{"title":"Enhancing NO2 Gas Sensing: The Dual Impact of UV and Thermal Activation on Vertically Aligned Nb-MoS2 for Superior Response and Selectivity","authors":"Suresh Kumar, Atanu Betal, Ashok Kumar, Atul G. Chakkar, Pradeep Kumar, Monika Kwoka, Satyajit Sahu, Mahesh Kumar","doi":"10.1021/acssensors.4c03489","DOIUrl":"https://doi.org/10.1021/acssensors.4c03489","url":null,"abstract":"Nitrogen dioxide (NO<sub>2</sub>) is considered to be a highly hazardous gas found in combustion engine exhaust, which causes several diseases at a young age. To detect NO<sub>2</sub> at room temperature (RT), two-dimensional transition metal dichalcogenides play an essential role because of their greater surface-to-volume ratio. However, their higher limit of detection (LOD), slow response, and incomplete recovery kinetics hinder their use in efficient gas sensors. To mitigate these issues, we fabricate a facile and robust niobium (Nb)-doped molybdenum disulfide (MoS<sub>2</sub>) sensor using low-pressure chemical vapor deposition on a SiO<sub>2</sub>/Si substrate. Doping is confirmed through various characterization techniques. As compared to pristine MoS<sub>2</sub>, three batches of sensors are prepared with different weight percentages of Nb (8, 16, and 24%). Out of these, the 16% Nb-MoS<sub>2</sub> sensor gives a greatly enhanced relative response of ∼30% for 500 ppb NO<sub>2</sub> at 100 °C with an LOD of 489 ppt. Also, the sensor gives an ultrahigh response of ∼39% (18%) for 50 ppm (500 ppb) NO<sub>2</sub> under 0.4 mW/cm<sup>2</sup> intensity of UV light and exhibits a lower LOD of 117 ppt at RT. In addition, the 16% Nb-MoS<sub>2</sub> sensor shows impressive selectivity toward NO<sub>2</sub> against a range of reducing and oxidizing gases, along with exceptional long-term durability and stability. Based on density functional theory calculations, a comprehensive gas sensing mechanism is proposed. The calculations focus on identifying the favorable sites for NO<sub>2</sub> adsorption on 16% Nb-MoS<sub>2</sub> nanoflakes. This study offers a compelling and practical approach to boosting the efficiency of Nb-MoS<sub>2</sub>-based NO<sub>2</sub> gas sensors.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"66 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-03-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143532736","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}
ACS SensorsPub Date : 2025-03-02DOI: 10.1021/acssensors.4c03450
Mark Potter, Suman Debnath, Pavan Mandapati, Ken Schmidt, Kathy Janzen, Marcus W. Drover, Simon Rondeau-Gagné, Bulent Mutus
{"title":"The Selective and Sensitive Fluorogenic Detection of Hydrogen Gas Using an Azomethine-H Dye","authors":"Mark Potter, Suman Debnath, Pavan Mandapati, Ken Schmidt, Kathy Janzen, Marcus W. Drover, Simon Rondeau-Gagné, Bulent Mutus","doi":"10.1021/acssensors.4c03450","DOIUrl":"https://doi.org/10.1021/acssensors.4c03450","url":null,"abstract":"Hydrogen (H<sub>2(g)</sub>) is a viable green fossil fuel alternative, as its combustion yields only water and energy. However, H<sub>2(g)</sub> is highly flammable, explosive, and lacks odor. These characteristics warrant sensitive and specific detection methods for its widespread use as an alternative fuel source. Recently, there has been growing interest in the development of H<sub>2(g)</sub> sensors, particularly those that are easy to use, environmentally friendly, and sensitive. Here, we show the first example of an optical fluorogenic hydrogen sensing platform, which employs a readily available dye azomethine-H (Az-H, 4-hydroxy-5-(2-hydroxy-benzylideneamino)-naphthalene-2,7-disulfonic acid) and a hydrogen-transferring compound [{Ir(Cp*)(Cl)}<sub>2</sub>(thbpym)](Cl)<sub>2</sub> (IrCp*, (Cp* = C<sub>5</sub>Me<sub>5</sub><sup>–</sup>, thbpym = 4,4′,6,6′-tetrahydroxy-2,2′-bipyrimidine)) to engineer H<sub>2(g)</sub> gas selectivity with high sensitivity at room temperature and pressure. This system yields ∼47–fold fluorescence enhancement when exposed to H<sub>2(g)</sub> in aqueous solution or ∼2.4–fold in a carboxymethyl cellulose (CMC) hydrogel matrix, with an estimated detection limit of ∼0.5% H<sub>2(g)</sub> with no cross-reactivity observed for potentially contaminating gases such as nitrogen (N<sub>2(g)</sub>), oxygen (O<sub>2(g)</sub>), or air.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"9 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-03-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143532735","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}
ACS SensorsPub Date : 2025-03-01DOI: 10.1021/acssensors.4c03047
Stefan Kucharski, Michael Vorochta, Lesia Piliai, Andrew M. Beale, Christopher Blackman
