An RCA product is a promising scaffold for the construction of DNA nanostructures, but so far, there is no RCA scaffold-based dynamic reconfigurable nanorobot for biological applications. In this contribution, we develop an intracellular stimuli-responsive reconfigurable coiled DNA nanosnake (N-Snake) by using incomplete aptamer-functionalized (A) DNA tetrahedrons (T) to fold a long tandemly repetitive DNA strand synthesized by rolling circle amplification reaction (R) with the help of palindromic fragment (P). A DNA-assembled product, ARTP, including spiked aptamers, can retain the structural integrity even if exposed to fetal bovine serum (FBS) for 24 h and displays substantially enhanced target molecule-dependent cellular internalization efficiency. ARTP contains tetrahedral containers and linear containers, so that there are 500 doxorubicins (DOXs) and 12.5 siRNAs per ARTP. Moreover, ARTP can precisely transport anticancer drugs to cancerous sites and controllably release via the structural reconfiguration upon intracellular stimuli, almost 100% inhibiting tumor growth without detectable systemic toxicity owing to the synergistic RNAi-/Chemotherapy. Apparently, coiled N-snake, DOX/siPlk1-loaded ARTP, can specifically enter tumor cells, uncoil upon intracellular stimuli, and attack the cells from the inside, exerting precise cancer therapy.
{"title":"Folding an RCA Scaffold into an Intelligent Coiled Nanosnake for Precise/Synergistic RNAi-/Chemotherapy of Cancer","authors":"Congcong Li, Wenqing Lin, Weijun Wang, Jingting Wu, Shasha Luo, Linhuan Chen, Rong Wu, Zhifa Shen, Zai-Sheng Wu","doi":"10.1021/acs.analchem.4c03437","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c03437","url":null,"abstract":"An RCA product is a promising scaffold for the construction of DNA nanostructures, but so far, there is no RCA scaffold-based dynamic reconfigurable nanorobot for biological applications. In this contribution, we develop an intracellular stimuli-responsive reconfigurable coiled DNA nanosnake (N-Snake) by using incomplete aptamer-functionalized (A) DNA tetrahedrons (T) to fold a long tandemly repetitive DNA strand synthesized by rolling circle amplification reaction (R) with the help of palindromic fragment (P). A DNA-assembled product, ARTP, including spiked aptamers, can retain the structural integrity even if exposed to fetal bovine serum (FBS) for 24 h and displays substantially enhanced target molecule-dependent cellular internalization efficiency. ARTP contains tetrahedral containers and linear containers, so that there are 500 doxorubicins (DOXs) and 12.5 siRNAs per ARTP. Moreover, ARTP can precisely transport anticancer drugs to cancerous sites and controllably release via the structural reconfiguration upon intracellular stimuli, almost 100% inhibiting tumor growth without detectable systemic toxicity owing to the synergistic RNAi-/Chemotherapy. Apparently, coiled N-snake, DOX/siPlk1-loaded ARTP, can specifically enter tumor cells, uncoil upon intracellular stimuli, and attack the cells from the inside, exerting precise cancer therapy.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"16 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142940545","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 : 2025-01-09DOI: 10.1021/acs.analchem.4c04442
Lijuan Ma, Chaofu Ma, Zijian Wang, Yunan Wei, Nan Li, Jing Wang, Mingshuang Li, Zhisheng Wu, Yang Du
The development of multitargeted drugs is urgent for ischemic stroke. TRPV1 and TRPM8 are important targets of ischemic stroke. Previous drug candidate screening has identified that muscone, l-borneol, and ferulic acid may target TRPV1 and TRPM8 for ischemic stroke. However, the mechanisms of these drug candidates on targets were ill-informed. Therefore, firstly, a tongue-tissue biosensor was constructed. It explored the activation or inhibition mechanisms of drug candidates targeting TRPV1 and TRPM8 in a near-physiological environment. It was found that muscone could specifically inhibit TRPM8 and selectively activate TRPV1, while l-borneol exhibited the opposite effect. It suggested a synergistic network between these two drug candidates. Furthermore, more selective protein biosensors were developed to delve deeper into the synergistic mechanisms. A strong synergistic effect of muscone and l-borneol was proved. Molecular docking revealed that the synergistic effect was caused by different action sites, respectively. Subsequently, the synergistic effect of muscone and l-borneol was further confirmed by hypoxic nerve injury models of Caenorhabditis elegans (C. elegans) and