Bioelectrochemistry最新文献

英文中文

The acceleration of localized copper corrosion by extracellular polymeric substances of sulfate-reducing bacteria

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2025-04-05 DOI: 10.1016/j.bioelechem.2025.108980

Huixuan Qian, Tianguan Wang, Bo Zhang, Guozhe Meng

Microbial-induced corrosion (MIC) of copper pipelines, especially in sulfate-reducing bacteria (SRB)-rich environments, poses a significant challenge. Despite its importance, the role of SRB-secreted extracellular polymeric substances (EPS) in copper corrosion particularly their time-dependent interactions remains unclear. This knowledge gap limits the development of effective corrosion mitigation strategies. In this study, we investigate the impact of EPS on copper corrosion using electrochemical and surface characterization techniques. Our findings reveal that EPS exhibits a dual role in copper corrosion. During the initial immersion phase (1–3 days), EPS adsorption forms a protective layer, temporarily inhibiting corrosion. In the middle stage (4–8 days), EPS accelerates corrosion by degrading the copper oxide film, as evidenced by a negative shift in the breakdown potential (E_b). In the final stage (9–14 days), uneven EPS coverage exacerbates localized corrosion. Thus, SRB-secreted EPS initially acts as a corrosion inhibitor but later promotes localized corrosion through oxide film disruption and non-uniform coverage. We systematically investigated the mechanisms of EPS-mediated corrosion inhibition across different immersion periods, identifying the critical transition threshold between the inhibition and promotion phases.

{"title":"The acceleration of localized copper corrosion by extracellular polymeric substances of sulfate-reducing bacteria","authors":"Huixuan Qian, Tianguan Wang, Bo Zhang, Guozhe Meng","doi":"10.1016/j.bioelechem.2025.108980","DOIUrl":"10.1016/j.bioelechem.2025.108980","url":null,"abstract":"<div><div>Microbial-induced corrosion (MIC) of copper pipelines, especially in sulfate-reducing bacteria (SRB)-rich environments, poses a significant challenge. Despite its importance, the role of SRB-secreted extracellular polymeric substances (EPS) in copper corrosion particularly their time-dependent interactions remains unclear. This knowledge gap limits the development of effective corrosion mitigation strategies. In this study, we investigate the impact of EPS on copper corrosion using electrochemical and surface characterization techniques. Our findings reveal that EPS exhibits a dual role in copper corrosion. During the initial immersion phase (1–3 days), EPS adsorption forms a protective layer, temporarily inhibiting corrosion. In the middle stage (4–8 days), EPS accelerates corrosion by degrading the copper oxide film, as evidenced by a negative shift in the breakdown potential (<em>E</em><sub>b</sub>). In the final stage (9–14 days), uneven EPS coverage exacerbates localized corrosion. Thus, SRB-secreted EPS initially acts as a corrosion inhibitor but later promotes localized corrosion through oxide film disruption and non-uniform coverage. We systematically investigated the mechanisms of EPS-mediated corrosion inhibition across different immersion periods, identifying the critical transition threshold between the inhibition and promotion phases.</div></div>","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"165 ","pages":"Article 108980"},"PeriodicalIF":4.8,"publicationDate":"2025-04-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143790972","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

A colorimetric and electrochemical dual-modal ochratoxin a aptasensor based on branched hybridization chain reaction signal amplification

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2025-04-05 DOI: 10.1016/j.bioelechem.2025.108984

Yihao Li , Yulu Cao , Junjie Huang , Jiachen Zhang , Yonghong Wang , Yuanqing Wang , Ge Ning

Ochratoxin A (OTA), a fungal toxin, induces various toxic effects in animals and humans through the enrichment of toxin residues. In this work, a dual-modal biosensor based on gold nanoparticles (AuNPs) and branched hybridization chain reaction (bHCR) was proposed for the detection of OTA. The strategy is contingent on OTA aptamer-bridged occurrence of bHCR and the salt-induced aggregation of AuNPs. OTA-apt/cDNA could be used to specifically identify the OTA and trigger bHCR reactions, producing a long-branched dsDNA polymer. The electroactive molecule-methylene blue (MB) can be inserted into the superstructure of branched DNA due to the formation of DNA polymers, leading to dynamic changes in MB redox signaling. The residual DNA hairpins were added and adhered to the surface of AuNPs, but they were inadequate to prevent the AuNPs from salt-induced aggregation. The dual-modal yields limits of detection of 4.8 pM (electrochemical assay) and 0.25 nM (colorimetric assay), respectively. It exhibited excellent specificity against common mycotoxins (AFB1, DON, FB1, ZEN), with satisfactory recoveries in corn flour (92.9–108.3 %). This aptasensor, which adopts a dual-modal strategy, features self-calibration to reduce false-positive results and improve accuracy. It demonstrates significant advantages in mycotoxin detection.

