Pub Date : 2025-03-05DOI: 10.1021/acssensors.4c03572
Zhenjin Xu, Wei Xiao, Keqi Deng, Yang Zhang, Tingting Shen, Xin Liu, Zhengmao Ding, Qiulin Tan, Dezhi Wu
Growing imperative for intelligent transformation of electro-ionic actuators in soft robotics has necessitated self-perception for accurately mapping their nonlinear dynamic responses. Despite the promise of integrating crack-based strain sensors for such a purpose, significant challenges remain in controlling crack propagation to prevent the induction of through-cracks, resulting in lower sensitivity, linearity, and poor detection limits. Herein, we propose a hierarchical crack-based synergistic enhancement structure by incorporating conductive poly(pyrrole)-coated polystyrene nanospheres and Ti3C2Tx MXene to induce cross-long sensing cracks via point-to-plane contacts, along with silver nanowires for positively engineering networked microcracks for linearity tuning. The prepared microstrain sensor achieves high linearity (GF = 152.4, R2 = 0.99) regulation within ∼6% strain range, ultralow detection limit of 0.02%, and ultrafast response/recovery time of 31 ms/32 ms under 0.2%. Notably, state-of-the-art sensing performance by detecting minimal strain changes down to one millionth, i.e., ∼1 microstrain, has been demonstrated by voiceprint recognition, while maintaining superior dynamic measurement capability and long-term stability for mechanical vibrations up to 100 Hz with a response time of 5 ms. Moreover, the introduction of an adhesive and cross-linking layer facilitates robust bonding between the actuator and sensing structure, enabling real-time tracking of the actuation strain without structural interference by a resistance change resolution of 0.01%, providing significant insights for empowering soft robotics with integrated perception and intelligence.
{"title":"Hierarchical Crack Engineering-Enabled High-Linearity and Ultrasensitive Strain Sensors","authors":"Zhenjin Xu, Wei Xiao, Keqi Deng, Yang Zhang, Tingting Shen, Xin Liu, Zhengmao Ding, Qiulin Tan, Dezhi Wu","doi":"10.1021/acssensors.4c03572","DOIUrl":"https://doi.org/10.1021/acssensors.4c03572","url":null,"abstract":"Growing imperative for intelligent transformation of electro-ionic actuators in soft robotics has necessitated self-perception for accurately mapping their nonlinear dynamic responses. Despite the promise of integrating crack-based strain sensors for such a purpose, significant challenges remain in controlling crack propagation to prevent the induction of through-cracks, resulting in lower sensitivity, linearity, and poor detection limits. Herein, we propose a hierarchical crack-based synergistic enhancement structure by incorporating conductive poly(pyrrole)-coated polystyrene nanospheres and Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub> MXene to induce cross-long sensing cracks via point-to-plane contacts, along with silver nanowires for positively engineering networked microcracks for linearity tuning. The prepared microstrain sensor achieves high linearity (GF = 152.4, <i>R</i><sup>2</sup> = 0.99) regulation within ∼6% strain range, ultralow detection limit of 0.02%, and ultrafast response/recovery time of 31 ms/32 ms under 0.2%. Notably, state-of-the-art sensing performance by detecting minimal strain changes down to one millionth, i.e., ∼1 microstrain, has been demonstrated by voiceprint recognition, while maintaining superior dynamic measurement capability and long-term stability for mechanical vibrations up to 100 Hz with a response time of 5 ms. Moreover, the introduction of an adhesive and cross-linking layer facilitates robust bonding between the actuator and sensing structure, enabling real-time tracking of the actuation strain without structural interference by a resistance change resolution of 0.01%, providing significant insights for empowering soft robotics with integrated perception and intelligence.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"36 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143561032","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}
Engrailed-2 (EN2) protein, a transcription factor in the homologous domain expressed in prostate cancer (PCa) cells and secreted into the urine, is considered a promising biomarker for noninvasive detection of PCa. EN2 protein in urine samples can be obtained by noninvasive means, but the low biomarker concentration in urine samples poses a great challenge for noninvasive detection of the PCa biomarker. Herein, we develop a solution-gated graphene transistor (SGGT) biosensor to detect the biomarker of the EN2 protein for PCa diagnosis. The aptamer probes are immobilized to the gold gate electrode through Au–S bonds. The effect of aptamer configurations on the biosensor’s responses is also investigated. It can be found that the SGGT biosensor with the long-chain probes with a stem-like loop structure exhibits optimal performance. The limit of detection of biosensors can reach 0.1 fg/mL, and a rapid response time of 19 min is achieved. The SGGT biosensor also exhibits high specificity for the EN2 protein. More importantly, testing of clinical urine samples indicates that our sensor can distinguish PCa patients from non-PCa subjects. Compared to traditional hospital prostate-specific antigen tests, our sensor exhibits better accuracy for the noninvasive diagnosis of PCa.
