Pub Date : 2025-02-28Epub Date: 2025-01-30DOI: 10.1021/acssensors.4c03184
James Humphries, Jody Hobson-Peters, Saikat Ghosh, Christopher B Howard, Pie Huda, Craig A Bell, Nicholas L Fletcher, Kristian Kempe, Kristofer J Thurecht
Recent examples of immune responses directed against the synthetic polymer poly(ethylene glycol) (PEG) have led to the development of biocompatible polymers, which are viewed as promising candidates to act as surrogate materials for use in biological applications, such as hydrophilic poly(2-oxazoline)s (POx). Despite this, the characterization of critical aspects of the immune response against these emerging materials is sparse, in part because no known monoclonal antibodies (mAbs) against this family of synthetic material have been reported. To advance the understanding of such responses, we report the successful isolation and characterization of hybridoma-derived mAbs with excellent specificity for different POx species and notable selectivity for highly branched polymer architectures over linear systems. In conjunction with established mAbs targeted against PEG, we show that these antibodies can be employed for sensitive in vivo multiplex-detection of label-free polymer therapeutics based on the specificity of the polymer-antibody binding. This approach enables scalable therapeutic drug monitoring of multiple polymer therapeutics within a single animal, simultaneously.
{"title":"Multiplexing Label-Free Polymeric Nanocarriers via Antipolymer Antibodies.","authors":"James Humphries, Jody Hobson-Peters, Saikat Ghosh, Christopher B Howard, Pie Huda, Craig A Bell, Nicholas L Fletcher, Kristian Kempe, Kristofer J Thurecht","doi":"10.1021/acssensors.4c03184","DOIUrl":"10.1021/acssensors.4c03184","url":null,"abstract":"<p><p>Recent examples of immune responses directed against the synthetic polymer poly(ethylene glycol) (PEG) have led to the development of biocompatible polymers, which are viewed as promising candidates to act as surrogate materials for use in biological applications, such as hydrophilic poly(2-oxazoline)s (POx). Despite this, the characterization of critical aspects of the immune response against these emerging materials is sparse, in part because no known monoclonal antibodies (mAbs) against this family of synthetic material have been reported. To advance the understanding of such responses, we report the successful isolation and characterization of hybridoma-derived mAbs with excellent specificity for different POx species and notable selectivity for highly branched polymer architectures over linear systems. In conjunction with established mAbs targeted against PEG, we show that these antibodies can be employed for sensitive <i>in vivo</i> multiplex-detection of label-free polymer therapeutics based on the specificity of the polymer-antibody binding. This approach enables scalable therapeutic drug monitoring of multiple polymer therapeutics within a single animal, simultaneously.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":" ","pages":"1280-1288"},"PeriodicalIF":8.2,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143062217","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}
Flexible electrodes fabricated through cost-effective thick-film strategies are important for developing electrochemical devices, such as sensors. Properly engineered nanocomposite electrodes can enhance the electrochemically active surface area, facilitate mass and charge transport, and allow for tailored surface chemistry and structure. Although great efforts have been devoted to developing porous nanocomposite electrodes, a facile method to achieve screen-printed porous nanocomposite electrodes in the form of flexible electrodes with tunable electrochemical performance has been overlooked. This article introduces a strategy for fabricating flexible porous electrodes using screen printing and electrochemical surface treatments, resulting in enhanced surface chemistry and electrochemical properties. By applying selective etching and anodization, the electrode’s surface area increases by 214% compared to a nontreated electrode, enabling programmable sensitivity to specific molecules. The engineered electrode improves the hydroquinone-to-salicylic acid detection ratio from less than 1 to over 10, allowing selective detection of neutral and positively charged molecules while rendering the electrode inactive for negatively charged species. This flexible sensor can be integrated into a wearable glove for rapid analysis and has also been successfully implemented in a second-generation glucose biosensor. This approach holds significant potential for advancing surface electrochemistry, offering new possibilities for tailoring electrode surfaces for diverse analytical applications.
