing, decision tree model, and low-cost analysis ($0.015 per assay) has great potential for high-throughput screening of MNPs in agrifood and environmental systems.
{"title":"Cost-Effective and Wireless Portable Device for Rapid and Sensitive Quantification of Micro/Nanoplastics.","authors":"Haoxin Ye, Xinzhe Zheng, Haoming Yang, Matthew D Kowal, Teresa M Seifried, Gurvendra Pal Singh, Krishna Aayush, Guang Gao, Edward Grant, David Kitts, Rickey Y Yada, Tianxi Yang","doi":"10.1021/acssensors.4c00957","DOIUrl":"10.1021/acssensors.4c00957","url":null,"abstract":"<p><p>The accumulation of micro/nanoplastics (MNPs) in ecosystems poses tremendous environmental risks for terrestrial and aquatic organisms. Designing rapid, field-deployable, and sensitive devices for assessing the potential risks of MNPs pollution is critical. However, current techniques for MNPs detection have limited effectiveness. Here, we design a wireless portable device that allows rapid, sensitive, and on-site detection of MNPs, followed by remote data processing via machine learning algorithms for quantitative fluorescence imaging. We utilized a supramolecular labeling strategy, employing luminescent metal-phenolic networks composed of zirconium ions, tannic acid, and rhodamine B, to efficiently label various sizes of MNPs (e.g., 50 nm-10 μm). Results showed that our device can quantify MNPs as low as 330 microplastics and 3.08 × 10<sup>6</sup> nanoplastics in less than 20 min. We demonstrated the applicability of the device to real-world samples through determination of MNPs released from plastic cups after hot water and flow induction and nanoplastics in tap water. Moreover, the device is user-friendly and operative by untrained personnel to conduct data processing on the APP remotely. The analytical platform integrating quantitative imaging, customized data processing, decision tree model, and low-cost analysis ($0.015 per assay) has great potential for high-throughput screening of MNPs in agrifood and environmental systems.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":null,"pages":null},"PeriodicalIF":8.2,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141915420","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}