Bioelectrochemistry最新文献

英文中文

Whole-cell redox biosensor for triclosan detection: Integrating spectrophotometric and electrochemical detection

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2025-01-28 DOI: 10.1016/j.bioelechem.2025.108921

Himanshu Khandelwal , Sakuntala Mutyala , Minsoo Kim , Da Seul Kong , Jung Rae Kim

Organic pollutants like bisphenol, acetaminophen, and triclosan, widely used in healthcare products, pose environmental risks and act as endocrine disruptors. These pollutants can alter the intracellular redox balance, making engineered whole-cell redox biosensors valuable for their detection. This study utilized the SoxRS regulatory system in bacteria, which responds to oxidative stress through NADP⁺/NADPH levels by modulating gene expression of SoxS through the SoxS promoter (pSoxS). A plasmid containing SoxR-pSoxS and the LacZ reporter gene was constructed and introduced into E. coli BL21 (ΔLacZ SoxRS+). The LacZ gene enabled dual detection using O-nitrophenyl-β-galactopyranoside (ONPG) for spectrophotometric detection or p-aminophenyl β-D-galactopyranoside (PAPG) for electrochemical detection. The whole-cell pRUSL12 redox biosensor was activated by redox inducers such as pyocyanin and methyl viologen, measurable via β-galactosidase assays. Among pollutants tested, triclosan specifically repressed SoxR:pSoxS::lacZ activity in the presence of pyocyanin or methyl viologen. Optimization identified pyocyanin as the more effective inducer for triclosan detection, with the biosensor capable of detecting triclosan in the 100–400 µg/L range. These redox-based biosensors offer a powerful tool for monitoring metabolic redox changes and identifying specific organic pollutants in the environment.

{"title":"Whole-cell redox biosensor for triclosan detection: Integrating spectrophotometric and electrochemical detection","authors":"Himanshu Khandelwal , Sakuntala Mutyala , Minsoo Kim , Da Seul Kong , Jung Rae Kim","doi":"10.1016/j.bioelechem.2025.108921","DOIUrl":"10.1016/j.bioelechem.2025.108921","url":null,"abstract":"<div><div>Organic pollutants like bisphenol, acetaminophen, and triclosan, widely used in healthcare products, pose environmental risks and act as endocrine disruptors. These pollutants can alter the intracellular redox balance, making engineered whole-cell redox biosensors valuable for their detection. This study utilized the SoxRS regulatory system in bacteria, which responds to oxidative stress through NADP<sup>+</sup>/NADPH levels by modulating gene expression of SoxS through the SoxS promoter (pSoxS). A plasmid containing SoxR-pSoxS and the LacZ reporter gene was constructed and introduced into <em>E. coli</em> BL21 (ΔLacZ SoxRS+). The LacZ gene enabled dual detection using O-nitrophenyl-β-galactopyranoside (ONPG) for spectrophotometric detection or p-aminophenyl β-D-galactopyranoside (PAPG) for electrochemical detection. The whole-cell pRUSL12 redox biosensor was activated by redox inducers such as pyocyanin and methyl viologen, measurable via β-galactosidase assays. Among pollutants tested, triclosan specifically repressed SoxR:pSoxS::lacZ activity in the presence of pyocyanin or methyl viologen. Optimization identified pyocyanin as the more effective inducer for triclosan detection, with the biosensor capable of detecting triclosan in the 100–400 µg/L range. These redox-based biosensors offer a powerful tool for monitoring metabolic redox changes and identifying specific organic pollutants in the environment.</div></div>","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"164 ","pages":"Article 108921"},"PeriodicalIF":4.8,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143155966","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Bidirectional electro-enzymatic reaction of coenzyme F420 using benzyl viologen and F420-dependent sulfite reductase

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2025-01-28 DOI: 10.1016/j.bioelechem.2025.108922

Satoshi Furota , Masanori Kaneko , Seiya Tsujimura , Daijiro Takeshita , Yusuke Nakamichi , Kensuke Igarashi , Masaru K. Nobu , Miho Yoshikawa , Kenta Asahina , Chie Fukaya , Toshie Ishitsuka , Kazuma Shimada