{"title":"Interplay between CO and Surface Lattice Oxygen Ions in the Vacancy-Mediated Response Mechanism of SnO2-Based Gas Sensors","authors":"Stefan Kucharski, Michael Vorochta, Lesia Piliai, Andrew M. Beale, Christopher Blackman","doi":"10.1021/acssensors.4c03047","DOIUrl":"https://doi.org/10.1021/acssensors.4c03047","url":null,"abstract":"Despite having been commercially available for more than half a century, conductometric gas sensors still lack a definite description of their operation mechanism, which hinders research into improving their characteristics. With the advent of operando spectroscopy comes the opportunity to elucidate their working principle by observing their surface during sensing. To that end, we have employed near-ambient pressure (NAP) XPS with simultaneous resistance measurements to correlate the macroscopic sensor response with atomistic changes to the sensor’s surface under exposure to CO, a common target gas. Our results show a clear relationship between the sensor response and the change in surface stoichiometry of SnO<sub>2</sub>, suggesting that near-surface oxygen vacancies play a vital role in the sensing mechanism, in support of a vacancy-modulated “surface conductivity” mechanism.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"86 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143528214","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}
ACS SensorsPub Date : 2025-03-01DOI: 10.1021/acssensors.4c03312
Guangrong Zou, Penglong Si, Jiaqi Wang, Meihua Yang, Jie Chen, Chaoxing Liu, Zhaofan Luo
{"title":"Chemical Modification Coupled with Isothermal CRISPR-Based Assay for Sensitive Detection of DNA Hydroxymethylation","authors":"Guangrong Zou, Penglong Si, Jiaqi Wang, Meihua Yang, Jie Chen, Chaoxing Liu, Zhaofan Luo","doi":"10.1021/acssensors.4c03312","DOIUrl":"https://doi.org/10.1021/acssensors.4c03312","url":null,"abstract":"5-Hydroxymethylcytosine (5hmC) plays a key role in the DNA demethylation process and serves as a stable epigenetic marker in the human genome which is closely associated with disease progression, particularly in diabetes, colorectal cancer, and liver cancer. However, convenient and sensitive methods for detecting and quantifying 5hmC in the genome are scarce, especially in complex biological environments. Herein, a novel attempt at hypersensitive quantitative detection of 5hmC was presented. A multifunctional photosensitive probe was therefore introduced for specific labeling, enrichment, and elution of 5hmC-DNA. Combining with isothermal assay leveraging rolling circle amplification and Cas12a for accurate recognition, we achieved quantitative detection of 5hmC DNA in trace amounts at a level of 11 fM. Global 5hmC was measured in various biological samples using as little as 10 ng of input DNA by a real-time PCR instrument. The reported approach imposed no sequence restrictions, demonstrating promising potential for detecting modified bases in trace amounts of nucleic acids within complex environments, such as blood, urine, and saliva samples.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"34 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143526293","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}
ACS SensorsPub Date : 2025-02-28Epub Date: 2025-02-13DOI: 10.1021/acssensors.4c03534
Jiayi Chen, Ziyun Miao, Chengjie Ma, Bing Qi, Lingling Qiu, Jiahui Tan, Yurong Wei, Jie Wang
{"title":"Bispecific Metabolic Monitoring Platform for Bacterial Identification and Antibiotic Susceptibility Testing.","authors":"Jiayi Chen, Ziyun Miao, Chengjie Ma, Bing Qi, Lingling Qiu, Jiahui Tan, Yurong Wei, Jie Wang","doi":"10.1021/acssensors.4c03534","DOIUrl":"10.1021/acssensors.4c03534","url":null,"abstract":"<p><p>Prompt and reliable bacterial identification and antibiotic susceptibility testing are vital for combating bacterial infections and drug resistance. Herein, we designed a bispecific metabolic monitoring platform that targets enzyme-catalyzed biochemical reactions for bacterial identification and antibiotic susceptibility testing. Specifically, we designed two kinds of coreshell-structured persistent luminescence nanoparticles with surface-confined red and green persistent luminescence, respectively. The persistent luminescence nanoparticles were functionalized with energy acceptors that can be specifically cleaved by bacterial enzymes. The surface-confined persistent luminescence amplified the Förster resonance energy transfer (FRET) efficacy from the nanoparticles to the surface energy acceptors, even though the diameter of the nanoparticles exceeded the critical size of FRET, which improved the sensitivity of bacterial enzyme monitoring. Due to the differentiated expression and secretion of enzymes, different species of bacteria produced discrepant red and green persistent luminescence after incubation with the persistent luminescence nanoprobes. Machine learning models were trained by the characteristic persistent luminescence patterns of bacteria for unknown bacterial identification. Prompt bacteria identification was realized, and the overall accuracy reached 100%. Moreover, the machine learning model could identify the active and inactive states of bacteria treated with antibiotics, which provided a prompt and convenient method to determine whether the bacteria were susceptible to the antibiotics. This study provides a robust method to monitor bacterial metabolism and offers a promising strategy for infection treatment, bacterial communication monitoring, and pathogenicity investigation.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":" ","pages":"1470-1482"},"PeriodicalIF":8.2,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143412314","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}