{"title":"A colorimetric and electrochemical dual-modal ochratoxin a aptasensor based on branched hybridization chain reaction signal amplification","authors":"Yihao Li , Yulu Cao , Junjie Huang , Jiachen Zhang , Yonghong Wang , Yuanqing Wang , Ge Ning","doi":"10.1016/j.bioelechem.2025.108984","DOIUrl":"10.1016/j.bioelechem.2025.108984","url":null,"abstract":"<div><div>Ochratoxin A (OTA), a fungal toxin, induces various toxic effects in animals and humans through the enrichment of toxin residues. In this work, a dual-modal biosensor based on gold nanoparticles (AuNPs) and branched hybridization chain reaction (bHCR) was proposed for the detection of OTA. The strategy is contingent on OTA aptamer-bridged occurrence of bHCR and the salt-induced aggregation of AuNPs. OTA-apt/cDNA could be used to specifically identify the OTA and trigger bHCR reactions, producing a long-branched dsDNA polymer. The electroactive molecule-methylene blue (MB) can be inserted into the superstructure of branched DNA due to the formation of DNA polymers, leading to dynamic changes in MB redox signaling. The residual DNA hairpins were added and adhered to the surface of AuNPs, but they were inadequate to prevent the AuNPs from salt-induced aggregation. The dual-modal yields limits of detection of 4.8 pM (electrochemical assay) and 0.25 nM (colorimetric assay), respectively. It exhibited excellent specificity against common mycotoxins (AFB1, DON, FB1, ZEN), with satisfactory recoveries in corn flour (92.9–108.3 %). This aptasensor, which adopts a dual-modal strategy, features self-calibration to reduce false-positive results and improve accuracy. It demonstrates significant advantages in mycotoxin detection.</div></div>","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"165 ","pages":"Article 108984"},"PeriodicalIF":4.8,"publicationDate":"2025-04-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143790924","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

Electrochemical quantification of β-glucosidase activity for inhibitor screening applications

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2025-04-04 DOI: 10.1016/j.bioelechem.2025.108981

Catalina Farcas , C. Reyes Mateo , Francisco Montilla

The measurement of enzymatic activity of glucosidases is essential for its use in various clinical and industrial applications. Inhibitors of these enzymes are promising candidates as antidiabetic drug. This study presents the development of an electrochemical device for quantifying β-glucosidase activity using an electrochemical transduction method. Enzyme activity was evaluated in a citrate buffer solution with p-arbutin (hydroquinone-β-D-glucopyranoside) as the substrate, employed for the first time in this context. The enzymatic hydrolysis of the glycosidic bond produced hydroquinone, which was quantified via voltammetric measurements to determine the hydrolysis rate. To develop a device for the screening of inhibitory effects on glucosidase, this enzyme was immobilized into silica matrix and its activity was evaluated. Entrapped enzyme shows partial retention of its catalytic function that can be measured by means of the electrochemical transduction. The inhibitory effects of various sugars and acarbose (a commonly used antidiabetic drug) were investigated using the sensor with the immobilized enzyme. Inhibition rates detected ranged from 87 % to 13 % for the sugars and 17 % for acarbose.

{"title":"Electrochemical quantification of β-glucosidase activity for inhibitor screening applications","authors":"Catalina Farcas , C. Reyes Mateo , Francisco Montilla","doi":"10.1016/j.bioelechem.2025.108981","DOIUrl":"10.1016/j.bioelechem.2025.108981","url":null,"abstract":"<div><div>The measurement of enzymatic activity of glucosidases is essential for its use in various clinical and industrial applications. Inhibitors of these enzymes are promising candidates as antidiabetic drug. This study presents the development of an electrochemical device for quantifying <em>β</em>-glucosidase activity using an electrochemical transduction method. Enzyme activity was evaluated in a citrate buffer solution with <em>p</em>-arbutin (hydroquinone-β-D-glucopyranoside) as the substrate, employed for the first time in this context. The enzymatic hydrolysis of the glycosidic bond produced hydroquinone, which was quantified via voltammetric measurements to determine the hydrolysis rate. To develop a device for the screening of inhibitory effects on glucosidase, this enzyme was immobilized into silica matrix and its activity was evaluated. Entrapped enzyme shows partial retention of its catalytic function that can be measured by means of the electrochemical transduction. The inhibitory effects of various sugars and acarbose (a commonly used antidiabetic drug) were investigated using the sensor with the immobilized enzyme. Inhibition rates detected ranged from 87 % to 13 % for the sugars and 17 % for acarbose.</div></div>","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"165 ","pages":"Article 108981"},"PeriodicalIF":4.8,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143790973","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