antithrombus and anti-ischemic models of zebrafish. Ultimately, through nontargeted metabolomics, it was found that muscone and l-borneol mainly regulated Ca2+ concentration and energy metabolism by pathways such as purine and amino acid metabolisms. In conclusion, this research identified critical targets and synergistic drug candidates for multitarget neuroprotection of ischemic stroke. In addition, it has systemically demonstrated the feasibility of the integration of tissue/protein biosensors and metabolomics for the research and development of multitarget drugs. Compared to other screening and validation methods for drugs and targets, the biosensors we developed not only achieved higher sensitivity and specificity in complex physiological environments, ensuring a wider detection range, but also greatly saved biological samples. Simultaneously, they could be extended to other complex systems, such as biomarker screening in clinical samples and exosomes isolated from stem cells.
{"title":"Unraveling the Synergistic Neuroprotective Mechanism of Natural Drug Candidates Targeting TRPV1 and TRPM8 on an Ischemic Stroke","authors":"Lijuan Ma, Chaofu Ma, Zijian Wang, Yunan Wei, Nan Li, Jing Wang, Mingshuang Li, Zhisheng Wu, Yang Du","doi":"10.1021/acs.analchem.4c04442","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c04442","url":null,"abstract":"The development of multitargeted drugs is urgent for ischemic stroke. TRPV1 and TRPM8 are important targets of ischemic stroke. Previous drug candidate screening has identified that muscone, <span>l</span>-borneol, and ferulic acid may target TRPV1 and TRPM8 for ischemic stroke. However, the mechanisms of these drug candidates on targets were ill-informed. Therefore, firstly, a tongue-tissue biosensor was constructed. It explored the activation or inhibition mechanisms of drug candidates targeting TRPV1 and TRPM8 in a near-physiological environment. It was found that muscone could specifically inhibit TRPM8 and selectively activate TRPV1, while <span>l</span>-borneol exhibited the opposite effect. It suggested a synergistic network between these two drug candidates. Furthermore, more selective protein biosensors were developed to delve deeper into the synergistic mechanisms. A strong synergistic effect of muscone and <span>l</span>-borneol was proved. Molecular docking revealed that the synergistic effect was caused by different action sites, respectively. Subsequently, the synergistic effect of muscone and <span>l</span>-borneol was further confirmed by hypoxic nerve injury models of <i>Caenorhabditis elegans</i> (<i>C. elegans</i>) and antithrombus and anti-ischemic models of zebrafish. Ultimately, through nontargeted metabolomics, it was found that muscone and <span>l</span>-borneol mainly regulated Ca<sup>2+</sup> concentration and energy metabolism by pathways such as purine and amino acid metabolisms. In conclusion, this research identified critical targets and synergistic drug candidates for multitarget neuroprotection of ischemic stroke. In addition, it has systemically demonstrated the feasibility of the integration of tissue/protein biosensors and metabolomics for the research and development of multitarget drugs. Compared to other screening and validation methods for drugs and targets, the biosensors we developed not only achieved higher sensitivity and specificity in complex physiological environments, ensuring a wider detection range, but also greatly saved biological samples. Simultaneously, they could be extended to other complex systems, such as biomarker screening in clinical samples and exosomes isolated from stem cells.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"36 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142940547","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 : 2025-01-09DOI: 10.1021/acs.analchem.4c05044
Xianmiao Zhang, Yuhang Zhang, Jia Chen, Rong Feng, Xiangwu Wu, Tao Zhang, Shengrong Yu, Ning Gan, Keqi Tang, Yong-Xiang Wu