Coenzyme F₄₂₀ is recognized as a crucial electron carrier in methane-generating metabolism but, beyond this, has garnered significant attention for its role in diverse microbial physiologies and relevance in industrial, medical, and environmental applications. However, one limitation of current application of F₄₂₀ is the necessity of chemical electron donors for its reduction. In this study, an electrochemical reaction system was designed to facilitate electron transfer between the electrode and F₄₂₀ using F₄₂₀-dependent sulfite reductase (Fsr) as the catalyst and benzyl viologen (BV) as the redox mediator. Photometric analysis and cyclic potential scanning demonstrated that the occurrence of bidirectional (reversible) electrochemical oxidation and reduction of F₄₂₀ in this system depended on the electrode potential. The formal redox potential of F₄₂₀ in this system was −540 mV vs. Ag|AgCl|sat. KCl, which aligned with values previously determined using biochemical assays.

{"title":"Bidirectional electro-enzymatic reaction of coenzyme F420 using benzyl viologen and F420-dependent sulfite reductase","authors":"Satoshi Furota , Masanori Kaneko , Seiya Tsujimura , Daijiro Takeshita , Yusuke Nakamichi , Kensuke Igarashi , Masaru K. Nobu , Miho Yoshikawa , Kenta Asahina , Chie Fukaya , Toshie Ishitsuka , Kazuma Shimada","doi":"10.1016/j.bioelechem.2025.108922","DOIUrl":"10.1016/j.bioelechem.2025.108922","url":null,"abstract":"<div><div>Coenzyme F<sub>420</sub> is recognized as a crucial electron carrier in methane-generating metabolism but, beyond this, has garnered significant attention for its role in diverse microbial physiologies and relevance in industrial, medical, and environmental applications. However, one limitation of current application of F<sub>420</sub> is the necessity of chemical electron donors for its reduction. In this study, an electrochemical reaction system was designed to facilitate electron transfer between the electrode and F<sub>420</sub> using F<sub>420</sub>-dependent sulfite reductase (Fsr) as the catalyst and benzyl viologen (BV) as the redox mediator. Photometric analysis and cyclic potential scanning demonstrated that the occurrence of bidirectional (reversible) electrochemical oxidation and reduction of F<sub>420</sub> in this system depended on the electrode potential. The formal redox potential of F<sub>420</sub> in this system was −540 mV vs. Ag|AgCl|sat. KCl, which aligned with values previously determined using biochemical assays.</div></div>","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"164 ","pages":"Article 108922"},"PeriodicalIF":4.8,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143072976","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Characterization of boron doped diamond electrodes with engineered sp2 carbon content and their application to structure-dependent DNA hybridization

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2025-01-27 DOI: 10.1016/j.bioelechem.2025.108910

Ondrej Hesko , Hana Pivoňková , Lukáš Fojt , Andrew Taylor , Jaromír Kopeček , Karolina Schwarzová-Pecková , Miroslav Fojta

Boron doped diamond electrodes brought a new potential in bioanalytical chemistry including studies of structure and interactions of nucleic acids. Herein, deposition conditions were optimized to produce a set of polycrystalline BDD electrodes with comparable boron concentration in solid phase of (1.8 − 2.1) · 10²¹ cm⁻³ akin to metallic-type conductivity but with increasing sp² carbon content. Increase of [CH₄]/[H₂] from 0.25 % to 2.0 % during deposition led to an obvious decrease in grain size from ca. 300 nm (BDD_0.25) to < 100 nm (BDD_2.0). Adsorption of oligodeoxynucleotides and their structural changes in the presence of K⁺ and Li⁺ ions were evaluated through enzyme-linked DNA hybridization assay in which oxidizable 1-naphthol was released from its phosphoester by streptavidin–alkaline phosphatase conjugate upon successful hybridization of the target oligodeoxynucleotide with a biotinylated complementary probe. With increasing sp² carbon content, the hybridization assay showed improved discrimination between a target forming guanine quadruplex (stabilized by K⁺ ions), yielding by 40 % – 60 % lower hybridization signal with the complementary probe, compared to the same but unstructured target oligodeoxynucleotide in the presence of Li⁺ ions that don’t stabilize the quadruplex structure. Such behaviour was observed also for commercial BDD electrode with surface roughness < 10 nm.