Riboflavin-mediated extracellular electron transfer enhances microbiologically influenced corrosion of 316L stainless steel by Enterococcus faecalis

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2025-04-01 DOI: 10.1016/j.bioelechem.2025.108982

Xiaomeng Liu , Enze Zhou , Yongqiang Fan , Fuhui Wang , Dake Xu

316L stainless steel (SS) is widely used in medical implants due to its excellent mechanical properties. However, the increasing use of metallic implants has made microbiologically influenced corrosion (MIC) a significant safety concern, as it can release harmful metal ions in the body. Despite this risk, research on MIC behavior and mechanisms of 316L SS in the intestinal environment is limited. This study provides novel evidence that Enterococcus faecalis, an intestinal electroactive microorganism, contributes to MIC of 316L SS. MIC occurrence by E. faecalis was confirmed in nutrient-rich media and simulated intestinal fluid, with increased MIC rates under carbon starvation, suggesting an extracellular electron transfer (EET) mechanism. Electrochemical tests and material analyses supported a riboflavin-mediated EET mechanism, indicating that E. faecalis biofilms deteriorate the protective oxide layer on 316L SS through EET, with riboflavin accelerating corrosion. These findings identify EET as the primary mechanism by which E. faecalis enhances MIC in the gut, providing insights into intestinal corrosion risks and guiding the development of corrosion-resistant biomaterials.

{"title":"Riboflavin-mediated extracellular electron transfer enhances microbiologically influenced corrosion of 316L stainless steel by Enterococcus faecalis","authors":"Xiaomeng Liu , Enze Zhou , Yongqiang Fan , Fuhui Wang , Dake Xu","doi":"10.1016/j.bioelechem.2025.108982","DOIUrl":"10.1016/j.bioelechem.2025.108982","url":null,"abstract":"<div><div>316L stainless steel (SS) is widely used in medical implants due to its excellent mechanical properties. However, the increasing use of metallic implants has made microbiologically influenced corrosion (MIC) a significant safety concern, as it can release harmful metal ions in the body. Despite this risk, research on MIC behavior and mechanisms of 316L SS in the intestinal environment is limited. This study provides novel evidence that <em>Enterococcus faecalis</em>, an intestinal electroactive microorganism, contributes to MIC of 316L SS. MIC occurrence by <em>E. faecalis</em> was confirmed in nutrient-rich media and simulated intestinal fluid, with increased MIC rates under carbon starvation, suggesting an extracellular electron transfer (EET) mechanism. Electrochemical tests and material analyses supported a riboflavin-mediated EET mechanism, indicating that <em>E. faecalis</em> biofilms deteriorate the protective oxide layer on 316L SS through EET, with riboflavin accelerating corrosion. These findings identify EET as the primary mechanism by which <em>E. faecalis</em> enhances MIC in the gut, providing insights into intestinal corrosion risks and guiding the development of corrosion-resistant biomaterials.</div></div>","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"165 ","pages":"Article 108982"},"PeriodicalIF":4.8,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143799471","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

Enhanced photocurrent generation of a bio-photocathode based on photosystem I integrated in solvated redox polymers films nanostructured by SWCNTs

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2025-03-28 DOI: 10.1016/j.bioelechem.2025.108979

Yanling Yu , Xiaodong Su , Tong Xing , Xuelin Zhao , Zhou Zhang , Wanqing Zhang , Xinping Wang , Weining Zhao , Mei Li , Fangyuan Zhao