Bioimaging technology has been broadly used in biomedicine, and the growth of multimodal imaging technology based on synergistic advantages can overcome the shortcomings of traditional single-modal bioimaging methods and attain high specificity and sensitivity in the fields of bioimaging and biosensing. The analysis of low-abundance microRNAs (miRNAs) in complex organisms is of high importance for early-stage diagnosis and clinical treatment of tumors. In our current study, a biosensing nanoplatform based on Tf-AuNCs and MnO2 nanosheets was developed for multimodal imaging of tumor cells. First, oxidizable MnO2 nanosheets provided a smart tool for use as nanocarriers and contrast agents for intracellular glutathione (GSH)-activated magnetic resonance imaging (MRI). Then, MnO2 nanosheets delivered Tf-AuNC-based biosensing nanoplatforms into cells through endocytosis. Endogenous GSH degraded MnO2 nanosheets into Mn2+, and the released functional nucleic acid probes can perform specific biosensing responses to miR-21 exhibiting multimodal imaging including two-photon near-infrared fluorescence imaging (TP-NIRFI), fluorescence lifetime imaging (FLIM), and MRI. Finally, the biosensing nanoplatform achieved satisfactory results in tumor cells and tissues by TP-NIRFI (300.0 μm penetration depth), FLIM (τ ≈ 50.0 ns), and MRI. Therefore, biosensing nanoplatforms based on Tf-AuNCs and MnO2 nanosheets show great potential for multimodal detection and imaging in tumor cells.
{"title":"Transferrin Modified Gold Nanoclusters-Based Biosensing Nanoplatform for High-Precision Multimodal Bioimaging of Tumor Cells","authors":"Xianmiao Zhang, Yuhang Zhang, Jia Chen, Rong Feng, Xiangwu Wu, Tao Zhang, Shengrong Yu, Ning Gan, Keqi Tang, Yong-Xiang Wu","doi":"10.1021/acs.analchem.4c05044","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05044","url":null,"abstract":"Bioimaging technology has been broadly used in biomedicine, and the growth of multimodal imaging technology based on synergistic advantages can overcome the shortcomings of traditional single-modal bioimaging methods and attain high specificity and sensitivity in the fields of bioimaging and biosensing. The analysis of low-abundance microRNAs (miRNAs) in complex organisms is of high importance for early-stage diagnosis and clinical treatment of tumors. In our current study, a biosensing nanoplatform based on Tf-AuNCs and MnO<sub>2</sub> nanosheets was developed for multimodal imaging of tumor cells. First, oxidizable MnO<sub>2</sub> nanosheets provided a smart tool for use as nanocarriers and contrast agents for intracellular glutathione (GSH)-activated magnetic resonance imaging (MRI). Then, MnO<sub>2</sub> nanosheets delivered Tf-AuNC-based biosensing nanoplatforms into cells through endocytosis. Endogenous GSH degraded MnO<sub>2</sub> nanosheets into Mn<sup>2+</sup>, and the released functional nucleic acid probes can perform specific biosensing responses to miR-21 exhibiting multimodal imaging including two-photon near-infrared fluorescence imaging (TP-NIRFI), fluorescence lifetime imaging (FLIM), and MRI. Finally, the biosensing nanoplatform achieved satisfactory results in tumor cells and tissues by TP-NIRFI (300.0 μm penetration depth), FLIM (τ ≈ 50.0 ns), and MRI. Therefore, biosensing nanoplatforms based on Tf-AuNCs and MnO<sub>2</sub> nanosheets show great potential for multimodal detection and imaging in tumor cells.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"39 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142937659","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}
This work describes fully integrated multifolding electrochemical paper-based devices (ePADs) for enhanced multiplexed voltammetric determination of heavy metals (Zn(II), Cd(II), and Pb(II)) using tunable passive preconcentration. The paper devices integrate five circular sample preconcentration layers and a 3-electrode electrochemical cell. The hydrophobic barriers of the devices are drawn by pen-plotting with hydrophobic ink, while the electrodes are deposited by screen-printing. The devices exploit the wicking ability of cellulose paper to perform passive preconcentration of the target analytes, resulting in a ∼6-fold signal enhancement. For this purpose, drops of the sample are placed at the five sample pads of the preconcentration layers, the device is folded, and the target metals are eluted in a vertical-flow mode to the electrochemical cell, where they are measured directly by anodic stripping voltammetry (ASV). The working electrode of the ePADs is bulk-modified with bismuth citrate; during the ASV measurements, the bismuth precursor is converted to nanodomains of metallic bismuth at the surface of the working electrode. By combining the triplex signal amplification through passive preconcentration, electrochemical preconcentration, and judicious working electrode modification with in situ generated bismuth nanoparticles, ultrasensitive and multiplexed heavy metal assays can be achieved. Due to their high degree of integration, low cost, easy and fast fabrication, and sensitivity, the multifolding ePADs are particularly suitable for on-site heavy metals' monitoring applications.