{"title":"Tuning the Surface: Screen-Printed Flexible Porous Nanocomposite Electrodes with Programmable Electrochemical Performances for Wearable Platforms","authors":"Adisak Pokprasert, Natcha Rasitanon, Irlesta Rahma Lani, Itthipon Jeerapan","doi":"10.1021/acssensors.4c03519","DOIUrl":"https://doi.org/10.1021/acssensors.4c03519","url":null,"abstract":"Flexible electrodes fabricated through cost-effective thick-film strategies are important for developing electrochemical devices, such as sensors. Properly engineered nanocomposite electrodes can enhance the electrochemically active surface area, facilitate mass and charge transport, and allow for tailored surface chemistry and structure. Although great efforts have been devoted to developing porous nanocomposite electrodes, a facile method to achieve screen-printed porous nanocomposite electrodes in the form of flexible electrodes with tunable electrochemical performance has been overlooked. This article introduces a strategy for fabricating flexible porous electrodes using screen printing and electrochemical surface treatments, resulting in enhanced surface chemistry and electrochemical properties. By applying selective etching and anodization, the electrode’s surface area increases by 214% compared to a nontreated electrode, enabling programmable sensitivity to specific molecules. The engineered electrode improves the hydroquinone-to-salicylic acid detection ratio from less than 1 to over 10, allowing selective detection of neutral and positively charged molecules while rendering the electrode inactive for negatively charged species. This flexible sensor can be integrated into a wearable glove for rapid analysis and has also been successfully implemented in a second-generation glucose biosensor. This approach holds significant potential for advancing surface electrochemistry, offering new possibilities for tailoring electrode surfaces for diverse analytical applications.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"7 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518580","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 : 2025-02-28Epub Date: 2025-02-13DOI: 10.1021/acssensors.4c03495
Luntao Xia, Wei Xiao, Luoxin Li, Xin Liu, Qibin Zhuang, Yong Huang, Tianhao Lan, Xiaohui Du, Yang Zhao, Dezhi Wu
Flexible capacitive pressure sensors are now widely used in the fields of electronic skin, medical monitoring, and human-computer interaction. However, most of the current flexible capacitive pressure sensors generally suffer easy saturation and low sensitivity under high pressure. This paper proposes a new strategy using evenly distributed spiked nickel (Ni) particles as fillers in a nanofiber membrane to prepare flexible capacitive pressure sensors. The spiked Ni particles are embedded into the interior of polyimide (PI) electrospun nanofiber membranes by electrostatic self-assembly. The experimental results show that the introduction of spiked Ni particles effectively increased the sensitivity of the sensor under high pressure due to the formation of many parallel microcapacitors. In addition, a novel combination method is adopted to integrate individual sensor modules into arbitrary sensor arrays for sensing field pressures. Specifically, the sensor prototype with a 2.7 weight ratio of spiked nickel/PI nanofiber membranes was characterized by short response/recovery times (30/40 ms), wide pressure detection range (1.5 MPa), and excellent mechanical stability (1000 cycles), more than 4-fold increase in sensor sensitivity (4.04 MPa-1 at 0-1.5 MPa) compared to pure PI nanofiber membrane dielectric layers. Due to its superior performance demonstration, the sensor could be applied in many scenarios, such as human motion detection, sleeping posture monitoring, and plantar pressure measurement, indicating good application prospects in diverse wearable systems.
