Pub Date : 2025-03-16DOI: 10.1021/acssensors.4c0344310.1021/acssensors.4c03443
Ke Ma, Senrong Ye, Gengzhe Shen, Baijun Li, Zijun Pan, Chenchen Bian, Zheng Liu, Chi Zhang, Haowei Kong, Haohan Wu, Yeqing Chen and Xin He*,
Iontronic pressure sensors (IPSs) are emerging as promising candidates for integration into wearable electronics and healthcare monitoring systems due to their high sensitivity and low power consumption. However, achieving high sensitivity across a broad linear pressure range remains a significant challenge. This study presents a novel IPS device with an asymmetric sandwich structure, which includes a three-dimensional electrode made of nickel manganese oxide/carbon nanotubes (NMO/CNT) and an embedded iron needles ionic dielectric layer. The proposed device demonstrates exceptional linearity over 1700 kPa, with a sensitivity exceeding 7700 kPa–1. It exhibits rapid response and recovery times in the millisecond range and maintains a consistent capacitive response over 15,000 loading–unloading cycles. Moreover, the device enables noncontact sensing in response to magnetic field variations, broadening its potential applications. The innovative IPS design effectively balances high sensitivity and a wide linear pressure range, rendering it suitable for various applications such as nonverbal communication aids and healthcare monitoring systems.
{"title":"Iron-Supported Asymmetric Iontronic Pressure Sensors with High Sensitivity and Extended Linearity","authors":"Ke Ma, Senrong Ye, Gengzhe Shen, Baijun Li, Zijun Pan, Chenchen Bian, Zheng Liu, Chi Zhang, Haowei Kong, Haohan Wu, Yeqing Chen and Xin He*, ","doi":"10.1021/acssensors.4c0344310.1021/acssensors.4c03443","DOIUrl":"https://doi.org/10.1021/acssensors.4c03443https://doi.org/10.1021/acssensors.4c03443","url":null,"abstract":"<p >Iontronic pressure sensors (IPSs) are emerging as promising candidates for integration into wearable electronics and healthcare monitoring systems due to their high sensitivity and low power consumption. However, achieving high sensitivity across a broad linear pressure range remains a significant challenge. This study presents a novel IPS device with an asymmetric sandwich structure, which includes a three-dimensional electrode made of nickel manganese oxide/carbon nanotubes (NMO/CNT) and an embedded iron needles ionic dielectric layer. The proposed device demonstrates exceptional linearity over 1700 kPa, with a sensitivity exceeding 7700 kPa<sup>–1</sup>. It exhibits rapid response and recovery times in the millisecond range and maintains a consistent capacitive response over 15,000 loading–unloading cycles. Moreover, the device enables noncontact sensing in response to magnetic field variations, broadening its potential applications. The innovative IPS design effectively balances high sensitivity and a wide linear pressure range, rendering it suitable for various applications such as nonverbal communication aids and healthcare monitoring systems.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"10 3","pages":"2162–2172 2162–2172"},"PeriodicalIF":8.2,"publicationDate":"2025-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713830","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 : 2025-03-14DOI: 10.1021/acssensors.4c0317510.1021/acssensors.4c03175
Caio Lenon Chaves Carvalho, Steffane Q. Nascimento, Thiago Bertaglia, Luana C. I. Faria, Erika R. Manuli, Geovana M. Pereira, Welter Cantanhêde da Silva, Carlos M. Costa, Josu Fernández Maestu, Senentxu Lanceros-Méndez, Osvaldo N. Oliveira Jr., Ester C. Sabino and Frank N. Crespilho*,
The COVID-19 pandemic has highlighted the critical need for scalable, rapid, and cost-effective diagnostic solutions, especially in resource-limited settings. In this study, we developed a sustainable magnetic electrochemical biosensor for the mass testing of SARS-CoV-2, emphasizing affordability, environmental impact reduction, and clinical applicability. By leveraging recycled materials from spent batteries and plastics, we achieved a circular economy-based fabrication process with a recyclability rate of 98.5%. The biosensor employs MnFe2O4 nanoparticles functionalized with anti-SARS-CoV-2 antibodies, integrated into a 3D-printed electrochemical device for decentralized testing. Advanced characterization confirmed the biosensor’s robust performance, including high sensitivity (LOD: 3.46 pg mL–1) and specificity, with results demonstrating a 95% correlation to RT-PCR gold standard testing. The cost of materials used per biosensor test is only USD 0.2, making it highly affordable and suitable for large-scale production using additive manufacturing. Key features include simple preparation, rapid response, and reusability, making it ideal for point-of-care diagnostics. Beyond COVID-19, this platform’s modularity allows for adaptation to other viral diseases, offering a versatile solution to global diagnostic challenges. This work highlights the potential of integrating electrochemical sensing with sustainable practices to address healthcare inequities and reduce environmental impact.