{"title":"Multifolding Vertical-Flow Electrochemical Paper-Based Devices with Tunable Dual Preconcentration for Enhanced Multiplexed Assays of Heavy Metals","authors":"Dionysios Soulis, Electra Mermiga, Varvara Pagkali, Maria Trachioti, Christos Kokkinos, Mamas Prodromidis, Anastasios Economou","doi":"10.1021/acs.analchem.4c06982","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06982","url":null,"abstract":"This work describes fully integrated multifolding electrochemical paper-based devices (ePADs) for enhanced multiplexed voltammetric determination of heavy metals (Zn(II), Cd(II), and Pb(II)) using tunable passive preconcentration. The paper devices integrate five circular sample preconcentration layers and a 3-electrode electrochemical cell. The hydrophobic barriers of the devices are drawn by pen-plotting with hydrophobic ink, while the electrodes are deposited by screen-printing. The devices exploit the wicking ability of cellulose paper to perform passive preconcentration of the target analytes, resulting in a ∼6-fold signal enhancement. For this purpose, drops of the sample are placed at the five sample pads of the preconcentration layers, the device is folded, and the target metals are eluted in a vertical-flow mode to the electrochemical cell, where they are measured directly by anodic stripping voltammetry (ASV). The working electrode of the ePADs is bulk-modified with bismuth citrate; during the ASV measurements, the bismuth precursor is converted to nanodomains of metallic bismuth at the surface of the working electrode. By combining the triplex signal amplification through passive preconcentration, electrochemical preconcentration, and judicious working electrode modification with <i>in situ</i> generated bismuth nanoparticles, ultrasensitive and multiplexed heavy metal assays can be achieved. Due to their high degree of integration, low cost, easy and fast fabrication, and sensitivity, the multifolding ePADs are particularly suitable for on-site heavy metals' monitoring applications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"6 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142937524","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
A linear spot-type multipass cell-enhanced fiber-optic photoacoustic gas microprobe is proposed. To further reduce the volume of the gas chamber and enhance the photoacoustic signal, we designed the cross section of the photoacoustic tube as a slit with a height of 10 mm and a width of 1.5 mm. The volume of the gas chamber is only 210 μL. Through theoretical analysis and multiphysical field simulation, the photoacoustic intensity of the slit cross section is more than 6 times that of traditional circular cross section. A cantilever beam is integrated into the photoacoustic microprobe and forms a Fabry–Perot (FP) interferometer with an optical fiber, achieving enhanced photoacoustic detection. By adjusting the angle of the collimator, the light passes through the photoacoustic cell 26 times, and 13 linear spots are formed on the reflecting surface. The photoacoustic signal with multiple linear reflections is 12.4 times that of a single reflection. The gas enters the sensor in a freely diffused manner, and the response time of the sensing system is 54 s. When the averaging time is 400 s, the detection limit of the designed sensor for acetylene gas reaches 1.5 ppb. The minimum detectable absorption coefficient (αmin) and the normalized noise equivalent absorption coefficient (NNEA) are 1.7 × 10–8 cm–1 and 1.9 × 10–9 Wcm–1/Hz1/2, respectively.