{"title":"High-Performance Flexible Capacitive Pressure Sensor Based on a Spiked Nickel/Polyimide Composite Nanofiber Membrane.","authors":"Luntao Xia, Wei Xiao, Luoxin Li, Xin Liu, Qibin Zhuang, Yong Huang, Tianhao Lan, Xiaohui Du, Yang Zhao, Dezhi Wu","doi":"10.1021/acssensors.4c03495","DOIUrl":"10.1021/acssensors.4c03495","url":null,"abstract":"<p><p>Flexible capacitive pressure sensors are now widely used in the fields of electronic skin, medical monitoring, and human-computer interaction. However, most of the current flexible capacitive pressure sensors generally suffer easy saturation and low sensitivity under high pressure. This paper proposes a new strategy using evenly distributed spiked nickel (Ni) particles as fillers in a nanofiber membrane to prepare flexible capacitive pressure sensors. The spiked Ni particles are embedded into the interior of polyimide (PI) electrospun nanofiber membranes by electrostatic self-assembly. The experimental results show that the introduction of spiked Ni particles effectively increased the sensitivity of the sensor under high pressure due to the formation of many parallel microcapacitors. In addition, a novel combination method is adopted to integrate individual sensor modules into arbitrary sensor arrays for sensing field pressures. Specifically, the sensor prototype with a 2.7 weight ratio of spiked nickel/PI nanofiber membranes was characterized by short response/recovery times (30/40 ms), wide pressure detection range (1.5 MPa), and excellent mechanical stability (1000 cycles), more than 4-fold increase in sensor sensitivity (4.04 MPa<sup>-1</sup> at 0-1.5 MPa) compared to pure PI nanofiber membrane dielectric layers. Due to its superior performance demonstration, the sensor could be applied in many scenarios, such as human motion detection, sleeping posture monitoring, and plantar pressure measurement, indicating good application prospects in diverse wearable systems.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":" ","pages":"1450-1460"},"PeriodicalIF":8.2,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143412316","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 : 2025-02-28DOI: 10.1021/acssensors.5c00330
Guozhen Liu
Rather than being famous only in the gene editing field, by revealing the collateral cleavage activity of Cas12a, Cas13a, and Cas14 effectors, Clustered Regularly Interspaced Short Palindromic Repeats (CRISPR)/CRISPR associated (Cas) systems (i.e., CRISPR/Cas) have received significant credit in modern analytical science with the capability of detecting versatile analytes with superior sensitivity and specificity. (1,2) A variety of exciting CRISPR/Cas biosensing systems have now been developed successfully for detection of different analytes varying from nucleic acids to non-nucleic acids (such as metabolites, proteins, exosomes, and metal ions). Although the most popular signal output in CRISPR/Cas biosensors is fluorescence, various signal output modalities such as colorimetric, electrochemiluminescence, electrochemical, and electrical have been applied in CRISPR/Cas biosensing systems. Furthermore, the potential of CRISPR/Cas has been demonstrated in multiplex detection by integration with microfluidics or other devices enabling identification of the presence of multiple targets. However, despite extensive efforts and success to develop CRISPR/Cas diagnostic tools based on trans-cleavage enzymatic activity, these systems encounter unavoidable challenges, including inadequate detection limit (near the picomole level) for detecting clinically relevant biomarkers at subpicomolar levels and limited catalytic efficiency for DNA cleavage. These limitations significantly hinder the widespread adoption of CRISPR/Cas diagnostic tools in clinical diagnostics and point-of-care testing. To further enhance detection sensitivity and avoid the necessity for sophisticated and costly equipment, nucleic acids-based preamplification techniques, including thermal-dependent amplification, such as polymerase chain reaction (PCR), and thermal-independent amplification, rolling circle amplification (RCA), recombinase polymerase amplification (RPA), or loop-mediated isothermal amplification (LAMP), are frequently integrated with CRISPR/Cas based assays. Although preamplification techniques significantly increase the sensitivity, they inevitably overshadow Cas effectors and neglect the intrinsic detection capability of Cas effectors. Preamplification also extends detection time and reduces the efficiency of subsequent detection due to nonspecific amplification and primer interference, while substantially increasing the risk of aerosol contamination. The most sensitive nucleic acid amplification strategies employ exponential amplification formats in which amplicons (amplification products) are recycled as primers or templates. However, because of the exponential format, nonspecific background products that lead to false-positive results are inevitable after long reaction times and can be caused by, for example, contaminants, off-template polymerase products, and secondary structures of primers or templates. Therefore, the reaction time of exponential amplification has