{"title":"Characterization of boron doped diamond electrodes with engineered sp2 carbon content and their application to structure-dependent DNA hybridization","authors":"Ondrej Hesko , Hana Pivoňková , Lukáš Fojt , Andrew Taylor , Jaromír Kopeček , Karolina Schwarzová-Pecková , Miroslav Fojta","doi":"10.1016/j.bioelechem.2025.108910","DOIUrl":"10.1016/j.bioelechem.2025.108910","url":null,"abstract":"<div><div>Boron doped diamond electrodes brought a new potential in bioanalytical chemistry including studies of structure and interactions of nucleic acids. Herein, deposition conditionswere optimized to produce a set of polycrystalline BDD electrodes with comparable boron concentration in solid phase of (1.8 − 2.1) · 10<sup>21</sup> cm<sup>−3</sup> akin to metallic-type conductivity but with increasing sp<sup>2</sup>   300 nm (BDD<sub>0.25</sub>) to < 100 nm (BDD<sub>2.0</sub>). Adsorption of oligodeoxynucleotides and their structural changes in the presence of K<sup>+</sup> and Li<sup>+</sup> ions were evaluated through enzyme-linked DNA hybridization assay in which oxidizable 1-naphthol was released from its phosphoesterbystreptavidin–alkaline phosphatase conjugate upon successful hybridization of the target oligodeoxynucleotide with a biotinylated complementary probe. With increasing sp<sup>2</sup> ions that don’t stabilize the quadruplex structure. Such behaviour was observed also for commercial BDD electrode with surface roughness < 10 nm.</div></div>","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"164 ","pages":"Article 108910"},"PeriodicalIF":4.8,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143155964","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Label-free electrochemical immunosensors based on Cu-Ni metal–organic framework and carbon nanotube composite for carcinoembryonic antigen detection

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2025-01-27 DOI: 10.1016/j.bioelechem.2025.108918

Shi Wang , Jialin Ao , Saiwen Ding , Ting Shu

Monitoring cancer biomarkers is of great significance in clinical diagnosis. In this work, a label-free MWCNTs-COOH/CuNi-BTC/FTO electrochemical immunosensor was developed to quantitatively detect carcinoembryonic antigen (CEA). The bimetallic CuNi-BTC showed enhanced current than singe Ni-BTC, and the addition of the MWCNTs-COOH increased the conductivity and further amplified the current signal. The electrode was further modified with CEA antigen (Ag) and bovine serum albumin (BSA) was used to block the non-specific binding sites. Using the emplified current signal of CuNi-BTC, CEA was detected by a DPV method through the current change caused by the specific recognition reaction of Ag and Ab. Under optimal conditions, a range of 0.80–140 ng/mL and a detection limit of 0.046 ng/mL for CEA was obtained. This electrochemical immunosensor possessed good selectivity, reproducibility and long-term stability.

引用次数: 0

Ferredoxin NADP+ reductase for NADPH and NADH regeneration in a flow bioelectrochemical reactor

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2025-01-27 DOI: 10.1016/j.bioelechem.2025.108919

Wassim El Housseini , François Lapicque , Alain Walcarius , Elisabeth Lojou , Nicolas Rouhier , Mathieu Etienne

Ferredoxin-NADP⁺ reductase (FNR) is an efficient and selective biocatalyst to continuously regenerate the NADPH cofactor consumed in biomolecular synthesis for the chemical and pharmaceutical sectors. In this work, FNR from Chlamydomonas reinhardtii was applied to electrochemical regeneration of the nicotinamide cofactors, by combining this enzymatic catalyst in a flow reactor with the oxidation of hydrogen, a clean source of electrons and protons. FNR was immobilized on the surface of oxidized multi-walled carbon nanotubes, which allowed maintaining its activity for over six days under high flow rate. Surprisingly, this modified FNR electrode was effective not only in regenerating NADPH but also NADH. The cofactor regeneration was then applied to the NADH-dependent production of lactate from pyruvate, using L-lactate dehydrogenase (LDH) in the presence of low NAD⁺ concentration (10 µM). Both FNR and LDH enzymes were immobilized in the bioelectrochemical system that achieved a remarkable total turnover number (TTN) of 10⁴ for the nicotinamide cofactor and a faradaic efficiency higher than 80 %.