{"title":"Sustainable Electrochemical-Magnetic Biosensor Fabricated from Recycled Materials for Label-Free Detection of SARS-CoV-2 in Human Saliva","authors":"Caio Lenon Chaves Carvalho, Steffane Q. Nascimento, Thiago Bertaglia, Luana C. I. Faria, Erika R. Manuli, Geovana M. Pereira, Welter Cantanhêde da Silva, Carlos M. Costa, Josu Fernández Maestu, Senentxu Lanceros-Méndez, Osvaldo N. Oliveira Jr., Ester C. Sabino and Frank N. Crespilho*, ","doi":"10.1021/acssensors.4c0317510.1021/acssensors.4c03175","DOIUrl":"https://doi.org/10.1021/acssensors.4c03175https://doi.org/10.1021/acssensors.4c03175","url":null,"abstract":"<p >The COVID-19 pandemic has highlighted the critical need for scalable, rapid, and cost-effective diagnostic solutions, especially in resource-limited settings. In this study, we developed a sustainable magnetic electrochemical biosensor for the mass testing of SARS-CoV-2, emphasizing affordability, environmental impact reduction, and clinical applicability. By leveraging recycled materials from spent batteries and plastics, we achieved a circular economy-based fabrication process with a recyclability rate of 98.5%. The biosensor employs MnFe<sub>2</sub>O<sub>4</sub> nanoparticles functionalized with anti-SARS-CoV-2 antibodies, integrated into a 3D-printed electrochemical device for decentralized testing. Advanced characterization confirmed the biosensor’s robust performance, including high sensitivity (LOD: 3.46 pg mL<sup>–1</sup>) and specificity, with results demonstrating a 95% correlation to RT-PCR gold standard testing. The cost of materials used per biosensor test is only USD 0.2, making it highly affordable and suitable for large-scale production using additive manufacturing. Key features include simple preparation, rapid response, and reusability, making it ideal for point-of-care diagnostics. Beyond COVID-19, this platform’s modularity allows for adaptation to other viral diseases, offering a versatile solution to global diagnostic challenges. This work highlights the potential of integrating electrochemical sensing with sustainable practices to address healthcare inequities and reduce environmental impact.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"10 3","pages":"1970–1985 1970–1985"},"PeriodicalIF":8.2,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acssensors.4c03175","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143714105","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-03-14DOI: 10.1021/acssensors.4c03175
Caio Lenon Chaves Carvalho, Steffane Q. Nascimento, Thiago Bertaglia, Luana C. I. Faria, Erika R. Manuli, Geovana M. Pereira, Welter Cantanhêde da Silva, Carlos M. Costa, Josu Fernández Maestu, Senentxu Lanceros-Méndez, Osvaldo N. Oliveira, Jr., Ester C. Sabino, Frank N. Crespilho
The COVID-19 pandemic has highlighted the critical need for scalable, rapid, and cost-effective diagnostic solutions, especially in resource-limited settings. In this study, we developed a sustainable magnetic electrochemical biosensor for the mass testing of SARS-CoV-2, emphasizing affordability, environmental impact reduction, and clinical applicability. By leveraging recycled materials from spent batteries and plastics, we achieved a circular economy-based fabrication process with a recyclability rate of 98.5%. The biosensor employs MnFe2O4 nanoparticles functionalized with anti-SARS-CoV-2 antibodies, integrated into a 3D-printed electrochemical device for decentralized testing. Advanced characterization confirmed the biosensor’s robust performance, including high sensitivity (LOD: 3.46 pg mL–1) and specificity, with results demonstrating a 95% correlation to RT-PCR gold standard testing. The cost of materials used per biosensor test is only USD 0.2, making it highly affordable and suitable for large-scale production using additive manufacturing. Key features include simple preparation, rapid response, and reusability, making it ideal for point-of-care diagnostics. Beyond COVID-19, this platform’s modularity allows for adaptation to other viral diseases, offering a versatile solution to global diagnostic challenges. This work highlights the potential of integrating electrochemical sensing with sustainable practices to address healthcare inequities and reduce environmental impact.