The most energetic light-induced charge-separation step in nature is driven by photosystem I (PSI), making this photosynthetic protein an attractive candidate for the development of semi-artificial energy conversion devices. Despite significant progress in semiconductor-free bio-photocathodes, the highest photocurrent density was only 322 ± 19 μA cm⁻², achieved by integrating PSI within a pH-dependent poly(vinyl)imidazole Os(bispyridine)₂Cl redox polymer (T Kothe et al., Chem. Eur. J., 2014, 20, 11029). This study presents a more efficient PSI-based bio-photocathode by incorporating single-walled carbon nanotubes (SWCNTs) into the redox hydrogel composed of the same Osmium-containing redox polymer. The nanostructured redox hydrogel film with SWCNTs serving as electric scaffolds significantly improves the stability, loading amount, and heterogeneous electron transfer rate, resulting in a substantial increase in photocurrent density exceeding 2 mA cm⁻², the highest achieved in a semiconductor-free PSI based photocathode to date. Bioelectrodes constructed by pre-depositing SWCNTs on the electrode surface via covalent bonds outperform those formed by co-immobilizing SWCNTs with the redox hydrogel. The dependence of photocurrent on light intensity and the photocurrent spectrum action demonstrate that the photocurrent unequivocally arises from PSI charge separation. This research lays a promising foundation for the development of semi-artificial photoelectrochemical devices for light-to-energy conversion.

{"title":"Enhanced photocurrent generation of a bio-photocathode based on photosystem I integrated in solvated redox polymers films nanostructured by SWCNTs","authors":"Yanling Yu , Xiaodong Su , Tong Xing , Xuelin Zhao , Zhou Zhang , Wanqing Zhang , Xinping Wang , Weining Zhao , Mei Li , Fangyuan Zhao","doi":"10.1016/j.bioelechem.2025.108979","DOIUrl":"10.1016/j.bioelechem.2025.108979","url":null,"abstract":"<div><div>The most energetic light-induced charge-separation step in nature is driven by photosystem I (PSI), making this photosynthetic protein an attractive candidate for the development of semi-artificial energy conversion devices. Despite significant progress in semiconductor-free bio-photocathodes, the highest photocurrent density was only 322 ± 19 μA cm<sup>−2</sup>, achieved by integrating PSI within a pH-dependent poly(vinyl)imidazole Os(bispyridine)<sub>2</sub>Cl redox polymer (T Kothe et al., <em>Chem. Eur. J.</em>, 2014, 20, 11029). This study presents a more efficient PSI-based bio-photocathode by incorporating single-walled carbon nanotubes (SWCNTs) into the redox hydrogel composed of the same Osmium-containing redox polymer. The nanostructured redox hydrogel film with SWCNTs serving as electric scaffolds significantly improves the stability, loading amount, and heterogeneous electron transfer rate, resulting in a substantial increase in photocurrent density exceeding 2 mA cm<sup>−2</sup>, the highest achieved in a semiconductor-free PSI based photocathode to date. Bioelectrodes constructed by pre-depositing SWCNTs on the electrode surface via covalent bonds outperform those formed by co-immobilizing SWCNTs with the redox hydrogel. The dependence of photocurrent on light intensity and the photocurrent spectrum action demonstrate that the photocurrent unequivocally arises from PSI charge separation. This research lays a promising foundation for the development of semi-artificial photoelectrochemical devices for light-to-energy conversion.</div></div>","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"165 ","pages":"Article 108979"},"PeriodicalIF":4.8,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143739244","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

Interfacial extracellular electron uptake is linked to nitrate respiration in the marine heterotroph, Thalassospira xiamenensis SN3

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2025-03-26 DOI: 10.1016/j.bioelechem.2025.108976

Joshua D. Sackett , Gabriel P. Tonucci , Annette R. Rowe

Thalassospira species are ubiquitous marine bacteria with poorly understood ecology, and some have been implicated in iron corrosion. To better elucidate the mechanisms and ecological implications of extracellular electron transfer (EET) in oxidative processes, we conducted genomic and bioelectrochemical characterization of Thalassospira xiamenensis strain SN3, an obligate heterotroph isolated from coastal marine sediment cathode-oxidizing enrichments. Physiologic and genomic analyses indicate that SN3 lacks the capacity for lithoautotrophic growth and lacks homologs to genes canonically involved in EET. Bioelectrochemical characterization of SN3 cells shows that inward EET requires a terminal electron acceptor (respiration). Deletion of nitrate reductase catalytic subunit napA abolished current consumption and catalytic activity under nitrate-reducing conditions. Media exchange experiments demonstrate that inward EET in SN3 is facilitated by direct contact with the electrode, with a formal midpoint potential of −153 ± 16 mV vs. SHE. Through deletion of the formate dehydrogenase fdhABCD and electrochemical characterization of mutant cells, we show that inward EET is not a function of Fdh enzyme sorption to the electrode, as has been demonstrated for other organisms. This provides further evidence of a cell-mediated and contact-dependent EET mechanism. This work provides a foundation for investigating this metabolically versatile organism's yet uncharacterized mechanism of EET.