{"title":"Ferredoxin NADP+ reductase for NADPH and NADH regeneration in a flow bioelectrochemical reactor","authors":"Wassim El Housseini , François Lapicque , Alain Walcarius , Elisabeth Lojou , Nicolas Rouhier , Mathieu Etienne","doi":"10.1016/j.bioelechem.2025.108919","DOIUrl":"10.1016/j.bioelechem.2025.108919","url":null,"abstract":"<div><div>Ferredoxin-NADP<sup>+</sup> reductase (FNR) is an efficient and selective biocatalyst to continuously regenerate the NADPH cofactor consumed in biomolecular synthesis for the chemical and pharmaceutical sectors. In this work, FNR from <em>Chlamydomonas reinhardtii</em> was applied to electrochemical regeneration of the nicotinamide cofactors, by combining this enzymatic catalyst in a flow reactor with the oxidation of hydrogen, a clean source of electrons and protons. FNR was immobilized on the surface of oxidized multi-walled carbon nanotubes, which allowed maintaining its activity for over six days under high flow rate. Surprisingly, this modified FNR electrode was effective not only in regenerating NADPH but also NADH. The cofactor regeneration was then applied to the NADH-dependent production of lactate from pyruvate, using L-lactate dehydrogenase (LDH) in the presence of low NAD<sup>+</sup> concentration (10 µM). Both FNR and LDH enzymes were immobilized in the bioelectrochemical system that achieved a remarkable total turnover number (TTN) of 10<sup>4</sup> for the nicotinamide cofactor and a faradaic efficiency higher than 80 %.</div></div>","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"164 ","pages":"Article 108919"},"PeriodicalIF":4.8,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143155965","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Exploring the electrochemical behaviour of digestive enzymes at a liquid|liquid micro-interface array

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2025-01-26 DOI: 10.1016/j.bioelechem.2025.108911

Shaheda Zannah, Damien W.M. Arrigan

Trypsin and pepsin are proteolytic enzymes secreted by the digestive system to digest proteins. Here, we examine the electrochemical behaviour and detection of trypsin and pepsin at a liquid/liquid (L|L) micro-interface array. For both proteins, aqueous phase of 10 mM hydrochloric acid was the only electrolyte solution in which they were electroactive. Neither protein was detected below 30 μM by cyclic voltammetry (CV) but stripping voltammetry following adsorption (AdSV) enabled the detection of sub-micromolar concentrations of both proteins. Although pepsin was electroactive at the micro-interface array in aqueous phase of 10 mM HCl, its behaviour was ill-defined and unsuitable for characterization by CV. It was found that pepsin easily blocked the micro-interfaces, as seen by greatly hampered ion transfer voltammetry of tetrapropylammonium ion (TPrA⁺) whereas trypsin only slightly impeded TPrA⁺ transfer. This highlights the dissimilarity between pepsin and trypsin. These results illustrate the rich viability of electrochemistry at L|L micro-interface arrays as a tool to explore the behaviour and detection of biological macromolecules.