{"title":"Sustainable Electrochemical-Magnetic Biosensor Fabricated from Recycled Materials for Label-Free Detection of SARS-CoV-2 in Human Saliva","authors":"Caio Lenon Chaves Carvalho, Steffane Q. Nascimento, Thiago Bertaglia, Luana C. I. Faria, Erika R. Manuli, Geovana M. Pereira, Welter Cantanhêde da Silva, Carlos M. Costa, Josu Fernández Maestu, Senentxu Lanceros-Méndez, Osvaldo N. Oliveira, Jr., Ester C. Sabino, Frank N. Crespilho","doi":"10.1021/acssensors.4c03175","DOIUrl":"https://doi.org/10.1021/acssensors.4c03175","url":null,"abstract":"The COVID-19 pandemic has highlighted the critical need for scalable, rapid, and cost-effective diagnostic solutions, especially in resource-limited settings. In this study, we developed a sustainable magnetic electrochemical biosensor for the mass testing of SARS-CoV-2, emphasizing affordability, environmental impact reduction, and clinical applicability. By leveraging recycled materials from spent batteries and plastics, we achieved a circular economy-based fabrication process with a recyclability rate of 98.5%. The biosensor employs MnFe<sub>2</sub>O<sub>4</sub> nanoparticles functionalized with anti-SARS-CoV-2 antibodies, integrated into a 3D-printed electrochemical device for decentralized testing. Advanced characterization confirmed the biosensor’s robust performance, including high sensitivity (LOD: 3.46 pg mL<sup>–1</sup>) and specificity, with results demonstrating a 95% correlation to RT-PCR gold standard testing. The cost of materials used per biosensor test is only USD 0.2, making it highly affordable and suitable for large-scale production using additive manufacturing. Key features include simple preparation, rapid response, and reusability, making it ideal for point-of-care diagnostics. Beyond COVID-19, this platform’s modularity allows for adaptation to other viral diseases, offering a versatile solution to global diagnostic challenges. This work highlights the potential of integrating electrochemical sensing with sustainable practices to address healthcare inequities and reduce environmental impact.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"56 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143619025","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}
Surface-enhanced Raman scattering (SERS) offers significant advantages for single-molecule detection. However, stochastic molecular motion makes it challenging to consistently capture signals from single-molecule binding events, particularly in complex environments. Herein, we propose a novel SERS system via the pore nanoconfinement effect of covalent organic frameworks (COFs) to achieve reliable single-molecule detection. The self-assembled COF thin films on SERS metal substrates (Au/Ag) create a nanogap of 3 nm, allowing electric field enhancement. By precise tuning of the COF shell thickness, a molecular-scale pore volume is formed, effectively trapping individual molecules from molecular aggregates. Furthermore, the strong intermolecular forces within the COF pores significantly enhance the residence time of individual molecules, thereby increasing the probability of detecting single-molecule binding events. This innovative approach ensures consistent and reliable SERS single-molecule detection in complex mixtures, paving the way for advanced applications in biochemical sensing and diagnostics.