{"title":"Interfacial extracellular electron uptake is linked to nitrate respiration in the marine heterotroph, Thalassospira xiamenensis SN3","authors":"Joshua D. Sackett , Gabriel P. Tonucci , Annette R. Rowe","doi":"10.1016/j.bioelechem.2025.108976","DOIUrl":"10.1016/j.bioelechem.2025.108976","url":null,"abstract":"<div><div><em>Thalassospira</em> species are ubiquitous marine bacteria with poorly understood ecology, and some have been implicated in iron corrosion. To better elucidate the mechanisms and ecological implications of extracellular electron transfer (EET) in oxidative processes, we conducted genomic and bioelectrochemical characterization of <em>Thalassospira xiamenensis</em> strain SN3, an obligate heterotroph isolated from coastal marine sediment cathode-oxidizing enrichments. Physiologic and genomic analyses indicate that SN3 lacks the capacity for lithoautotrophic growth and lacks homologs to genes canonically involved in EET. Bioelectrochemical characterization of SN3 cells shows that inward EET requires a terminal electron acceptor (respiration). Deletion of nitrate reductase catalytic subunit <em>napA</em> abolished current consumption and catalytic activity under nitrate-reducing conditions. Media exchange experiments demonstrate that inward EET in SN3 is facilitated by direct contact with the electrode, with a formal midpoint potential of −153 ± 16 mV vs. SHE. Through deletion of the formate dehydrogenase <em>fdhABCD</em> and electrochemical characterization of mutant cells, we show that inward EET is not a function of Fdh enzyme sorption to the electrode, as has been demonstrated for other organisms. This provides further evidence of a cell-mediated and contact-dependent EET mechanism. This work provides a foundation for investigating this metabolically versatile organism's yet uncharacterized mechanism of EET.</div></div>","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"165 ","pages":"Article 108976"},"PeriodicalIF":4.8,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143748551","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

Hybridization chain reaction and CRISPR/Cas12a-integrated biosensor for precise Ago2 detection

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2025-03-26 DOI: 10.1016/j.bioelechem.2025.108975

Qiang Tang , Jiayi Zhang , Jialuo Pang , Yingying Huang , Ying Guan , Yuanxun Gong , Qianli Tang , Kai Zhang , Xianjiu Liao

This study introduces an innovative electrochemiluminescence (ECL) biosensor for the highly sensitive and specific detection of Argonaute 2 (Ago2) activity. Ago2, a key enzyme in the RNA interference (RNAi) pathway, plays a crucial role in gene regulation, and its dysregulation is associated with diseases such as cancer and viral infections. The biosensor integrates hybridization chain reaction (HCR) amplification and the CRISPR/Cas12a system, leveraging a multi-stage signal amplification strategy. The detection mechanism begins with Ago2-mediated cleavage of a designed hairpin RNA (HP-RNA), releasing single-stranded RNA (ssRNA) that triggers HCR. This amplification step generates long DNA polymers, which serve as activators for the CRISPR/Cas12a system. Cas12a's collateral cleavage activity amplifies the signal further by cleaving a DNA reporter labeled with a ruthenium-based luminophore, enhancing the ECL output. This dual amplification strategy achieves exceptional sensitivity, with a detection limit of 0.126 aM. The biosensor demonstrates excellent specificity, distinguishing Ago2 from other Argonaute proteins, and maintains high reproducibility and stability, retaining 94 % of its signal after two weeks of storage. Real-world applicability was confirmed by accurately detecting Ago2 in spiked cell lysates, with recovery rates exceeding 100 %. The combination of HCR, CRISPR/Cas12a, and ECL establishes a robust platform for biomarker detection, offering superior sensitivity and adaptability for clinical diagnostics, disease monitoring, and therapeutic evaluation. This biosensor represents a significant advancement in the development of next-generation diagnostic tools.