{"title":"Exploring the electrochemical behaviour of digestive enzymes at a liquid|liquid micro-interface array","authors":"Shaheda Zannah, Damien W.M. Arrigan","doi":"10.1016/j.bioelechem.2025.108911","DOIUrl":"10.1016/j.bioelechem.2025.108911","url":null,"abstract":"<div><div>Trypsin and pepsin are proteolytic enzymes secreted by the digestive system to digest proteins. Here, we examine the electrochemical behaviour and detection of trypsin and pepsin at a liquid/liquid (L|L) micro-interface array. For both proteins, aqueous phase of 10 mM hydrochloric acid was the only electrolyte solution in which they were electroactive. Neither protein was detected below 30 μM by cyclic voltammetry (CV) but stripping voltammetry following adsorption (AdSV) enabled the detection of sub-micromolar concentrations of both proteins. Although pepsin was electroactive at the micro-interface array in aqueous phase of 10 mM HCl, its behaviour was ill-defined and unsuitable for characterization by CV. It was found that pepsin easily blocked the micro-interfaces, as seen by greatly hampered ion transfer voltammetry of tetrapropylammonium ion (TPrA<sup>+</sup>) whereas trypsin only slightly impeded TPrA<sup>+</sup> transfer. This highlights the dissimilarity between pepsin and trypsin. These results illustrate the rich viability of electrochemistry at L|L micro-interface arrays as a tool to explore the behaviour and detection of biological macromolecules.</div></div>","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"164 ","pages":"Article 108911"},"PeriodicalIF":4.8,"publicationDate":"2025-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143372069","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Paper-based electrochemiluminescence telomerase activity detection using hybridization chain reaction and CRISPR/Cas12a dual signal amplification

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2025-01-26 DOI: 10.1016/j.bioelechem.2025.108916

Yun Zhang , Liang Gao , Zhe Shi , Qiong Wu , Xiangmin Miao

Sensitive telomerase activity detection becomes particularly significance since the important value of it in early cancer diagnosis as a potential biomarker. Herein, we developed a paper-based analytical devices (PADs) for telomerase activity detection, using positively charged Au@luminol nanoparticles ((+)Au@luminol NPs) as electrochemiluminescence (ECL) signal probe coupling with hybridization chain reaction (HCR) and CRISPR/Cas12a dual signal amplification. Firstly, the initial strong ECL signal was obtained based on the electrostatic adsorption of (+)Au@luminol NPs onto the surface of HCR double-stranded hybrid aggregates. In the presence of telomerase, the primer was efficiently elongated with telomeric repeats of (TTAGGG)_n to release activator DNA and trigger the CRISPR/Cas12a, which can prevent the happen of HCR and the adsorption of (+)Au@luminol NPs through cleaving the capture probe on the electrode surface, such results directly inducing the decrease of the ECL signal that was proportional to telomerase concentration, due to the efficient signal amplification of HCR and CRISPR/Cas12a, a low detection limit of 2.3 cells/mL for telomerase could be detected. Moreover, the sensor realized the effective application for telomerase extracts analysis in human serum samples, making it possess potential application value for telomerase activity assays in cancer diagnostics.

{"title":"Paper-based electrochemiluminescence telomerase activity detection using hybridization chain reaction and CRISPR/Cas12a dual signal amplification","authors":"Yun Zhang , Liang Gao , Zhe Shi , Qiong Wu , Xiangmin Miao","doi":"10.1016/j.bioelechem.2025.108916","DOIUrl":"10.1016/j.bioelechem.2025.108916","url":null,"abstract":"<div><div>Sensitive telomerase activity detection becomes particularly significance since the important value of it in early cancer diagnosis as a potential biomarker. Herein, we developed a paper-based analytical devices (PADs) for telomerase activity detection, using positively charged Au@luminol nanoparticles ((+)Au@luminol NPs) as electrochemiluminescence (ECL) signal probe coupling with hybridization chain reaction (HCR) and CRISPR/Cas12a dual signal amplification. Firstly, the initial strong ECL signal was obtained based on the electrostatic adsorption of (+)Au@luminol NPs onto the surface of HCR double-stranded hybrid aggregates. In the presence of telomerase, the primer was efficiently elongated with telomeric repeats of (TTAGGG)<sub>n</sub> to release activator DNA and trigger the CRISPR/Cas12a, which can prevent the happen of HCR and the adsorption of (+)Au@luminol NPs through cleaving the capture probe on the electrode surface, such results directly inducing the decrease of the ECL signal that was proportional to telomerase concentration, due to the efficient signal amplification of HCR and CRISPR/Cas12a, a low detection limit of 2.3 cells/mL for telomerase could be detected. Moreover, the sensor realized the effective application for telomerase extracts analysis in human serum samples, making it possess potential application value for telomerase activity assays in cancer diagnostics.</div></div>","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"164 ","pages":"Article 108916"},"PeriodicalIF":4.8,"publicationDate":"2025-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143155422","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