{"title":"Single-Molecule Detection via Pore Nanoconfinement of Covalent Organic Frameworks for Surface-Enhanced Raman Scattering","authors":"Mengya Lv, Xiao Wu, Wen Wang, Dandan Han, Sheng Chen, Yifan Hu, Qidong Zhang, Qiyan Wang, Ronghan Wei","doi":"10.1021/acssensors.4c02391","DOIUrl":"https://doi.org/10.1021/acssensors.4c02391","url":null,"abstract":"Surface-enhanced Raman scattering (SERS) offers significant advantages for single-molecule detection. However, stochastic molecular motion makes it challenging to consistently capture signals from single-molecule binding events, particularly in complex environments. Herein, we propose a novel SERS system via the pore nanoconfinement effect of covalent organic frameworks (COFs) to achieve reliable single-molecule detection. The self-assembled COF thin films on SERS metal substrates (Au/Ag) create a nanogap of 3 nm, allowing electric field enhancement. By precise tuning of the COF shell thickness, a molecular-scale pore volume is formed, effectively trapping individual molecules from molecular aggregates. Furthermore, the strong intermolecular forces within the COF pores significantly enhance the residence time of individual molecules, thereby increasing the probability of detecting single-molecule binding events. This innovative approach ensures consistent and reliable SERS single-molecule detection in complex mixtures, paving the way for advanced applications in biochemical sensing and diagnostics.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"5 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143608432","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 outbreak and continued spread of coronavirus disease 2019 (COVID-19) have significantly threatened public health. Antibody testing is essential for infection diagnosis, seroepidemiological analysis, and vaccine evaluation. However, achieving convenient, fast, and accurate detection remains challenging in this prolonged battle. This study reports a highly sensitive severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) spike protein detection platform based on organic electrochemical transistors (OECTs) for biosensing applications. We developed a nanostructured poly(3,4-ethylenedioxythiophene) (PEDOT) conductive polymer with the carboxylic acid functional group (PEDOTAc) for modifying specific antibodies on an OECT channel for the detection of the COVID-19 spike protein. The OECT device features a channel composed of a PEDOT:polystyrenesulfonate (PEDOT:PSS) bottom layer, with the upper layer decorated with PEDOTAc nanorod arrays via the oxidative polymerization and a trans-printing method. Our novel PEDOTAc nanorod array-based OECT device exhibits promising potential for future healthcare and point-of-care sensing due to its rapid response, high sensitivity, and high accuracy. Through optimization, we achieved specific detection of the SARS-CoV-2 spike protein within minutes, with a detectable region from 10 fM to 100 nM. These biosensors hold significant promise for use in the diagnosis and prognosis of COVID-19.