{"title":"Advancing CRISPR/Cas Biosensing with Integrated Devices","authors":"Guozhen Liu","doi":"10.1021/acssensors.5c00330","DOIUrl":"https://doi.org/10.1021/acssensors.5c00330","url":null,"abstract":"Rather than being famous only in the gene editing field, by revealing the collateral cleavage activity of Cas12a, Cas13a, and Cas14 effectors, Clustered Regularly Interspaced Short Palindromic Repeats (CRISPR)/CRISPR associated (Cas) systems (i.e., CRISPR/Cas) have received significant credit in modern analytical science with the capability of detecting versatile analytes with superior sensitivity and specificity. (1,2) A variety of exciting CRISPR/Cas biosensing systems have now been developed successfully for detection of different analytes varying from nucleic acids to non-nucleic acids (such as metabolites, proteins, exosomes, and metal ions). Although the most popular signal output in CRISPR/Cas biosensors is fluorescence, various signal output modalities such as colorimetric, electrochemiluminescence, electrochemical, and electrical have been applied in CRISPR/Cas biosensing systems. Furthermore, the potential of CRISPR/Cas has been demonstrated in multiplex detection by integration with microfluidics or other devices enabling identification of the presence of multiple targets. However, despite extensive efforts and success to develop CRISPR/Cas diagnostic tools based on trans-cleavage enzymatic activity, these systems encounter unavoidable challenges, including inadequate detection limit (near the picomole level) for detecting clinically relevant biomarkers at subpicomolar levels and limited catalytic efficiency for DNA cleavage. These limitations significantly hinder the widespread adoption of CRISPR/Cas diagnostic tools in clinical diagnostics and point-of-care testing. To further enhance detection sensitivity and avoid the necessity for sophisticated and costly equipment, nucleic acids-based preamplification techniques, including thermal-dependent amplification, such as polymerase chain reaction (PCR), and thermal-independent amplification, rolling circle amplification (RCA), recombinase polymerase amplification (RPA), or loop-mediated isothermal amplification (LAMP), are frequently integrated with CRISPR/Cas based assays. Although preamplification techniques significantly increase the sensitivity, they inevitably overshadow Cas effectors and neglect the intrinsic detection capability of Cas effectors. Preamplification also extends detection time and reduces the efficiency of subsequent detection due to nonspecific amplification and primer interference, while substantially increasing the risk of aerosol contamination. The most sensitive nucleic acid amplification strategies employ exponential amplification formats in which amplicons (amplification products) are recycled as primers or templates. However, because of the exponential format, nonspecific background products that lead to false-positive results are inevitable after long reaction times and can be caused by, for example, contaminants, off-template polymerase products, and secondary structures of primers or templates. Therefore, the reaction time of exponential amplification has ","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"28 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518583","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 : 2025-02-28DOI: 10.1021/acssensors.4c03167
Seyed Mohammad Miri, Büşra N. Ata, Şeyma Çimen, Sarah Barakat, Asal Ghaffari Zaki, Joudi Armouch, Emre Vatandaşlar, Sven Vilain, Gürkan Öztürk, Emrah Eroğlu
Reactive oxygen species, particularly hydrogen peroxide (H2O2), play crucial roles in cellular signaling, with Nrf2 serving as a key transcription factor in maintaining redox homeostasis. However, the precise influence of H2O2 on Nrf2 activity under physiological normoxia remains unclear due to the limitations of oxygen-sensitive imaging methods. To address this, we developed and validated an oxygen-insensitive Nrf2 reporter named pericellular oxygen-insensitive Nrf2 transcriptional performance reporter (POINTER). We employed this reporter in human cerebral microvascular endothelial cells (hCMEC/D3). Using POINTER, we investigated how varying intracellular H2O2 concentrations affect Nrf2 regulation under normoxia (5 kPa O2) compared to hyperoxia (ambient air, 21 kPa O2). We manipulated intracellular H2O2 levels through exogenous application, chemogenetic production using a modified amino acid oxidase, and pharmacological induction with Auranofin. Our findings reveal that Nrf2 transcriptional activity is significantly lower under normoxia than under hyperoxia, supporting previous literature and expectations. Using POINTER, we found that both antioxidant pathway inhibition and sustained H2O2 elevation are essential for modulating Nrf2 activity. These findings provide new insights into the regulation of Nrf2 by H2O2.