{"title":"Fiber-Optic Photoacoustic Gas Microprobe Based on Linear Spot-Type Multipass Cell","authors":"Heng Wang, Yufu Xu, Jingya Zhang, Xinyu Zhao, Zhaodong Zhang, Ke Chen","doi":"10.1021/acs.analchem.4c05486","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05486","url":null,"abstract":"A linear spot-type multipass cell-enhanced fiber-optic photoacoustic gas microprobe is proposed. To further reduce the volume of the gas chamber and enhance the photoacoustic signal, we designed the cross section of the photoacoustic tube as a slit with a height of 10 mm and a width of 1.5 mm. The volume of the gas chamber is only 210 μL. Through theoretical analysis and multiphysical field simulation, the photoacoustic intensity of the slit cross section is more than 6 times that of traditional circular cross section. A cantilever beam is integrated into the photoacoustic microprobe and forms a Fabry–Perot (FP) interferometer with an optical fiber, achieving enhanced photoacoustic detection. By adjusting the angle of the collimator, the light passes through the photoacoustic cell 26 times, and 13 linear spots are formed on the reflecting surface. The photoacoustic signal with multiple linear reflections is 12.4 times that of a single reflection. The gas enters the sensor in a freely diffused manner, and the response time of the sensing system is 54 s. When the averaging time is 400 s, the detection limit of the designed sensor for acetylene gas reaches 1.5 ppb. The minimum detectable absorption coefficient (α<sub>min</sub>) and the normalized noise equivalent absorption coefficient (NNEA) are 1.7 × 10<sup>–8</sup> cm<sup>–1</sup> and 1.9 × 10<sup>–9</sup> Wcm<sup>–1</sup>/Hz<sup>1/2</sup>, respectively.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"75 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142940546","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 : 2025-01-09DOI: 10.1021/acs.analchem.4c05982
Dianfeng Dai, Zhimin Zhang, Mo Ma, Jingkang Li, Siqi Zhang, Pinyi Ma, Daqian Song
Vanin-1 is a pantetheine hydrolase that plays a key role in inflammatory diseases. Effective tools for noninvasive, real-time monitoring of Vanin-1 are lacking, largely due to background fluorescence interference in existing probes. To address this issue, we developed a dual-modal fluorescent and colorimetric probe, MB-Van1, to detect Vanin-1 with high sensitivity and selectivity. MB-Van1 has a structure optimized to exhibit nearly zero background fluorescence, resulting in a high signal-to-noise ratio that enables the accurate detection of Vanin-1 activity in various biological tissues. In vitro experiments demonstrated that MB-Van1 had a detection limit as low as 0.031 ng/mL in the fluorescence mode. We successfully employ MB-Van1 to observe elevated Vanin-1 levels in inflammatory tissues of various mouse models of rheumatoid arthritis (RA), drug-induced liver injury (DILI), and nonsteroidal anti-inflammatory drug (NSAID) enteropathy models, within only 5 min. This advancement provides a novel approach for monitoring the dynamic changes of Vanin-1 during inflammation, offering new strategies for the early diagnosis and therapeutic assessment of other related diseases.