{"title":"Poly(3,4-ethylenedioxythiophene) Nanorod Arrays-Based Organic Electrochemical Transistor for SARS-CoV-2 Spike Protein Detection in Artificial Saliva","authors":"Syed Atif Ali, Ying-Lin Chen, Hsueh-Sheng Tseng, Hailemichael Ayalew, Jia-Wei She, Bhaskarchand Gautam, Hsiung-Lin Tu, Yu-Sheng Hsiao, Hsiao-hua Yu","doi":"10.1021/acssensors.4c03207","DOIUrl":"https://doi.org/10.1021/acssensors.4c03207","url":null,"abstract":"The outbreak and continued spread of coronavirus disease 2019 (COVID-19) have significantly threatened public health. Antibody testing is essential for infection diagnosis, seroepidemiological analysis, and vaccine evaluation. However, achieving convenient, fast, and accurate detection remains challenging in this prolonged battle. This study reports a highly sensitive severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) spike protein detection platform based on organic electrochemical transistors (OECTs) for biosensing applications. We developed a nanostructured poly(3,4-ethylenedioxythiophene) (PEDOT) conductive polymer with the carboxylic acid functional group (PEDOTAc) for modifying specific antibodies on an OECT channel for the detection of the COVID-19 spike protein. The OECT device features a channel composed of a PEDOT:polystyrenesulfonate (PEDOT:PSS) bottom layer, with the upper layer decorated with PEDOTAc nanorod arrays via the oxidative polymerization and a trans-printing method. Our novel PEDOTAc nanorod array-based OECT device exhibits promising potential for future healthcare and point-of-care sensing due to its rapid response, high sensitivity, and high accuracy. Through optimization, we achieved specific detection of the SARS-CoV-2 spike protein within minutes, with a detectable region from 10 fM to 100 nM. These biosensors hold significant promise for use in the diagnosis and prognosis of COVID-19.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"4 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143619046","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}
How to modulate the molecular structure to finely manipulate the sensing performance is of great significance for propelling the oriented design of the optical sensing probe. Here, by taking the optical detection toward amphetamine (AMP) as a model, a structural regulation strategy for the D-π-A probe was proposed to manipulate the reaction activity and optical response. The optimal probe was screened out from a series of D-π-A molecules with an electrophilic site owing to its faster response and more remarkable emission shift, as well as the desirable specificity. In particular, it was found that the probe reactivity induced two trade-off effects. First, it is kinetically expressed by the reaction time that greatly affects the sensitivity (emission shift), and second, it thermodynamically determines the specificity. Upon fine modulation, the optimal probe in the solid state integrated in a portable sensing chip was demonstrated with fast and visualized analysis for AMP in complicated scenarios. Overall, the proposed structure–performance correlation and the mediation on the trade-off effect would provide an in-depth insight for the oriented design of an optical sensor with a desirable sensing performance.
{"title":"Highly Sensitive, Specific, and Fast Fluorescent Sensing of Amphetamine via Structural Regulation","authors":"Sifan Cao, Yuan Liu*, Yanan Guo, Baiyi Zu, Fei Yan, Dong-Sheng Guo* and Xincun Dou*, ","doi":"10.1021/acssensors.4c0319810.1021/acssensors.4c03198","DOIUrl":"https://doi.org/10.1021/acssensors.4c03198https://doi.org/10.1021/acssensors.4c03198","url":null,"abstract":"<p >How to modulate the molecular structure to finely manipulate the sensing performance is of great significance for propelling the oriented design of the optical sensing probe. Here, by taking the optical detection toward amphetamine (AMP) as a model, a structural regulation strategy for the D-π-A probe was proposed to manipulate the reaction activity and optical response. The optimal probe was screened out from a series of D-π-A molecules with an electrophilic site owing to its faster response and more remarkable emission shift, as well as the desirable specificity. In particular, it was found that the probe reactivity induced two trade-off effects. First, it is kinetically expressed by the reaction time that greatly affects the sensitivity (emission shift), and second, it thermodynamically determines the specificity. Upon fine modulation, the optimal probe in the solid state integrated in a portable sensing chip was demonstrated with fast and visualized analysis for AMP in complicated scenarios. Overall, the proposed structure–performance correlation and the mediation on the trade-off effect would provide an in-depth insight for the oriented design of an optical sensor with a desirable sensing performance.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"10 3","pages":"1998–2006 1998–2006"},"PeriodicalIF":8.2,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143714045","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 : 2025-03-13DOI: 10.1021/acssensors.4c0306910.1021/acssensors.4c03069
Jihang Liu*, Doris Keh Ting Ng, Yul Koh, Subhranu Samanta, Weiguo Chen, Md Hazwani Khairy Md Husni, Merugu Srinivas, Qingxin Zhang, Fuu Ming Kai, Peter Hyun Kee Chang and Yao Zhu*,
Highly sensitive, selective, and compact hydrogen (H2) sensors for safety and process monitoring are needed due to the growing adoption of H2 as a clean energy carrier. Current resonant frequency-based H2 sensors face a critical challenge in simultaneously achieving high sensitivity, low operating frequency, and miniaturization while maintaining a high figure of merit (FOM). This study addresses these challenges by introducing a novel piezoelectric micro diagram (PMD) H2 sensor that achieves an unprecedented FOM exceeding 104. The sensor uniquely integrates a PMD resonator with a palladium (Pd) sensing layer, operating on a stress-based mechanism distinct from traditional mass-loading principles. Despite a low operating frequency of 150 kHz, the sensor demonstrates a remarkable sensitivity of 18.5 kHz/% H2. Comprehensive characterization also reveals a minimal cross-sensitivity to humidity and common gases and a compact form factor (600 μm lateral length) suitable for IC integration. The sensor’s performance was systematically evaluated across various Pd thicknesses (40–125 nm) and piezoelectric stack covering ratios (50% and 70%), revealing a trade-off between sensitivity and response time. This PMD H2 sensor represents a significant advancement in resonant frequency-based H2 sensing, offering superior sensitivity, compact size, and robust performance for diverse applications in H2 detection and monitoring.