{"title":"Development of an Oxygen-Insensitive Nrf2 Reporter Reveals Redox Regulation under Physiological Normoxia","authors":"Seyed Mohammad Miri, Büşra N. Ata, Şeyma Çimen, Sarah Barakat, Asal Ghaffari Zaki, Joudi Armouch, Emre Vatandaşlar, Sven Vilain, Gürkan Öztürk, Emrah Eroğlu","doi":"10.1021/acssensors.4c03167","DOIUrl":"https://doi.org/10.1021/acssensors.4c03167","url":null,"abstract":"Reactive oxygen species, particularly hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>), play crucial roles in cellular signaling, with Nrf2 serving as a key transcription factor in maintaining redox homeostasis. However, the precise influence of H<sub>2</sub>O<sub>2</sub> on Nrf2 activity under physiological normoxia remains unclear due to the limitations of oxygen-sensitive imaging methods. To address this, we developed and validated an oxygen-insensitive Nrf2 reporter named pericellular oxygen-insensitive Nrf2 transcriptional performance reporter (POINTER). We employed this reporter in human cerebral microvascular endothelial cells (hCMEC/D3). Using POINTER, we investigated how varying intracellular H<sub>2</sub>O<sub>2</sub> concentrations affect Nrf2 regulation under normoxia (5 kPa O<sub>2</sub>) compared to hyperoxia (ambient air, 21 kPa O<sub>2</sub>). We manipulated intracellular H<sub>2</sub>O<sub>2</sub> levels through exogenous application, chemogenetic production using a modified amino acid oxidase, and pharmacological induction with Auranofin. Our findings reveal that Nrf2 transcriptional activity is significantly lower under normoxia than under hyperoxia, supporting previous literature and expectations. Using POINTER, we found that both antioxidant pathway inhibition and sustained H<sub>2</sub>O<sub>2</sub> elevation are essential for modulating Nrf2 activity. These findings provide new insights into the regulation of Nrf2 by H<sub>2</sub>O<sub>2</sub>.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"28 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143526292","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}
A composite of sulfur nanosheets (S-NSs) with hydrophobic carbon nanotubes (H-CNTs) was designed, and a chemiresistive gas sensor based on this composite material was constructed for breath analysis of NH3 detection at room temperature. Taking advantage of the capillary condensation of CNTs, the hydrophobic effect of hexadecyltrimethoxysilane (HDTMS), and the high sensitivity of S-NSs to NH3 detection, the constructed sensor showed an improved humidity-resistant capacity and is capable of detecting breath-relevant NH3 concentrations down to ppb level under high humidity. The fabricated gas sensor exhibited fast response/recovery (18/26 s) and good stability. Online monitoring for exhaled breath analysis shows good recovery with a stable baseline, providing a potential practical application. The research also facilitates the development of commercial low-cost breath analysis sensors.
{"title":"Room Temperature and Humidity Resistant NH3 Detection Based on a Composite of Hydrophobic CNTs with Sulfur Nanosheets","authors":"Xiaoni Cui, Huaipeng Wang, Xinglei Wang, Yuchen Tang, Yaozhou Zhang, Yu Dong, Liuwei Jing, Lihua Shen","doi":"10.1021/acssensors.4c02076","DOIUrl":"https://doi.org/10.1021/acssensors.4c02076","url":null,"abstract":"A composite of sulfur nanosheets (S-NSs) with hydrophobic carbon nanotubes (H-CNTs) was designed, and a chemiresistive gas sensor based on this composite material was constructed for breath analysis of NH<sub>3</sub> detection at room temperature. Taking advantage of the capillary condensation of CNTs, the hydrophobic effect of hexadecyltrimethoxysilane (HDTMS), and the high sensitivity of S-NSs to NH<sub>3</sub> detection, the constructed sensor showed an improved humidity-resistant capacity and is capable of detecting breath-relevant NH<sub>3</sub> concentrations down to ppb level under high humidity. The fabricated gas sensor exhibited fast response/recovery (18/26 s) and good stability. Online monitoring for exhaled breath analysis shows good recovery with a stable baseline, providing a potential practical application. The research also facilitates the development of commercial low-cost breath analysis sensors.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"33 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518579","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 : 2025-02-28Epub Date: 2025-01-30DOI: 10.1021/acssensors.4c02954
Dexun Yang, Qilu Nie, Mengen Cheng, Shilong Pei, Cheng Cheng, Donglai Guo, Minghong Yang
This paper presents a compact all-fiber multicomponent gas Raman probe using a dual-fiber architecture within a platinum-coated capillary. The probe eliminates the need for conventional optical components like filters and dichroic mirrors by strategically employing metal coating on the excitation fiber's surface to suppress interference signals. A detailed analysis of the silica Raman signal and fluorescence propagation within the system facilitated this design. Metal-coated capillary (MCC), produced via atomic layer deposition (ALD) of platinum on silica capillaries, exhibits excellent optical properties and environmental resilience, boosting gas Raman signal reception. Careful alignment of the dual fibers relative to the platinum-coated capillary optimizes signal-to-noise ratio enhancement. The system achieves detection limits of 21 ppm for CH4, 30 ppm for C2H4, and 51 ppm for C2H6 within 45 s of exposure, alongside a rapid response time of 25 s (relative to systems based on hollow-core antiresonant fibers) and robust stability. Its streamlined optical path and compact design enhance practicality across diverse fields, including agriculture, industry, environmental monitoring, and healthcare, advancing multicomponent gas detection technology.