{"title":"Combating Pathogenic Immune Evasion: Sialidase-Activated Thermally Delayed Fluorescence for Probing and Modulating Host-Pathogen Interactions.","authors":"Qian Liu, Qinghua Wang, Xiangchuan Meng, Xiang Wang, Qingyang Zhang, Hai-Yu Hu","doi":"10.1021/acssensors.4c02917","DOIUrl":"10.1021/acssensors.4c02917","url":null,"abstract":"<p><p>Innate immunity represents the primary defense against invasive pathogens with phagocytosis playing a central role in host defense and mediating immune and inflammatory responses. However, pathogens such as <i>Clostridium perfringens</i> have developed strategies to overcome phagocytic clearance. Developing molecular tools to identify and target key factors in pathogenic immune evasion can deepen our understanding of host-pathogen interactions and aid in exploring novel therapeutic strategies. As a key enzyme in the sialylation process of <i>C. perfringens</i>, the virulence factor sialidase is a potential target for investigating pathogenic immune evasion. Herein, a \"turn-on\" thermally activated delayed fluorescent probe <b>SA-HBT-PXZ</b> is developed as a highly selective and sensitive sialidase sensor, enabling time-resolved fluorescence imaging of <i>C. perfringens</i> in live bacterial cells, tissue sections, and even infected mice. Furthermore, <b>SA-HBT-PXZ</b> is successfully employed to screen sialidase inhibitors based on prompt and delayed fluorescence emissions. The identified lead compounds effectively inhibit the activity of sialidases from <i>C. perfringens</i>, leading to an increased level of differentiation of macrophages into the M1 subtype. This, in turn, enhances the phagocytosis of <i>C. perfringens</i> and ultimately suppresses the immune escape of the bacteria. Our study provides a potential target and lead compounds for novel therapeutic strategies against <i>C. perfringens</i> infections.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":" ","pages":"1072-1082"},"PeriodicalIF":8.2,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143412315","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}
ACS SensorsPub Date : 2025-02-28Epub Date: 2025-02-14DOI: 10.1021/acssensors.4c02765
Yapeng Wu, Bei Lv, Xintian Ni, Sheng Zhu, Dawei Li
{"title":"\"All-U-Want\" Strand Displacement Amplification: A Versatile Signal Amplification Method for Nucleic Acid Biosensing.","authors":"Yapeng Wu, Bei Lv, Xintian Ni, Sheng Zhu, Dawei Li","doi":"10.1021/acssensors.4c02765","DOIUrl":"10.1021/acssensors.4c02765","url":null,"abstract":"<p><p>Strand displacement amplification (SDA) is an isothermal DNA amplification technique. Herein, we developed a novel SDA system, designated All-U-Want SDA (AUW-SDA), which was used as a signal amplification strategy for the construction of nucleic acid detection biosensors. AUW-SDA is capable of target turnover and can be utilized for detection of nucleic acid sequences without available 3'-ends. Of particular significance is the ability of AUW-SDA to generate a substantial number of programmable sequences in accordance with the specifications of the sensor signal output methods, irrespective of the sequence of the target nucleic acid. We used the <i>N</i> gene of SARS-CoV-2 as a model target to develop a sensing platform with dual signal outputs. The colorimetric signals were generated by the G-quadruplex/hemin DNAzyme, in which the G-rich sequences were produced by AUW-SDA with a C-rich primer. On the other hand, by altering the sequence within the replaceable region of the primer, an activator sequence was obtained from AUW-SDA, which could trigger the activity of CRISPR/Cas12a, cleaving the probes modified with a fluorophore and quencher at each end and subsequently yielding the fluorescent signals. After the DNA sequences and reaction conditions were optimized, the limit of detection (LOD) values of the fluorescent and colorimetric assays were estimated to be 0.672 fM and 13.3 fM, respectively. The biosensors were utilized for biological sample detection. The reliability of the proposed method was validated against RT-qPCR results. In addition, a portable scanner-assisted high-throughput RGB analysis (PSHRA) method was developed. This method was applied to our biosensor for multilocus detection of SARS-CoV-2. The results obtained were satisfactory, indicating the potential of this approach for field testing or point-of-care (POC) diagnostics.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":" ","pages":"965-976"},"PeriodicalIF":8.2,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143416703","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}