{"title":"High-Performance Piezoelectric Micro Diaphragm Hydrogen Sensor","authors":"Jihang Liu*, Doris Keh Ting Ng, Yul Koh, Subhranu Samanta, Weiguo Chen, Md Hazwani Khairy Md Husni, Merugu Srinivas, Qingxin Zhang, Fuu Ming Kai, Peter Hyun Kee Chang and Yao Zhu*, ","doi":"10.1021/acssensors.4c0306910.1021/acssensors.4c03069","DOIUrl":"https://doi.org/10.1021/acssensors.4c03069https://doi.org/10.1021/acssensors.4c03069","url":null,"abstract":"<p >Highly sensitive, selective, and compact hydrogen (H<sub>2</sub>) sensors for safety and process monitoring are needed due to the growing adoption of H<sub>2</sub> as a clean energy carrier. Current resonant frequency-based H<sub>2</sub> sensors face a critical challenge in simultaneously achieving high sensitivity, low operating frequency, and miniaturization while maintaining a high figure of merit (FOM). This study addresses these challenges by introducing a novel piezoelectric micro diagram (PMD) H<sub>2</sub> sensor that achieves an unprecedented FOM exceeding 10<sup>4</sup>. The sensor uniquely integrates a PMD resonator with a palladium (Pd) sensing layer, operating on a stress-based mechanism distinct from traditional mass-loading principles. Despite a low operating frequency of 150 kHz, the sensor demonstrates a remarkable sensitivity of 18.5 kHz/% H<sub>2</sub>. Comprehensive characterization also reveals a minimal cross-sensitivity to humidity and common gases and a compact form factor (600 μm lateral length) suitable for IC integration. The sensor’s performance was systematically evaluated across various Pd thicknesses (40–125 nm) and piezoelectric stack covering ratios (50% and 70%), revealing a trade-off between sensitivity and response time. This PMD H<sub>2</sub> sensor represents a significant advancement in resonant frequency-based H<sub>2</sub> sensing, offering superior sensitivity, compact size, and robust performance for diverse applications in H<sub>2</sub> detection and monitoring.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"10 3","pages":"1922–1929 1922–1929"},"PeriodicalIF":8.2,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acssensors.4c03069","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143714091","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
How to modulate the molecular structure to finely manipulate the sensing performance is of great significance for propelling the oriented design of the optical sensing probe. Here, by taking the optical detection toward amphetamine (AMP) as a model, a structural regulation strategy for the D-π-A probe was proposed to manipulate the reaction activity and optical response. The optimal probe was screened out from a series of D-π-A molecules with an electrophilic site owing to its faster response and more remarkable emission shift, as well as the desirable specificity. In particular, it was found that the probe reactivity induced two trade-off effects. First, it is kinetically expressed by the reaction time that greatly affects the sensitivity (emission shift), and second, it thermodynamically determines the specificity. Upon fine modulation, the optimal probe in the solid state integrated in a portable sensing chip was demonstrated with fast and visualized analysis for AMP in complicated scenarios. Overall, the proposed structure–performance correlation and the mediation on the trade-off effect would provide an in-depth insight for the oriented design of an optical sensor with a desirable sensing performance.