An electrochemiluminescence strategy with proximity ligation triggered multiple catalytic hairpin assembly induced CRISPR/Cas 12a system for analysis of paraquat

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2025-01-25 DOI: 10.1016/j.bioelechem.2025.108915

Wen-Jie Zhong , Wei-Guo Yang , Ying Zhang , Tao Li , Ming-Li Su , Ruo Yuan , Shangcheng Xu , Wen-Bin Liang

Paraquat (PQ) as a widely used non-selective herbicides has gained attention in agricultural residue detection and food safety. Herein, a novel quantitative analysis approach for PQ was proposed based on a novel kind of aggregation-induced emission electrochemiluminescence (AIECL) emitters, tetraphenylethylene-luminol (TPE-L) with a small molecule-induced multiple catalytic hairpin assembly (CHA) amplification strategy, the competitive immune reaction and CRISPR/Cas12a system. The target molecule PQ is introduced into a signal cycle, and auxiliary sensitization cycles are constructed by virtue of the cleavage characteristics of the CRISPR/Cas12a system, which realized the multiple utilization of the target by using both cis- and trans-cleavage activities. In addition, the new multiple CHA amplification strategy was attributed to cross-catalytic hairpin assembly caused by the products of the CHA cycle as the initiator chain of the next CHA cycle, realizing the efficient utilization of cyclic products and producing high-efficiency signal amplification. Thus, the ECL biosensor for ultrasensitive analysis of PQ was successfully constructed with a limit of detection of 0.7 pg/mL. Importantly, it could be easily-extended to other small molecules simply by replacing paired antibodies, providing prospects in agricultural residue detection, food safety and related medical applications.

{"title":"An electrochemiluminescence strategy with proximity ligation triggered multiple catalytic hairpin assembly induced CRISPR/Cas 12a system for analysis of paraquat","authors":"Wen-Jie Zhong , Wei-Guo Yang , Ying Zhang , Tao Li , Ming-Li Su , Ruo Yuan , Shangcheng Xu , Wen-Bin Liang","doi":"10.1016/j.bioelechem.2025.108915","DOIUrl":"10.1016/j.bioelechem.2025.108915","url":null,"abstract":"<div><div>Paraquat (PQ) as a widely used non-selective herbicides has gained attention in agricultural residue detection and food safety. Herein, a novel quantitative analysis approach for PQ was proposed based on a novel kind of aggregation-induced emission electrochemiluminescence (AIECL) emitters, tetraphenylethylene-luminol (TPE-L) with a small molecule-induced multiple catalytic hairpin assembly (CHA) amplification strategy, the competitive immune reaction and CRISPR/Cas12a system. The target molecule PQ is introduced into a signal cycle, and auxiliary sensitization cycles are constructed by virtue of the cleavage characteristics of the CRISPR/Cas12a system, which realized the multiple utilization of the target by using both cis- and <em>trans</em>-cleavage activities. In addition, the new multiple CHA amplification strategy was attributed to cross-catalytic hairpin assembly caused by the products of the CHA cycle as the initiator chain of the next CHA cycle, realizing the efficient utilization of cyclic products and producing high-efficiency signal amplification. Thus, the ECL biosensor for ultrasensitive analysis of PQ was successfully constructed with a limit of detection of 0.7 pg/mL. Importantly, it could be easily-extended to other small molecules simply by replacing paired antibodies, providing prospects in agricultural residue detection, food safety and related medical applications.</div></div>","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"164 ","pages":"Article 108915"},"PeriodicalIF":4.8,"publicationDate":"2025-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143155967","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Advanced cortisol detection: A cMWCNTs-enhanced MB@Zr-MOF ratiometric electrochemical aptasensor

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2025-01-23 DOI: 10.1016/j.bioelechem.2025.108914

Runran Ma , Te Li , Xueying Li , Jianwei Han , Xin Zhang , Tingting Di , Jiabo Wang , Weijun Kong