{"title":"All-Fiber Multicomponent Gas Raman Probe Based on Platinum-Coated Capillary Enhanced Raman Spectroscopy.","authors":"Dexun Yang, Qilu Nie, Mengen Cheng, Shilong Pei, Cheng Cheng, Donglai Guo, Minghong Yang","doi":"10.1021/acssensors.4c02954","DOIUrl":"10.1021/acssensors.4c02954","url":null,"abstract":"<p><p>This paper presents a compact all-fiber multicomponent gas Raman probe using a dual-fiber architecture within a platinum-coated capillary. The probe eliminates the need for conventional optical components like filters and dichroic mirrors by strategically employing metal coating on the excitation fiber's surface to suppress interference signals. A detailed analysis of the silica Raman signal and fluorescence propagation within the system facilitated this design. Metal-coated capillary (MCC), produced via atomic layer deposition (ALD) of platinum on silica capillaries, exhibits excellent optical properties and environmental resilience, boosting gas Raman signal reception. Careful alignment of the dual fibers relative to the platinum-coated capillary optimizes signal-to-noise ratio enhancement. The system achieves detection limits of 21 ppm for CH<sub>4</sub>, 30 ppm for C<sub>2</sub>H<sub>4</sub>, and 51 ppm for C<sub>2</sub>H<sub>6</sub> within 45 s of exposure, alongside a rapid response time of 25 s (relative to systems based on hollow-core antiresonant fibers) and robust stability. Its streamlined optical path and compact design enhance practicality across diverse fields, including agriculture, industry, environmental monitoring, and healthcare, advancing multicomponent gas detection technology.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":" ","pages":"1113-1122"},"PeriodicalIF":8.2,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143062211","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 : 2025-02-28DOI: 10.1021/acssensors.4c03544
Anubhav Dhull, Ki Wan Park, Aqib Iqbal Dar, Andrew Wang, Anu Rani, Rishi Sharma, Tulio A Valdez, Anjali Sharma
Surgical site infections (SSIs) remain the most common cause for readmission following surgery and are associated with significant medical comorbidities. Distinguishing between inflammation and early infection postsurgery is a critical challenge for clinicians. Intraoperative surgical debridement of infectious tissues relies heavily on the surgeon’s experience, risking error due to difficulty in distinguishing infection from inflammation. We evaluated the simultaneous use of two fluorescent probes, maltotriose-indocyanine-green (ICG-DBCO-maltotriose) and a mixed-layered 2-deoxyglucose dendrimer (2DG-D) labeled with cyanine 5 (2DG-D-Cy5), to delineate between SSI and inflammation in vitro in cell-bacteria coculture and in vivo in an early implant SSI model via multiplexed short-wave infrared (SWIR) imaging. To our knowledge, this study is the first to use multiple fluorescent dyes combined with small molecules and dendrimer-based nanoprobes to differentiate between inflammation and infection within the same experimental model. We synthesized 2DG-D using a convergent method, simplifying synthesis and purification. 2DG-D-Cy5 exclusively labeled the macrophages associated with inflammation in vitro. In vivo SWIR imaging using both probes in a murine implant infection model successfully distinguished infection from inflammation in real time, allowing targeted surgical debridement. This real-time detection of infection and inflammation may enhance diagnostic confidence and aid in the monitoring of therapeutic responses.