{"title":"Highly Sensitive, Specific, and Fast Fluorescent Sensing of Amphetamine via Structural Regulation","authors":"Sifan Cao, Yuan Liu, Yanan Guo, Baiyi Zu, Fei Yan, Dong-Sheng Guo, Xincun Dou","doi":"10.1021/acssensors.4c03198","DOIUrl":"https://doi.org/10.1021/acssensors.4c03198","url":null,"abstract":"How to modulate the molecular structure to finely manipulate the sensing performance is of great significance for propelling the oriented design of the optical sensing probe. Here, by taking the optical detection toward amphetamine (AMP) as a model, a structural regulation strategy for the D-π-A probe was proposed to manipulate the reaction activity and optical response. The optimal probe was screened out from a series of D-π-A molecules with an electrophilic site owing to its faster response and more remarkable emission shift, as well as the desirable specificity. In particular, it was found that the probe reactivity induced two trade-off effects. First, it is kinetically expressed by the reaction time that greatly affects the sensitivity (emission shift), and second, it thermodynamically determines the specificity. Upon fine modulation, the optimal probe in the solid state integrated in a portable sensing chip was demonstrated with fast and visualized analysis for AMP in complicated scenarios. Overall, the proposed structure–performance correlation and the mediation on the trade-off effect would provide an in-depth insight for the oriented design of an optical sensor with a desirable sensing performance.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"183 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143619047","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}
Surface-enhanced Raman scattering (SERS) offers significant advantages for single-molecule detection. However, stochastic molecular motion makes it challenging to consistently capture signals from single-molecule binding events, particularly in complex environments. Herein, we propose a novel SERS system via the pore nanoconfinement effect of covalent organic frameworks (COFs) to achieve reliable single-molecule detection. The self-assembled COF thin films on SERS metal substrates (Au/Ag) create a nanogap of 3 nm, allowing electric field enhancement. By precise tuning of the COF shell thickness, a molecular-scale pore volume is formed, effectively trapping individual molecules from molecular aggregates. Furthermore, the strong intermolecular forces within the COF pores significantly enhance the residence time of individual molecules, thereby increasing the probability of detecting single-molecule binding events. This innovative approach ensures consistent and reliable SERS single-molecule detection in complex mixtures, paving the way for advanced applications in biochemical sensing and diagnostics.
{"title":"Single-Molecule Detection via Pore Nanoconfinement of Covalent Organic Frameworks for Surface-Enhanced Raman Scattering","authors":"Mengya Lv, Xiao Wu, Wen Wang, Dandan Han, Sheng Chen, Yifan Hu, Qidong Zhang, Qiyan Wang* and Ronghan Wei, ","doi":"10.1021/acssensors.4c0239110.1021/acssensors.4c02391","DOIUrl":"https://doi.org/10.1021/acssensors.4c02391https://doi.org/10.1021/acssensors.4c02391","url":null,"abstract":"<p >Surface-enhanced Raman scattering (SERS) offers significant advantages for single-molecule detection. However, stochastic molecular motion makes it challenging to consistently capture signals from single-molecule binding events, particularly in complex environments. Herein, we propose a novel SERS system via the pore nanoconfinement effect of covalent organic frameworks (COFs) to achieve reliable single-molecule detection. The self-assembled COF thin films on SERS metal substrates (Au/Ag) create a nanogap of 3 nm, allowing electric field enhancement. By precise tuning of the COF shell thickness, a molecular-scale pore volume is formed, effectively trapping individual molecules from molecular aggregates. Furthermore, the strong intermolecular forces within the COF pores significantly enhance the residence time of individual molecules, thereby increasing the probability of detecting single-molecule binding events. This innovative approach ensures consistent and reliable SERS single-molecule detection in complex mixtures, paving the way for advanced applications in biochemical sensing and diagnostics.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"10 3","pages":"1778–1787 1778–1787"},"PeriodicalIF":8.2,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143714042","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 : 2025-03-13DOI: 10.1021/acssensors.4c03069