ACS SensorsPub Date : 2025-02-28Epub Date: 2025-01-30DOI: 10.1021/acssensors.4c03336
Yingkai Lyu, Binmao Zhang, Yujuan Chai, Jie Zhang, Li Wang, Yujin Xiao, Bangning Cheng, Chungen Qian, Hui Yang, Hao Li, Xiaotian Tan
{"title":"A Quantitative First Passage Time Model for Tubular Microfluidic Immunoassays.","authors":"Yingkai Lyu, Binmao Zhang, Yujuan Chai, Jie Zhang, Li Wang, Yujin Xiao, Bangning Cheng, Chungen Qian, Hui Yang, Hao Li, Xiaotian Tan","doi":"10.1021/acssensors.4c03336","DOIUrl":"10.1021/acssensors.4c03336","url":null,"abstract":"<p><p>Solid-phase immunosorbent reactions, such as ELISA, are widely used for detecting, identifying, and quantifying protein markers. However, traditional centimeter scale well-based immunoreactors suffer from low surface-to-volume (S/V) ratios, leading to large sample consumption and a long assay time. Microfluidic technologies, particularly tubular microfluidic immunoreactors, have emerged as promising alternatives due to their high S/V ratios. Despite experimental advancements, multifactor theoretical studies on tubular microfluidic systems are limited. In this study, we present a theoretical model based on the first passage time method to analyze diffusion-controlled reaction kinetics in tubular microfluidic immunoreactors. We focus on key parameters including binding kinetics, reactor size, and solution viscosity. To validate the model, controlled laboratory experiments were conducted using our in-house developed tip optofluidic immunoassay (TOI). These experimental results confirmed the reliability of theoretical models in the behavior prediction of tubular microfluidic systems under real-world conditions. Our model revealed that accurate and rapid protein biomarker quantification requires not only the development of microscale bioreactors but also the design of next-generation probes with extraordinary binding affinity and specificity. This work offers insights into optimizing critical design parameters in future microfluidic immunoassay development, paving ways for next generation microliter-sized biomolecular analysis.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":" ","pages":"1387-1397"},"PeriodicalIF":8.2,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143062209","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}
{"title":"Parts-per-Trillion-Level Acetone Gas Detection Using a Suspended Graphene/SiO<sub>2</sub> SAW Breath and Skin Gas Sensor: Simulation and Experimental Study.","authors":"Haolong Zhou, Sankar Ganesh Ramaraj, Md Shamim Sarker, Siyi Tang, Hiroyasu Yamahara, Hitoshi Tabata","doi":"10.1021/acssensors.4c02344","DOIUrl":"10.1021/acssensors.4c02344","url":null,"abstract":"<p><p>Detection of parts-per-trillion (ppt)-level acetone gas molecules at room temperature using suspended graphene on SiO<sub>2</sub> micropillars has rarely been achieved using solid-state devices or surface acoustic wave (SAW) sensors. This paper presents the effect of SiO<sub>2</sub> micropillars and suspended graphene as a guiding and sensing layer to detect acetone gas. The integration of suspended graphene with SiO<sub>2</sub> micropillars introduces a coupled resonance effect arising from the interaction between the mechanical vibrations of the graphene and the acoustic vibrations of the micropillars. This effect leads to the formation of hybrid resonance modes when the natural frequencies of the vibrations align. This coupling mechanism amplifies the displacement and energy of the Love wave propagating along the surface of the sensor, enhancing its overall performance. Additionally, the interaction of the Love waves with the SiO<sub>2</sub> micropillars and the suspended graphene generates characteristic dips in the transmission spectra. These dips correspond to the excitation of specific flexural and torsional resonance modes within the structure. A custom-fabricated SAW device, featuring micropillars with a diameter of 4 μm and heights of 1.0 and 1.2 μm, demonstrated exceptionally high sensitivity toward acetone gas at a concentration of 500 ppt. Moreover, the suspended graphene exhibited rapid response and recovery times across a wide range of acetone concentrations.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":" ","pages":"804-813"},"PeriodicalIF":8.2,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143412317","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}