{"title":"Mixed-Layered Glycodendrimer Probe for Imaging Inflammation at Surgical Site Infections","authors":"Anubhav Dhull, Ki Wan Park, Aqib Iqbal Dar, Andrew Wang, Anu Rani, Rishi Sharma, Tulio A Valdez, Anjali Sharma","doi":"10.1021/acssensors.4c03544","DOIUrl":"https://doi.org/10.1021/acssensors.4c03544","url":null,"abstract":"Surgical site infections (SSIs) remain the most common cause for readmission following surgery and are associated with significant medical comorbidities. Distinguishing between inflammation and early infection postsurgery is a critical challenge for clinicians. Intraoperative surgical debridement of infectious tissues relies heavily on the surgeon’s experience, risking error due to difficulty in distinguishing infection from inflammation. We evaluated the simultaneous use of two fluorescent probes, maltotriose-indocyanine-green (ICG-DBCO-maltotriose) and a mixed-layered 2-deoxyglucose dendrimer (2DG-D) labeled with cyanine 5 (2DG-D-Cy5), to delineate between SSI and inflammation in vitro in cell-bacteria coculture and in vivo in an early implant SSI model via multiplexed short-wave infrared (SWIR) imaging. To our knowledge, this study is the first to use multiple fluorescent dyes combined with small molecules and dendrimer-based nanoprobes to differentiate between inflammation and infection within the same experimental model. We synthesized 2DG-D using a convergent method, simplifying synthesis and purification. 2DG-D-Cy5 exclusively labeled the macrophages associated with inflammation in vitro. In vivo SWIR imaging using both probes in a murine implant infection model successfully distinguished infection from inflammation in real time, allowing targeted surgical debridement. This real-time detection of infection and inflammation may enhance diagnostic confidence and aid in the monitoring of therapeutic responses.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"13 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143526294","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}
High sensitivity, low concentration, and excellent selectivity are pronounced primary challenges for semiconductor gas sensors to monitor acetone from exhaled breath. In this study, nitrogen-doped carbon quantum dots (N-CQDs) with high reactivity were used to activate dandelion-like hierarchical tungsten oxide (WO3) microspheres to construct an efficient and stable acetone gas sensor. Benefiting from the synergistic effect of both the abundant active sites provided by the unique dandelion-like hierarchical structure and the high reaction potential generated by the sensitization of the N-CQDs, the resulting 16 wt % N-CQDs/WO3 sensor shows an ultrahigh response value (Ra/Rg = 74@1 ppm acetone), low detection limit (0.05 ppm), outstanding selectivity, and reliable stability to acetone at the optimum working temperature of 210 °C. Noteworthy that the N-CQDs facilitate the carrier migration and intensify the reaction between acetone and WO3 during the sensing process. Considering the above advantages, N-CQDs as a sensitizer to achieve excellent gas-sensitive properties of WO3 are a promising new strategy for achieving accurate acetone detection in real time and facilitating the development of portable human-exhaled gas sensors.
{"title":"Nitrogen-Doped Carbon Quantum Dots Activated Dandelion-Like Hierarchical WO<sub>3</sub> for Highly Sensitive and Selective MEMS Sensors in Diabetes Detection.","authors":"Tianjun Ni, Zhonghu Dong, Kejie Xi, Yijia Lu, Kaiwen Chang, Chunpo Ge, Dong Liu, Zhijun Yang, Haijie Cai, Yongheng Zhu","doi":"10.1021/acssensors.4c01840","DOIUrl":"10.1021/acssensors.4c01840","url":null,"abstract":"<p><p>High sensitivity, low concentration, and excellent selectivity are pronounced primary challenges for semiconductor gas sensors to monitor acetone from exhaled breath. In this study, nitrogen-doped carbon quantum dots (N-CQDs) with high reactivity were used to activate dandelion-like hierarchical tungsten oxide (WO<sub>3</sub>) microspheres to construct an efficient and stable acetone gas sensor. Benefiting from the synergistic effect of both the abundant active sites provided by the unique dandelion-like hierarchical structure and the high reaction potential generated by the sensitization of the N-CQDs, the resulting 16 wt % N-CQDs/WO<sub>3</sub> sensor shows an ultrahigh response value (<i>R</i><sub>a</sub>/<i>R</i><sub>g</sub> = 74@1 ppm acetone), low detection limit (0.05 ppm), outstanding selectivity, and reliable stability to acetone at the optimum working temperature of 210 °C. Noteworthy that the N-CQDs facilitate the carrier migration and intensify the reaction between acetone and WO<sub>3</sub> during the sensing process. Considering the above advantages, N-CQDs as a sensitizer to achieve excellent gas-sensitive properties of WO<sub>3</sub> are a promising new strategy for achieving accurate acetone detection in real time and facilitating the development of portable human-exhaled gas sensors.