{"title":"Highly Sensitive Detection of Engrailed-2 Protein Biomarker in Urine for Using Solution-Gated Graphene Transistor Diagnosis of Prostate Cancer","authors":"Junqi Dong, Huan Yang, Peng Song, Tingting Yu, Zexun Pan, Ziwen Chen, Ruixue Wang, Minghua Deng, Xianbao Wang, Jinhua Li","doi":"10.1021/acssensors.4c03320","DOIUrl":"https://doi.org/10.1021/acssensors.4c03320","url":null,"abstract":"Engrailed-2 (EN2) protein, a transcription factor in the homologous domain expressed in prostate cancer (PCa) cells and secreted into the urine, is considered a promising biomarker for noninvasive detection of PCa. EN2 protein in urine samples can be obtained by noninvasive means, but the low biomarker concentration in urine samples poses a great challenge for noninvasive detection of the PCa biomarker. Herein, we develop a solution-gated graphene transistor (SGGT) biosensor to detect the biomarker of the EN2 protein for PCa diagnosis. The aptamer probes are immobilized to the gold gate electrode through Au–S bonds. The effect of aptamer configurations on the biosensor’s responses is also investigated. It can be found that the SGGT biosensor with the long-chain probes with a stem-like loop structure exhibits optimal performance. The limit of detection of biosensors can reach 0.1 fg/mL, and a rapid response time of 19 min is achieved. The SGGT biosensor also exhibits high specificity for the EN2 protein. More importantly, testing of clinical urine samples indicates that our sensor can distinguish PCa patients from non-PCa subjects. Compared to traditional hospital prostate-specific antigen tests, our sensor exhibits better accuracy for the noninvasive diagnosis of PCa.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"16 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546780","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}
Diabetic kidney disease (DKD) is a leading cause of death among diabetic patients, primarily due to ectopic lipid accumulation in nonadipose tissues. The lack of molecular tools for quantitatively visualizing this lipid accumulation has hindered in-depth studies. This study aims to develop a dual-emissive up-conversion fluorescent probe, DSDM, for precise in vivo and ex vivo analyses of lipid accumulation. DSDM exhibits up-conversion green emission and down-conversion near-infrared (NIR) fluorescence when excited at 561 nm. This allows for the simultaneous imaging of lipid droplets (LDs) and the endoplasmic reticulum (ER), the primary sites for lipid synthesis and storage. With intracellular lipid consumption and accumulation, the green emission in LDs decreased or increased, while the NIR fluorescence in the ER remained constant. Using the NIR emission as an internal control, the green-to-NIR emission intensity ratio can quantify the LD amount accurately, overcoming the possible interferences from inhomogeneous staining, variation in cell population, and other factors. With the probe, we quantitatively analyzed LD accumulation in human kidney cells with either overexpressed or silenced aquaporin 7 (AQP7), induced by palmitic acid. Herein, AQP7 is specifically expressed in kidney tubules and is the only channel that regulates adipose glycerol transport. In DKD mice with kidney-specific AQP7 knockout, the probe successfully detected up-regulated lipid accumulation and ER stress. Tissue imaging revealed that the inhibited close contact between LDs and ER might facilitate the assessment of lipid accumulation in DKD. This approach effectively addresses the limitations of precise tissue biopsy in DKD, thereby improving DKD management.