{"title":"Hybridization chain reaction and CRISPR/Cas12a-integrated biosensor for precise Ago2 detection","authors":"Qiang Tang , Jiayi Zhang , Jialuo Pang , Yingying Huang , Ying Guan , Yuanxun Gong , Qianli Tang , Kai Zhang , Xianjiu Liao","doi":"10.1016/j.bioelechem.2025.108975","DOIUrl":"10.1016/j.bioelechem.2025.108975","url":null,"abstract":"<div><div>This study introduces an innovative electrochemiluminescence (ECL) biosensor for the highly sensitive and specific detection of Argonaute 2 (Ago2) activity. Ago2, a key enzyme in the RNA interference (RNAi) pathway, plays a crucial role in gene regulation, and its dysregulation is associated with diseases such as cancer and viral infections. The biosensor integrates hybridization chain reaction (HCR) amplification and the CRISPR/Cas12a system, leveraging a multi-stage signal amplification strategy. The detection mechanism begins with Ago2-mediated cleavage of a designed hairpin RNA (HP-RNA), releasing single-stranded RNA (ssRNA) that triggers HCR. This amplification step generates long DNA polymers, which serve as activators for the CRISPR/Cas12a system. Cas12a's collateral cleavage activity amplifies the signal further by cleaving a DNA reporter labeled with a ruthenium-based luminophore, enhancing the ECL output. This dual amplification strategy achieves exceptional sensitivity, with a detection limit of 0.126 aM. The biosensor demonstrates excellent specificity, distinguishing Ago2 from other Argonaute proteins, and maintains high reproducibility and stability, retaining 94 % of its signal after two weeks of storage. Real-world applicability was confirmed by accurately detecting Ago2 in spiked cell lysates, with recovery rates exceeding 100 %. The combination of HCR, CRISPR/Cas12a, and ECL establishes a robust platform for biomarker detection, offering superior sensitivity and adaptability for clinical diagnostics, disease monitoring, and therapeutic evaluation. This biosensor represents a significant advancement in the development of next-generation diagnostic tools.</div></div>","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"165 ","pages":"Article 108975"},"PeriodicalIF":4.8,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143725330","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

A high-sensitivity label-free electrochemical aptasensor for point-of-care measurements of low-density lipoprotein in plasma based on aptamer and MXene-CMCS-Hemin nanocomposites

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2025-03-20 DOI: 10.1016/j.bioelechem.2025.108972

Jintao Liang , Shuaikang Dong , Xiaohong Tan , Junyan Gong , Xuyang Chen , Zhide Zhou , Guiyin Li

Cardiovascular disease (CVD) remains a significant worldwide health challenge, with mortality rates rising rapidly. Low-density lipoprotein (LDL) is a crucial serum biomarker for the early diagnosis of CVD, which can significantly improve outcomes and reduce mortality. Herein, a label-free electrochemical aptasensor for rapid detection of LDL was developed based on the titanium carbide–carboxymethyl chitosan–hemin (MXene-CMCS-Hemin) nanocomposites as the electrochemical signal probe. Firstly, gold nanoparticles (Au NPs) were electrodeposited onto a screen-printed carbon electrode (SPCE) to form a conductive substrate. Subsequently, the MXene-CMCS-Hemin nanocomposites were anchored onto the Au NPs/SPCE surface. Then LDL_Apt was immobilized on the surface of MXene-CMCS-Hemin/Au NPs/SPCE to construct the electrochemical aptasensor. When LDL specifically bound with the LDL_Apt to form LDL-LDL_Apt complexes, hindering the electron transfer and reducing the Hemin oxidation current, LDL detection can be achieved via differential pulse voltammetry (DPV). Under optimal circumstances, the changes of Hemin's oxidation current showed a good linear response with LDL concentration in the range of 0.1–4.0 μmol/L with a detection limit of 0.095 μmol/L (S/N = 3). The aptasensor demonstrated good performance with the relative errors of 0.60 % to 6.58 % for the direct detection of LDL in human serum samples, which offers a novel tool for the clinical diagnosis of CVD.