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":" ","pages":"699-708"},"PeriodicalIF":8.2,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142374701","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 : 2025-02-28Epub Date: 2025-01-31DOI: 10.1021/acssensors.4c03180
Xinxin Yuan, Wenchao Geng, Jiangying Ji, Zhiyi Yan, Jiarui Wei, Yongjun Wu, Ruiying Yang
Circular RNAs (circRNAs), as a class of noncoding RNA molecules with a circular structure exhibit high stability and spatiotemporal-specific expression, making them ideal cancer biomarkers for liquid biopsy. Herein, a new photoelectrochemical (PEC) biosensor for a highly sensitive circRNA assay in the whole blood of lung cancer patients was designed based on CRISPR/Cas13a-programmed Cu nanoclusters (Cu NCs) and a Z-scheme covalent organic framework/silver sulfide (T-COF/Ag2S) composite. This Z-scheme T-COF/Ag2S composite accelerates electron transfer and produces an excellent initial photocurrent. When CRISPR/Cas13a precisely targets circRNA, it nonspecifically cleaves the triple-helix molecular structure to release DNA fragments (C'/C"). After the C'/C" opens the DNA hairpin probe (HP) modified on the electrode, hybridization chain reactions are performed to produce abundant AT-rich double-stranded DNA with the addition of H1 and H2 probes. Upon the incubation of Cu2+, Cu NCs are in situ formed via the A-Cu2+-T bonds and can effectively quench the photocurrent of the Z-scheme T-COF/Ag2S due to the energy transfer process. This developed PEC biosensor for the circRNA assay shows a low limit of detection of 0.5 fM, and the reusability of DNA-modified magnetic beads (MB-DNA) reduces the detection cost. Moreover, the PEC biosensor can accurately quantify the circRNA level and distinguish the circRNA expression in whole blood from healthy controls and lung cancer patients, offering strong potential in clinical diagnosis.
{"title":"CRISPR/Cas13a-Programmed Cu NCs and <i>Z</i>-Scheme T-COF/Ag<sub>2</sub>S for Photoelectrochemical Biosensing of circRNA.","authors":"Xinxin Yuan, Wenchao Geng, Jiangying Ji, Zhiyi Yan, Jiarui Wei, Yongjun Wu, Ruiying Yang","doi":"10.1021/acssensors.4c03180","DOIUrl":"10.1021/acssensors.4c03180","url":null,"abstract":"<p><p>Circular RNAs (circRNAs), as a class of noncoding RNA molecules with a circular structure exhibit high stability and spatiotemporal-specific expression, making them ideal cancer biomarkers for liquid biopsy. Herein, a new photoelectrochemical (PEC) biosensor for a highly sensitive circRNA assay in the whole blood of lung cancer patients was designed based on CRISPR/Cas13a-programmed Cu nanoclusters (Cu NCs) and a <i>Z</i>-scheme covalent organic framework/silver sulfide (T-COF/Ag<sub>2</sub>S) composite. This <i>Z</i>-scheme T-COF/Ag<sub>2</sub>S composite accelerates electron transfer and produces an excellent initial photocurrent. When CRISPR/Cas13a precisely targets circRNA, it nonspecifically cleaves the triple-helix molecular structure to release DNA fragments (C'/C\"). After the C'/C\" opens the DNA hairpin probe (HP) modified on the electrode, hybridization chain reactions are performed to produce abundant AT-rich double-stranded DNA with the addition of H1 and H2 probes. Upon the incubation of Cu<sup>2+</sup>, Cu NCs are <i>in situ</i> formed via the A-Cu<sup>2+</sup>-T bonds and can effectively quench the photocurrent of the <i>Z</i>-scheme T-COF/Ag<sub>2</sub>S due to the energy transfer process. This developed PEC biosensor for the circRNA assay shows a low limit of detection of 0.5 fM, and the reusability of DNA-modified magnetic beads (MB-DNA) reduces the detection cost. Moreover, the PEC biosensor can accurately quantify the circRNA level and distinguish the circRNA expression in whole blood from healthy controls and lung cancer patients, offering strong potential in clinical diagnosis.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":" ","pages":"1270-1279"},"PeriodicalIF":8.2,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143062214","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}