{"title":"Novel Dual-Emissive Up-conversion Fluorescent Probe for Imaging Ectopic Lipid Accumulation in Diabetes Mellitus","authors":"Zheming Zhang, Zhiyuan Wang, Mengfan Kan, Minggang Tian, Zhongwen Zhang","doi":"10.1021/acssensors.4c03149","DOIUrl":"https://doi.org/10.1021/acssensors.4c03149","url":null,"abstract":"Diabetic kidney disease (DKD) is a leading cause of death among diabetic patients, primarily due to ectopic lipid accumulation in nonadipose tissues. The lack of molecular tools for quantitatively visualizing this lipid accumulation has hindered in-depth studies. This study aims to develop a dual-emissive up-conversion fluorescent probe, DSDM, for precise in vivo and ex vivo analyses of lipid accumulation. DSDM exhibits up-conversion green emission and down-conversion near-infrared (NIR) fluorescence when excited at 561 nm. This allows for the simultaneous imaging of lipid droplets (LDs) and the endoplasmic reticulum (ER), the primary sites for lipid synthesis and storage. With intracellular lipid consumption and accumulation, the green emission in LDs decreased or increased, while the NIR fluorescence in the ER remained constant. Using the NIR emission as an internal control, the green-to-NIR emission intensity ratio can quantify the LD amount accurately, overcoming the possible interferences from inhomogeneous staining, variation in cell population, and other factors. With the probe, we quantitatively analyzed LD accumulation in human kidney cells with either overexpressed or silenced aquaporin 7 (AQP7), induced by palmitic acid. Herein, AQP7 is specifically expressed in kidney tubules and is the only channel that regulates adipose glycerol transport. In DKD mice with kidney-specific AQP7 knockout, the probe successfully detected up-regulated lipid accumulation and ER stress. Tissue imaging revealed that the inhibited close contact between LDs and ER might facilitate the assessment of lipid accumulation in DKD. This approach effectively addresses the limitations of precise tissue biopsy in DKD, thereby improving DKD management.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"28 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546671","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 : 2025-03-04DOI: 10.1021/acssensors.4c03408
Yiwei Li, Shibo Song, Jin Song, Rui Gong, Ghulam Abbas
Nonhealing chronic wounds pose severe physiological and psychological distress to patients, making them a significant concern for global public health. Effective wound management strategies assisted by smart wearable pH monitoring have the potential to substantially alleviate both social and economic burdens. The pH of the wound exudate serves as a valuable indicator for predicting infections and assessing the healing status of wounds. This review comprehensively summarizes fundamental aspects related to wound pH, with a particular emphasis on the relationships between pH and healing status, infections, and other biochemical parameters that are crucial for wound health. It systematically discusses advancements in electrochemical pH sensors specifically designed for wearable devices, emphasizing their core performance in the care of chronic wounds. Additionally, the review outlines the challenges faced by this field and suggests future directions for research and development.