{"title":"Vanin-1-Activated Fluorescent Probe for Real-Time In Vivo Imaging of Inflammatory Responses Across Multiple Tissue Types","authors":"Dianfeng Dai, Zhimin Zhang, Mo Ma, Jingkang Li, Siqi Zhang, Pinyi Ma, Daqian Song","doi":"10.1021/acs.analchem.4c05982","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05982","url":null,"abstract":"Vanin-1 is a pantetheine hydrolase that plays a key role in inflammatory diseases. Effective tools for noninvasive, real-time monitoring of Vanin-1 are lacking, largely due to background fluorescence interference in existing probes. To address this issue, we developed a dual-modal fluorescent and colorimetric probe, MB-Van1, to detect Vanin-1 with high sensitivity and selectivity. MB-Van1 has a structure optimized to exhibit nearly zero background fluorescence, resulting in a high signal-to-noise ratio that enables the accurate detection of Vanin-1 activity in various biological tissues. <i>In vitro</i> experiments demonstrated that MB-Van1 had a detection limit as low as 0.031 ng/mL in the fluorescence mode. We successfully employ MB-Van1 to observe elevated Vanin-1 levels in inflammatory tissues of various mouse models of rheumatoid arthritis (RA), drug-induced liver injury (DILI), and nonsteroidal anti-inflammatory drug (NSAID) enteropathy models, within only 5 min. This advancement provides a novel approach for monitoring the dynamic changes of Vanin-1 during inflammation, offering new strategies for the early diagnosis and therapeutic assessment of other related diseases.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"85 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142940562","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}
We would like to correct a mistake in which the figures appear in our original paper. During the editing process, the images for Figure 3 were inadvertently switched such that the figures do not correspond to their respective captions. Figure 3. (a) Enzyme-like activity of Fe/Zn–N–C. (b) Effect of calcination temperature. (c) Effect of metal ratio. (d) Time-dependent variations in the catalytic activity of Fe/Zn–N–C. (e) Effect of solution pH. (f) Effect of reaction temperature. We would like to correct this error so that the figure and caption agree. The correct images and caption are provided here. This article has not yet been cited by other publications.
{"title":"Correction to “A Fe/Zn Dual Single-Atom Nanozyme with High Peroxidase Activities for Detection of Penicillin G”","authors":"Wen Wen, Yifei Lang, Zhongping Li, Li Li, Hung-Wing Li, Yingfu Li, Guangming Wen","doi":"10.1021/acs.analchem.4c07086","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c07086","url":null,"abstract":"We would like to correct a mistake in which the figures appear in our original paper. During the editing process, the images for Figure 3 were inadvertently switched such that the figures do not correspond to their respective captions. Figure 3. (a) Enzyme-like activity of Fe/Zn–N–C. (b) Effect of calcination temperature. (c) Effect of metal ratio. (d) Time-dependent variations in the catalytic activity of Fe/Zn–N–C. (e) Effect of solution pH. (f) Effect of reaction temperature. We would like to correct this error so that the figure and caption agree. The correct images and caption are provided here. This article has not yet been cited by other publications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"48 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142940565","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 : 2025-01-09DOI: 10.1021/acs.analchem.4c04871
Jiahui Dai, Beibei Wu, Fengxiang Ai, Zhugen Yang, Yanyan Lu, Cai Zinian, Kun Zeng, Zhen Zhang
The CRISPR-Cas12a system has shown tremendous potential for developing efficient biosensors. Albeit important, current CRISPR-Cas system-based diagnostic technologies (CRISPR-DX) highly rely on an additional preamplification procedure to obtain high sensitivity, inevitably leading to issues such as complicated assay workflow, cross-contamination, etc. Herein, a spherical protospacer-adjacent motif (PAM)-antenna-enhanced CRISPR-Cas12a system is fabricated for universal amplification-free nucleic acid detection with a detection limit of subfemtomolar. Meanwhile, the clinical detection capability of this sensor was further verified using gold-standard real-time quantitative polymerase chain reaction through Mycobacterium tuberculosis measurement, which demonstrated its good reliability for practical applications. Importantly, its excellent sensitivity is mainly ascribed to high efficiency of target search induced by a localized PAM-enriched microenvironment and improved catalytic activity of Cas12a (up to 4 folds). Our strategy provides some new insights for rapid and sensitive detection of nucleic acids in an amplification-free fashion.