{"title":"A high-sensitivity label-free electrochemical aptasensor for point-of-care measurements of low-density lipoprotein in plasma based on aptamer and MXene-CMCS-Hemin nanocomposites","authors":"Jintao Liang , Shuaikang Dong , Xiaohong Tan , Junyan Gong , Xuyang Chen , Zhide Zhou , Guiyin Li","doi":"10.1016/j.bioelechem.2025.108972","DOIUrl":"10.1016/j.bioelechem.2025.108972","url":null,"abstract":"<div><div>Cardiovascular disease (CVD) remains a significant worldwide health challenge, with mortality rates rising rapidly. Low-density lipoprotein (LDL) is a crucial serum biomarker for the early diagnosis of CVD, which can significantly improve outcomes and reduce mortality. Herein, a label-free electrochemical aptasensor for rapid detection of LDL was developed based on the titanium carbide–carboxymethyl chitosan–hemin (MXene-CMCS-Hemin) nanocomposites as the electrochemical signal probe. Firstly, gold nanoparticles (Au NPs) were electrodeposited onto a screen-printed carbon electrode (SPCE) to form a conductive substrate. Subsequently, the MXene-CMCS-Hemin nanocomposites were anchored onto the Au NPs/SPCE surface. Then LDL<sub>Apt</sub> was immobilized on the surface of MXene-CMCS-Hemin/Au NPs/SPCE to construct the electrochemical aptasensor. When LDL specifically bound with the LDL<sub>Apt</sub> to form LDL-LDL<sub>Apt</sub> complexes, hindering the electron transfer and reducing the Hemin oxidation current, LDL detection can be achieved via differential pulse voltammetry (DPV). Under optimal circumstances, the changes of Hemin's oxidation current showed a good linear response with LDL concentration in the range of 0.1–4.0 μmol/L with a detection limit of 0.095 μmol/L (S/N = 3). The aptasensor demonstrated good performance with the relative errors of 0.60 % to 6.58 % for the direct detection of LDL in human serum samples, which offers a novel tool for the clinical diagnosis of CVD.</div></div>","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"165 ","pages":"Article 108972"},"PeriodicalIF":4.8,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143696806","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

The unusual formaldehyde-induced activation of [NiFe]-hydrogenase: Implications from protein film electrochemistry and infrared spectroscopy

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2025-03-19 DOI: 10.1016/j.bioelechem.2025.108974

Lei Wan , Yanxin Gao , Serena DeBeer , Olaf Rüdiger

Here we investigate how formaldehyde (HCHO), a known strong inhibitor of [FeFe]‑hydrogenases and a mild inhibitor of [NiFe]‑hydrogenases, may exert more complex effects on this group of metalloenzymes, which reversibly catalyze the 2H⁺/H₂ reaction. We investigated the [NiFe]‑hydrogenase Hyd-2 from E. coli using protein film electrochemistry, a technique that enables the measurement of enzyme activity when the enzyme is adequately adsorbed on the electrode. The effect of HCHO on the electrocatalytic performance of Hyd-2 is highly dependent on the buffer pH and the direction of catalysis. During H₂ production, HCHO consistently acts as an inhibitor of Hyd-2. However, this effect is reversed in acidic pH values, where HCHO can mildly enhance the electrocatalytic H₂ oxidation by Hyd-2. FTIR investigations did not detect any new redox intermediate resulting from the inhibition or activation. Therefore, we propose that HCHO - a natural electrophile that can readily react with nucleophiles and proton acceptors - may facilitate the transfer protons during the rapid transformation of different redox species participating in the catalytic cycle of [NiFe]‑hydrogenases.

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引用次数: 0

Structural bioelectrochemistry of direct electron transfer-type multimeric dehydrogenases: Basic principle and rational strategies

IF 4.8 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2025-03-17 DOI: 10.1016/j.bioelechem.2025.108973

Konatsu Ichikawa, Taiki Adachi, Keisei Sowa

Direct electron transfer (DET)-type bioelectrocatalysis, a coupled enzymatic and electrode reaction without redox mediators, provides insights into enzyme properties that facilitate the construction of efficient biomimetic devices. Because many DET-type multimeric dehydrogenases are membrane-bound proteins, obtaining the overall steric structures of these enzymes using conventional X-ray crystallography has proved difficult for many decades. Novel cryo-electron microscopy (cryo-EM) and single-particle image analysis have recently been developed that enable elucidation of the overall structure of membrane-bound DET-type multimeric dehydrogenases. In particular, “structural bioelectrochemistry,” a fusion of structural biology and bioelectrochemistry, has enabled rapid hypothesis testing via the analysis of three-dimensional (3D) structures using enzyme engineering and electrochemistry. This review outlines critical related studies in the last decade and the epoch-making breakthroughs leading to next-generation applications.

引用次数: 0

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