{"title":"Electrochemical pH Sensor Incorporated Wearables for State-of-the-Art Wound Care","authors":"Yiwei Li, Shibo Song, Jin Song, Rui Gong, Ghulam Abbas","doi":"10.1021/acssensors.4c03408","DOIUrl":"https://doi.org/10.1021/acssensors.4c03408","url":null,"abstract":"Nonhealing chronic wounds pose severe physiological and psychological distress to patients, making them a significant concern for global public health. Effective wound management strategies assisted by smart wearable pH monitoring have the potential to substantially alleviate both social and economic burdens. The pH of the wound exudate serves as a valuable indicator for predicting infections and assessing the healing status of wounds. This review comprehensively summarizes fundamental aspects related to wound pH, with a particular emphasis on the relationships between pH and healing status, infections, and other biochemical parameters that are crucial for wound health. It systematically discusses advancements in electrochemical pH sensors specifically designed for wearable devices, emphasizing their core performance in the care of chronic wounds. Additionally, the review outlines the challenges faced by this field and suggests future directions for research and development.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"30 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546781","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}
Recently, flexible electronics have significantly transformed information and communications technology (ICT). In particular, wearable devices, via integration with attachable biosensors, have driven the development of new types of biosensors and diagnostic devices for point-of-care testing (POCT). Moreover, wearable electrochemical biosensors can be applied to diagnose diseases in real time based on the synergistic effect generated from the incorporation of the electrochemical technique. Besides, to improve the sensitivity of electrochemical biosensors while retaining their wearability, novel nanomaterials and nanotechnologies have been introduced. In this review, recent studies on nanotechnology-based wearable electrochemical biosensors for accurate disease diagnosis are discussed. First, widely used techniques for developing flexible electrodes, including nanolithography- and nano/microneedle-based patches, are presented. Next, the latest studies on developing wearable electrochemical biosensors for the diagnosis of diseases such as diabetes and dermatitis are discussed by categorizing the biosensors into nanolithography- and nano/microneedle-based categories. Finally, this review explores the latest research trends on the application of nanotechnology-enabled nanopatterning and nano/microneedle technologies to electrochemical wearable biosensors. This review suggests novel approaches and methods for developing wearable electrochemical biosensors for real-time disease diagnosis under POCT applications.
{"title":"Nanotechnology-Based Wearable Electrochemical Biosensor for Disease Diagnosis","authors":"Jinho Yoon, Nayeon Kwon, Yejin Lee, Seewoo Kim, Taek Lee, Jeong-Woo Choi","doi":"10.1021/acssensors.4c03371","DOIUrl":"https://doi.org/10.1021/acssensors.4c03371","url":null,"abstract":"Recently, flexible electronics have significantly transformed information and communications technology (ICT). In particular, wearable devices, via integration with attachable biosensors, have driven the development of new types of biosensors and diagnostic devices for point-of-care testing (POCT). Moreover, wearable electrochemical biosensors can be applied to diagnose diseases in real time based on the synergistic effect generated from the incorporation of the electrochemical technique. Besides, to improve the sensitivity of electrochemical biosensors while retaining their wearability, novel nanomaterials and nanotechnologies have been introduced. In this review, recent studies on nanotechnology-based wearable electrochemical biosensors for accurate disease diagnosis are discussed. First, widely used techniques for developing flexible electrodes, including nanolithography- and nano/microneedle-based patches, are presented. Next, the latest studies on developing wearable electrochemical biosensors for the diagnosis of diseases such as diabetes and dermatitis are discussed by categorizing the biosensors into nanolithography- and nano/microneedle-based categories. Finally, this review explores the latest research trends on the application of nanotechnology-enabled nanopatterning and nano/microneedle technologies to electrochemical wearable biosensors. This review suggests novel approaches and methods for developing wearable electrochemical biosensors for real-time disease diagnosis under POCT applications.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"23 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539009","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 : 2025-03-03DOI: 10.1021/acssensors.4c03532
Menglong Li, Wen Ye, Juanzhang Ruan, Qiuyuan Ren, Shihong Dong, Dongyun Chen, Najun Li, Qingfeng Xu, Hua Li, Jianmei Lu
Hydrogen sulfide (H2S) is an important respiratory biomarker of many diseases, and thus, developing H2S gas sensors with low detection limits at low operating temperatures is essential for the early diagnosis of diseases in low-resource environments. Although lead halide perovskites have unique electronic and optical properties, the high toxicity of lead has prompted the development of alternative materials. In this study, Cs2AgBiCl6 was synthesized using a simple method. The sensor based on Cs2AgBiCl6 showed excellent sensing of H2S gas at room temperature over a wide humidity range, with high response (90.6 vs 10 ppm of H2S) and fast response speed (99.6 s vs 400 ppb H2S). The detection limit was low (5 ppb H2S), and the selectivity at room temperature was excellent. Small changes in H2S concentration (<100 ppb) were detected as a fully reversible resistance signal. Additionally, sum frequency vibration spectroscopy and DFT calculations showed that the high gas sensitivity was attributed to the physical adsorption of H2S at Cl vacancies on the surface of Cs2AgBiCl6, as well as efficient charge transfer. This work provides an avenue for developing high-performance gas sensors based on nontoxic, wide band gap, halide double perovskite semiconductors operating at room temperature.