{"title":"Exploiting the Potential of Spherical PAM Antenna for Enhanced CRISPR-Cas12a: A Paradigm Shift toward a Universal Amplification-Free Nucleic Acid Test Platform","authors":"Jiahui Dai, Beibei Wu, Fengxiang Ai, Zhugen Yang, Yanyan Lu, Cai Zinian, Kun Zeng, Zhen Zhang","doi":"10.1021/acs.analchem.4c04871","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c04871","url":null,"abstract":"The CRISPR-Cas12a system has shown tremendous potential for developing efficient biosensors. Albeit important, current CRISPR-Cas system-based diagnostic technologies (CRISPR-DX) highly rely on an additional preamplification procedure to obtain high sensitivity, inevitably leading to issues such as complicated assay workflow, cross-contamination, etc. Herein, a spherical protospacer-adjacent motif (PAM)-antenna-enhanced CRISPR-Cas12a system is fabricated for universal amplification-free nucleic acid detection with a detection limit of subfemtomolar. Meanwhile, the clinical detection capability of this sensor was further verified using gold-standard real-time quantitative polymerase chain reaction through <i>Mycobacterium tuberculosis</i> measurement, which demonstrated its good reliability for practical applications. Importantly, its excellent sensitivity is mainly ascribed to high efficiency of target search induced by a localized PAM-enriched microenvironment and improved catalytic activity of Cas12a (up to 4 folds). Our strategy provides some new insights for rapid and sensitive detection of nucleic acids in an amplification-free fashion.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"28 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142937418","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}
Parkinson’s disease (PD) is a progressive neurodegenerative disorder characterized by the loss of dopaminergic neurons and the accumulation of alpha-synuclein. Glutathione (GSH), a key antioxidant, is significantly depleted in PD patients. This study presents a dual-mode detection strategy for selectively determining GSH using a single probe. A series of “turn-on” electrochemical and fluorescent probes were developed, with resorufin (Re) serving as the reporting unit and featuring specific GSH recognition sites. Among these, the 7-(3,5-dinitrophenoxy)-3H-phenoxazin-3-one (Re-DNP) probe was selected for its high selectivity as both a fluorescent and electrochemical probe. Its response to GSH was superior in comparison to that observed for hydrogen sulfide (H2S) and cysteine (Cys). For electrochemical detection using screen-printed carbon electrode (SPCE)/carbon nanotube (CNT) modified electrodes, the detection limit for GSH was 5 μM, with a linear range of 25–500 μM. In fluorescence detection, the probe produced a 78-fold increase in emission at 630 nm in the presence of GSH, with a strong linear correlation between fluorescence intensity and GSH concentration in the range of 10–700 μM, and a detection limit of 2 μM. When applied to real clinical serum samples, the probe demonstrated significantly lower GSH levels in both PD mice and human patients compared to healthy controls. This dual-mode detection method provides a sensitive and accurate tool for GSH detection, with potential applications in understanding GSH’s role in PD and related neurodegenerative diseases.
{"title":"High Selectivity Fluorescence and Electrochemical Dual-Mode Detection of Glutathione in the Serum of Parkinson’s Disease Model Mice and Humans","authors":"Hui Dong, Weitian Chen, Ke Xu, Linlin Zheng, Bingyu Wei, Ruiyu Liu, Jingru Yang, Tao Wang, Yanli Zhou, Yintang Zhang, Maotian Xu","doi":"10.1021/acs.analchem.4c05627","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05627","url":null,"abstract":"Parkinson’s disease (PD) is a progressive neurodegenerative disorder characterized by the loss of dopaminergic neurons and the accumulation of alpha-synuclein. Glutathione (GSH), a key antioxidant, is significantly depleted in PD patients. This study presents a dual-mode detection strategy for selectively determining GSH using a single probe. A series of “turn-on” electrochemical and fluorescent probes were developed, with resorufin (Re) serving as the reporting unit and featuring specific GSH recognition sites. Among these, the 7-(3,5-dinitrophenoxy)-3<i>H</i>-phenoxazin-3-one (Re-DNP) probe was selected for its high selectivity as both a fluorescent and electrochemical probe. Its response to GSH was superior in comparison to that observed for hydrogen sulfide (H<sub>2</sub>S) and cysteine (Cys). For electrochemical