Jihang Liu, Doris Keh Ting Ng, Yul Koh, Subhranu Samanta, Weiguo Chen, Md Hazwani Khairy Md Husni, Merugu Srinivas, Qingxin Zhang, Fuu Ming Kai, Peter Hyun Kee Chang, Yao Zhu
Highly sensitive, selective, and compact hydrogen (H2) sensors for safety and process monitoring are needed due to the growing adoption of H2 as a clean energy carrier. Current resonant frequency-based H2 sensors face a critical challenge in simultaneously achieving high sensitivity, low operating frequency, and miniaturization while maintaining a high figure of merit (FOM). This study addresses these challenges by introducing a novel piezoelectric micro diagram (PMD) H2 sensor that achieves an unprecedented FOM exceeding 104. The sensor uniquely integrates a PMD resonator with a palladium (Pd) sensing layer, operating on a stress-based mechanism distinct from traditional mass-loading principles. Despite a low operating frequency of 150 kHz, the sensor demonstrates a remarkable sensitivity of 18.5 kHz/% H2. Comprehensive characterization also reveals a minimal cross-sensitivity to humidity and common gases and a compact form factor (600 μm lateral length) suitable for IC integration. The sensor’s performance was systematically evaluated across various Pd thicknesses (40–125 nm) and piezoelectric stack covering ratios (50% and 70%), revealing a trade-off between sensitivity and response time. This PMD H2 sensor represents a significant advancement in resonant frequency-based H2 sensing, offering superior sensitivity, compact size, and robust performance for diverse applications in H2 detection and monitoring.
{"title":"High-Performance Piezoelectric Micro Diaphragm Hydrogen Sensor","authors":"Jihang Liu, Doris Keh Ting Ng, Yul Koh, Subhranu Samanta, Weiguo Chen, Md Hazwani Khairy Md Husni, Merugu Srinivas, Qingxin Zhang, Fuu Ming Kai, Peter Hyun Kee Chang, Yao Zhu","doi":"10.1021/acssensors.4c03069","DOIUrl":"https://doi.org/10.1021/acssensors.4c03069","url":null,"abstract":"Highly sensitive, selective, and compact hydrogen (H<sub>2</sub>) sensors for safety and process monitoring are needed due to the growing adoption of H<sub>2</sub> as a clean energy carrier. Current resonant frequency-based H<sub>2</sub> sensors face a critical challenge in simultaneously achieving high sensitivity, low operating frequency, and miniaturization while maintaining a high figure of merit (FOM). This study addresses these challenges by introducing a novel piezoelectric micro diagram (PMD) H<sub>2</sub> sensor that achieves an unprecedented FOM exceeding 10<sup>4</sup>. The sensor uniquely integrates a PMD resonator with a palladium (Pd) sensing layer, operating on a stress-based mechanism distinct from traditional mass-loading principles. Despite a low operating frequency of 150 kHz, the sensor demonstrates a remarkable sensitivity of 18.5 kHz/% H<sub>2</sub>. Comprehensive characterization also reveals a minimal cross-sensitivity to humidity and common gases and a compact form factor (600 μm lateral length) suitable for IC integration. The sensor’s performance was systematically evaluated across various Pd thicknesses (40–125 nm) and piezoelectric stack covering ratios (50% and 70%), revealing a trade-off between sensitivity and response time. This PMD H<sub>2</sub> sensor represents a significant advancement in resonant frequency-based H<sub>2</sub> sensing, offering superior sensitivity, compact size, and robust performance for diverse applications in H<sub>2</sub> detection and monitoring.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"16 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143619026","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}