{"title":"Lead-Free Halide Double Perovskite Cs2AgBiCl6 for H2S Trace Detection at Room Temperature","authors":"Menglong Li, Wen Ye, Juanzhang Ruan, Qiuyuan Ren, Shihong Dong, Dongyun Chen, Najun Li, Qingfeng Xu, Hua Li, Jianmei Lu","doi":"10.1021/acssensors.4c03532","DOIUrl":"https://doi.org/10.1021/acssensors.4c03532","url":null,"abstract":"Hydrogen sulfide (H<sub>2</sub>S) is an important respiratory biomarker of many diseases, and thus, developing H<sub>2</sub>S gas sensors with low detection limits at low operating temperatures is essential for the early diagnosis of diseases in low-resource environments. Although lead halide perovskites have unique electronic and optical properties, the high toxicity of lead has prompted the development of alternative materials. In this study, Cs<sub>2</sub>AgBiCl<sub>6</sub> was synthesized using a simple method. The sensor based on Cs<sub>2</sub>AgBiCl<sub>6</sub> showed excellent sensing of H<sub>2</sub>S gas at room temperature over a wide humidity range, with high response (90.6 vs 10 ppm of H<sub>2</sub>S) and fast response speed (99.6 s vs 400 ppb H<sub>2</sub>S). The detection limit was low (5 ppb H<sub>2</sub>S), and the selectivity at room temperature was excellent. Small changes in H<sub>2</sub>S concentration (<100 ppb) were detected as a fully reversible resistance signal. Additionally, sum frequency vibration spectroscopy and DFT calculations showed that the high gas sensitivity was attributed to the physical adsorption of H<sub>2</sub>S at Cl vacancies on the surface of Cs<sub>2</sub>AgBiCl<sub>6</sub>, as well as efficient charge transfer. This work provides an avenue for developing high-performance gas sensors based on nontoxic, wide band gap, halide double perovskite semiconductors operating at room temperature.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"49 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539166","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 : 2025-03-03DOI: 10.1021/acssensors.4c03642
Xiaotian Wang, Yaoyao Zhou, Xiufang Li, Mei Zou, Qiang Zhang, Weilin Xu, Yanfei Feng, Yingying Zhang, Renchuan You
Hydrogels with a combination of mechanical flexibility and good electrical conductivity hold significant potential for various applications. Nonetheless, it is inevitable that water-based conductive hydrogels lose their elasticity and conductivity at extremely low temperatures, severely limiting their utilization in ultralow temperature environments, such as those for Arctic/Antarctic exploration. In this study, we developed a conductive hydrogel based on a double network cross-linking strategy that incorporated silk fibroin (SF) and poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) within a lithium bromide (LiBr) solution, which shows exceptional antifreezing (−108 °C freezing point) and excellent conductivity (16.33 S m–1). The obtained SF/PEDOT:PSS/LiBr (SPL) hydrogel shows a stable and reliable response to a wide range of deformations (compression: 0.5–60%; tensile: 1.0–100%), with a short response/recovery time of approximately 70 ms. More importantly, the hydrogel displays well-maintained conductivity, robust mechanical properties, and dependable sensing capabilities, even under temperatures as low as −80 °C. For proof of concept, we demonstrated the applications of the SPL hydrogel in detecting body movements, monitoring climate conditions, and ensuring information security in ultralow temperature environments. The results indicate that the antifreezing hydrogel is a promising candidate for fabricating flexible sensors, particularly well-suited for use in challenging ultralow temperature scenarios.