detection using screen-printed carbon electrode (SPCE)/carbon nanotube (CNT) modified electrodes, the detection limit for GSH was 5 μM, with a linear range of 25–500 μM. In fluorescence detection, the probe produced a 78-fold increase in emission at 630 nm in the presence of GSH, with a strong linear correlation between fluorescence intensity and GSH concentration in the range of 10–700 μM, and a detection limit of 2 μM. When applied to real clinical serum samples, the probe demonstrated significantly lower GSH levels in both PD mice and human patients compared to healthy controls. This dual-mode detection method provides a sensitive and accurate tool for GSH detection, with potential applications in understanding GSH’s role in PD and related neurodegenerative diseases.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"45 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142937521","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 : 2025-01-09DOI: 10.1021/acs.analchem.4c05972
Yali Yang, Hong Zhang, Jing He, Yun Ju, Mingyi Wang, Lishun Wu, Jie Jiang
Newborn screening for acylcarnitine-related inherited metabolic diseases (IMDs) is a critical test after birth. Conventional extraction methods require shaking with heating, centrifugation, nitrogen blowing, redissolution, etc., and the total time is more than 1 h. Herein, a small amount of trifluoroacetic acid (TFA)-doped extraction method for acylcarnitines coupled with nanoelectrospray ionization mass spectrometry was developed. This simplified approach successfully quantified 21 acylcarnitines in both serum and dried blood spot samples through a fast, three-step process requiring only 7 min, achieving nearly 1-2 orders of magnitude in sensitivity enhancement compared with conventional methods. The performance was further verified by the recommended liquid chromatography-tandem mass spectrometry procedure. Furthermore, the TFA-doped extraction technique was tested on serum and whole blood samples from six healthy individuals. Mechanistic studies using inductively coupled plasma mass spectrometry, ultraviolet-visible spectroscopy, scanning electron microscopy, and energy dispersive X-ray spectroscopy showed that TFA promotes the coprecipitation of proteins and inorganic salts. These findings suggest that TFA-doped extraction with nanoelectrospray ionization mass spectrometry is a rapid, sensitive alternative for acylcarnitine screening, highlighting its considerable potential for clinical newborn IMD screening applications.
{"title":"Rapid Determination of Acylcarnitine Metabolic Diseases by Trifluoroacetic Acid-Doped Extraction Coupled with Nanoelectrospray Ionization Mass Spectrometry","authors":"Yali Yang, Hong Zhang, Jing He, Yun Ju, Mingyi Wang, Lishun Wu, Jie Jiang","doi":"10.1021/acs.analchem.4c05972","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05972","url":null,"abstract":"Newborn screening for acylcarnitine-related inherited metabolic diseases (IMDs) is a critical test after birth. Conventional extraction methods require shaking with heating, centrifugation, nitrogen blowing, redissolution, etc., and the total time is more than 1 h. Herein, a small amount of trifluoroacetic acid (TFA)-doped extraction method for acylcarnitines coupled with nanoelectrospray ionization mass spectrometry was developed. This simplified approach successfully quantified 21 acylcarnitines in both serum and dried blood spot samples through a fast, three-step process requiring only 7 min, achieving nearly 1-2 orders of magnitude in sensitivity enhancement compared with conventional methods. The performance was further verified by the recommended liquid chromatography-tandem mass spectrometry procedure. Furthermore, the TFA-doped extraction technique was tested on serum and whole blood samples from six healthy individuals. Mechanistic studies using inductively coupled plasma mass spectrometry, ultraviolet-visible spectroscopy, scanning electron microscopy, and energy dispersive X-ray spectroscopy showed that TFA promotes the coprecipitation of proteins and inorganic salts. These findings suggest that TFA-doped extraction with nanoelectrospray ionization mass spectrometry is a rapid, sensitive alternative for acylcarnitine screening, highlighting its considerable potential for clinical newborn IMD screening applications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"373 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142940548","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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