A ratiometric electrochemical aptasensor was developed for ultra-sensitive detection of cortisol using aptamer (Apt) as recognition element, methylene blue (MB) as signal probe, and zirconium metal–organic framework (Zr-MOF) as carrier loaded with abundant MB for signal amplification. The carboxylated multi-walled carbon nanotubes (cMWCNTs)-modified Au electrode showed excellent electrochemical performance to immobilize complementary DNA (cDNA) for hybridizing with MB@Zr-MOF-Apt via amide bonds. In the presence of cortisol, it would compete with cDNA for binding the Apt, resulting in the detachment of MB@Zr-MOF-Apt complex from the electrode surface, and the electrochemical signal of MB was decreased, while that of [Fe(CN)₆]^3−/4− was basically unchanged. The ratio of the electrochemical signals of [Fe(CN)₆]^3−/4− to MB was proportional to the cortisol concentration. Due to the greatly enhanced conductivity of the cMWCNTs-decorated Au electrode and the largely improved EC signals of Zr-MOF encapsulated MB probes, this ratiometric electrochemical aptasensor offered high sensitivity with an ultra-low detection limit of 0.0046 nM and a wide linearity of 0.01–1000 nM, as well as satisfactory accuracy with recoveries of 93.79–106.76 % in artificial sweat samples, providing a potential strategy for the detection of more trace hormones in different clinical samples by simply replacing the corresponding aptamers.

以适配体（Apt）为识别元件，亚甲基蓝（MB）为信号探针，锆金属有机框架（Zr-MOF）为载体，负载丰富的甲基蓝（MB）进行信号放大，开发了一种用于超灵敏检测皮质醇的比率计量电化学适配体传感器。羧化多壁碳纳米管（cMWCNTs）修饰的金电极显示出优异的电化学性能，可固定互补 DNA（cDNA），通过酰胺键与 MB@Zr-MOF-Apt 杂交。在皮质醇存在的情况下，皮质醇会与 cDNA 竞争结合 Apt，导致 MB@Zr-MOF-Apt 复合物从电极表面脱离，MB 的电化学信号降低，而[Fe(CN)6]3-/4- 的电化学信号基本不变。[Fe(CN)6]3-/4-与甲基溴电化学信号的比值与可的松浓度成正比。由于经 cMWCNTs 装饰的金电极的电导率大大提高，而封装了 Zr-MOF 的甲基溴探针的电化学信号也有很大改善，因此这种比率电化学传感器灵敏度高，检出限超低，仅为 0.0046 nM 的超低检测限和 0.01-1000 nM 的宽线性度，以及令人满意的准确度（在人工汗液样品中的回收率为 93.79-106.76 %）。

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引用次数: 0

An electrochemical aptasensor based on bimetallic carbon nanocomposites AuPt@rGO for ultrasensitive detection of adenosine on portable potentiostat

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2025-01-22 DOI: 10.1016/j.bioelechem.2025.108906

Zheng Gong , Hongli Zhao , Yi Mao , Fangfang Zhou , Zehui Shi , Minbo Lan

Adenosine plays a crucial role in the cardiovascular and nervous systems of living organisms. Excessive adenosine can lead to arrhythmias or heart failure, making the accurate detection of adenosine highly valuable. Given the widespread use of sensors for detecting small molecules, we propose a sensitive electrochemical aptasensor for adenosine detection in this study. The aptasensor utilized reduced graphene oxide (rGO) as the base material, and its performance was further enhanced by loading gold-platinum nanoparticles (AuPt@rGO) to improve the current response. The AuPt@rGO composite was synthesized using a simple process and was modified onto screen-printed electrodes (SPE) fabricated in the laboratory. This modification increased the effective area of the working electrode, providing more contact sites and enhancing sensitivity for adenosine detection. As a result, the sensor exhibited excellent performance in selectivity, sensitivity, and stability, with a linear response range for adenosine from 10 nM to 10 μM and a detection limit of 1.28 nM (n = 3). Furthermore, successful detection of adenosine levels in real samples was achieved using a portable potentiostat, demonstrating excellent recovery rates (95.99 %–103.4 %). These results indicate the aptasensor’s significant potential for future applications in field analysis and medical diagnostics.

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