{"title":"Silk Fibroin-Based Antifreezing and Highly Conductive Hydrogel for Sensing at Ultralow Temperature","authors":"Xiaotian Wang, Yaoyao Zhou, Xiufang Li, Mei Zou, Qiang Zhang, Weilin Xu, Yanfei Feng, Yingying Zhang, Renchuan You","doi":"10.1021/acssensors.4c03642","DOIUrl":"https://doi.org/10.1021/acssensors.4c03642","url":null,"abstract":"Hydrogels with a combination of mechanical flexibility and good electrical conductivity hold significant potential for various applications. Nonetheless, it is inevitable that water-based conductive hydrogels lose their elasticity and conductivity at extremely low temperatures, severely limiting their utilization in ultralow temperature environments, such as those for Arctic/Antarctic exploration. In this study, we developed a conductive hydrogel based on a double network cross-linking strategy that incorporated silk fibroin (SF) and poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) within a lithium bromide (LiBr) solution, which shows exceptional antifreezing (−108 °C freezing point) and excellent conductivity (16.33 S m<sup>–1</sup>). The obtained SF/PEDOT:PSS/LiBr (SPL) hydrogel shows a stable and reliable response to a wide range of deformations (compression: 0.5–60%; tensile: 1.0–100%), with a short response/recovery time of approximately 70 ms. More importantly, the hydrogel displays well-maintained conductivity, robust mechanical properties, and dependable sensing capabilities, even under temperatures as low as −80 °C. For proof of concept, we demonstrated the applications of the SPL hydrogel in detecting body movements, monitoring climate conditions, and ensuring information security in ultralow temperature environments. The results indicate that the antifreezing hydrogel is a promising candidate for fabricating flexible sensors, particularly well-suited for use in challenging ultralow temperature scenarios.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"2 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539167","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 : 2025-03-03DOI: 10.1021/acssensors.4c03085
Shaofeng Shao, Liangwei Yan, Jiale Li, Yizhou Zhang, Jun Zhang, Hyoun Woo Kim, Sang Sub Kim
Gas sensing materials based on transition metal perovskite oxides (TMPOs) have garnered extensive attention across various fields such as air quality control, environmental monitoring, healthcare, and national defense security. To overcome challenges encountered in traditional research, a deep learning framework combining natural language processing technology (Word2Vec) and crystal graph convolutional neural network (CGCNN) was adopted in this study, proposing a predictive method that incorporates a comprehensive data set consisting of 1.2 million literature abstracts and 110,000 crystal structure data entries. This method assessed the optimal combination of zinc–cobalt bimetallic ions complexed with ligands as precursors for perovskite oxides. The regulatory function of ligand concentration on the p-n transformation of zinc–cobalt oxide sensing performance was identified, and optimization strategies were provided. The Zn(II)/Co(III)/1-methyl-1H-imidazole-2-carboxylic acid complex was synthesized and demonstrated exceptional sensitivity and selectivity toward volatile organic compounds (VOCs), particularly 3-hydroxy-2-butanone (3H-2B). The p-n transformation mechanism of sensing performance was deeply analyzed through the construction of the hyper-synergistic ligand interaction matrix model for n-type sensors (HSLIM-n) and the parametrized surface-ligand resonance model for p-type sensors (PSLRM-p), enhancing the fundamental understanding of the sensing material properties. Even in highly interfering environments, the functionalized perovskite oxides exhibited outstanding sensitivity and selectivity toward 3H-2B gas, with a low detection limit of 25 parts per billion (ppb). This comprehensive research approach has facilitated the construction of a transfer learning-enhanced deep learning framework, which has shown high efficiency in predicting the performance and precise design of perovskite oxides, and its effectiveness was meticulously verified through detailed experimental validation.
{"title":"Harnessing Transfer Deep Learning Framework for the Investigation of Transition Metal Perovskite Oxides with Advanced p-n Transformation Sensing Performance","authors":"Shaofeng Shao, Liangwei Yan, Jiale Li, Yizhou Zhang, Jun Zhang, Hyoun Woo Kim, Sang Sub Kim","doi":"10.1021/acssensors.4c03085","DOIUrl":"https://doi.org/10.1021/acssensors.4c03085","url":null,"abstract":"Gas sensing materials based on transition metal perovskite oxides (TMPOs) have garnered extensive attention across various fields such as air quality control, environmental monitoring, healthcare, and national defense security. To overcome challenges encountered in traditional research, a deep learning framework combining natural language processing technology (Word2Vec) and crystal graph convolutional neural network (CGCNN) was adopted in this study, proposing a predictive method that incorporates a comprehensive data set consisting of 1.2 million literature abstracts and 110,000 crystal structure data entries. This method assessed the optimal combination of zinc–cobalt bimetallic ions complexed with ligands as precursors for perovskite oxides. The regulatory function of ligand concentration on the p-n transformation of zinc–cobalt oxide sensing performance was identified, and optimization strategies were provided. The Zn(II)/Co(III)/1-methyl-1<i>H</i>-imidazole-2-carboxylic acid complex was synthesized and demonstrated exceptional sensitivity and selectivity toward volatile organic compounds (VOCs), particularly 3-hydroxy-2-butanone (3H-2B). The p-n transformation mechanism of sensing performance was deeply analyzed through the construction of the hyper-synergistic ligand interaction matrix model for n-type sensors (HSLIM-n) and the parametrized surface-ligand resonance model for p-type sensors (PSLRM-p), enhancing the fundamental understanding of the sensing material properties. Even in highly interfering environments, the functionalized perovskite oxides exhibited outstanding sensitivity and selectivity toward 3H-2B gas, with a low detection limit of 25 parts per billion (ppb). This comprehensive research approach has facilitated the construction of a transfer learning-enhanced deep learning framework, which has shown high efficiency in predicting the performance and precise design of perovskite oxides, and its effectiveness was meticulously verified through detailed experimental validation.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"56 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539255","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}
Nitrogen dioxide (NO2) is considered to be a highly hazardous gas found in combustion engine exhaust, which causes several diseases at a young age. To detect NO2 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 (MoS2) sensor using low-pressure chemical vapor deposition on a SiO2/Si substrate. Doping is confirmed through various characterization techniques. As compared to pristine MoS2, three batches of sensors are prepared with different weight percentages of Nb (8, 16, and 24%). Out of these, the 16% Nb-MoS2 sensor gives a greatly enhanced relative response of ∼30% for 500 ppb NO2 at 100 °C with an LOD of 489 ppt. Also, the sensor gives an ultrahigh response of ∼39% (18%) for 50 ppm (500 ppb) NO2 under 0.4 mW/cm2 intensity of UV light and exhibits a lower LOD of 117 ppt at RT. In addition, the 16% Nb-MoS2 sensor shows impressive selectivity toward NO2 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 NO2 adsorption on 16% Nb-MoS2 nanoflakes. This study offers a compelling and practical approach to boosting the efficiency of Nb-MoS2-based NO2 gas sensors.
{"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}
Pub 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
Hydrogen (H2(g)) is a viable green fossil fuel alternative, as its combustion yields only water and energy. However, H2(g) 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 H2(g) 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)}2(thbpym)](Cl)2 (IrCp*, (Cp* = C5Me5–, thbpym = 4,4′,6,6′-tetrahydroxy-2,2′-bipyrimidine)) to engineer H2(g) gas selectivity with high sensitivity at room temperature and pressure. This system yields ∼47–fold fluorescence enhancement when exposed to H2(g) in aqueous solution or ∼2.4–fold in a carboxymethyl cellulose (CMC) hydrogel matrix, with an estimated detection limit of ∼0.5% H2(g) with no cross-reactivity observed for potentially contaminating gases such as nitrogen (N2(g)), oxygen (O2(g)), or air.
{"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}
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