Pub Date : 2025-01-27DOI: 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}
Pub Date : 2025-01-26DOI: 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}
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}
Pub Date : 2025-01-25DOI: 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}
Pub Date : 2025-01-23DOI: 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.
{"title":"Advanced cortisol detection: A cMWCNTs-enhanced MB@Zr-MOF ratiometric electrochemical aptasensor","authors":"Runran Ma , Te Li , Xueying Li , Jianwei Han , Xin Zhang , Tingting Di , Jiabo Wang , Weijun Kong","doi":"10.1016/j.bioelechem.2025.108914","DOIUrl":"10.1016/j.bioelechem.2025.108914","url":null,"abstract":"<div><div>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 <em>via</em> 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)<sub>6</sub>]<sup>3−/4−</sup> was basically unchanged. The ratio of the electrochemical signals of [Fe(CN)<sub>6</sub>]<sup>3−/4−</sup> 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.</div></div>","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"163 ","pages":"Article 108914"},"PeriodicalIF":4.8,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143051149","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}
Pub Date : 2025-01-22DOI: 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.
{"title":"An electrochemical aptasensor based on bimetallic carbon nanocomposites AuPt@rGO for ultrasensitive detection of adenosine on portable potentiostat","authors":"Zheng Gong , Hongli Zhao , Yi Mao , Fangfang Zhou , Zehui Shi , Minbo Lan","doi":"10.1016/j.bioelechem.2025.108906","DOIUrl":"10.1016/j.bioelechem.2025.108906","url":null,"abstract":"<div><div>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.</div></div>","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"163 ","pages":"Article 108906"},"PeriodicalIF":4.8,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143035346","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}
Pub Date : 2025-01-21DOI: 10.1016/j.bioelechem.2025.108913
Carina S.P. Vieira, Marcela A. Segundo, Alberto N. Araújo
The ability of the living world to flourish in the face of constant exposure to dangerous chemicals depends on the management ability of a widespread group of enzymes known as heme-thiolate monooxygenases or cytochrome P450 superfamily. About three-quarters of all reactions determining the metabolism of endogenous compounds, of those carried in foods, of taken drugs, or even of synthetic chemicals discarded into the environment depend on their catalytic performance. The chromatographic and (photo)luminometric methods routinely used as predictive and analytical tools in laboratories have significant drawbacks ranging from limited shelf-life of reagents, use of synthetic substrates, laborious and tedious procedures for highly sensitive detection. In this review, alternative electrochemical biosensors using the cytochrome P450 enzymes as bio-element are emphasized in their main aspects as well regarding their implementation and usefulness. Despite the various schemes proposed for the implementation, reports on real applications are scant for several reasons, including low reaction rates, broad substrate specificity, uncoupling reactions occurrence, and the need for expensive electron transfer partners to promote electron transfer. Finally, the prospect for future developments is introduced, focusing on integrating miniaturized systems with electrochemical techniques, alongside optimizing enzyme immobilization methods and electrode modifications to improve enzymatic stability and enhance sensor reliability. This progress represents a crucial step towards the creation of portable biosensors that mimic human physiological responses, supporting the precision medicine approach.
{"title":"Cytochrome P450 electrochemical biosensors transforming in vitro metabolism testing – Opportunities and challenges","authors":"Carina S.P. Vieira, Marcela A. Segundo, Alberto N. Araújo","doi":"10.1016/j.bioelechem.2025.108913","DOIUrl":"10.1016/j.bioelechem.2025.108913","url":null,"abstract":"<div><div>The ability of the living world to flourish in the face of constant exposure to dangerous chemicals depends on the management ability of a widespread group of enzymes known as heme-thiolate monooxygenases or cytochrome P450 superfamily. About three-quarters of all reactions determining the metabolism of endogenous compounds, of those carried in foods, of taken drugs, or even of synthetic chemicals discarded into the environment depend on their catalytic performance. The chromatographic and (photo)luminometric methods routinely used as predictive and analytical tools in laboratories have significant drawbacks ranging from limited shelf-life of reagents, use of synthetic substrates, laborious and tedious procedures for highly sensitive detection. In this review, alternative electrochemical biosensors using the cytochrome P450 enzymes as bio-element are emphasized in their main aspects as well regarding their implementation and usefulness. Despite the various schemes proposed for the implementation, reports on real applications are scant for several reasons, including low reaction rates, broad substrate specificity, uncoupling reactions occurrence, and the need for expensive electron transfer partners to promote electron transfer. Finally, the prospect for future developments is introduced, focusing on integrating miniaturized systems with electrochemical techniques, alongside optimizing enzyme immobilization methods and electrode modifications to improve enzymatic stability and enhance sensor reliability. This progress represents a crucial step towards the creation of portable biosensors that mimic human physiological responses, supporting the precision medicine approach.</div></div>","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"163 ","pages":"Article 108913"},"PeriodicalIF":4.8,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143035348","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}
<div><div>Heparin concentration <span><math><mrow><mi>c</mi></mrow></math></span> in a blood extracorporeal circulation has been real-timely predicted based on the relaxation strength <span><math><mrow><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mi>m</mi></msub></mrow></math></span> at relaxation frequency <span><math><mrow><msub><mi>f</mi><mi>m</mi></msub></mrow></math></span> extracted by relaxation time distribution (RTD). The simulated extracorporeal circulation was conducted to optimize the number of <span><math><mrow><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mi>m</mi></msub></mrow></math></span> for the prediction of <em>c</em> using the porcine whole blood (WB) and low-leukocyte and −platelet blood (LLPB) under the condition of the gradual increment of <span><math><mrow><mi>c</mi></mrow></math></span> from 0 to 8 U/mL with constant flow rate and blood temperature. The experimental results show that among the three relaxation strengths <span><math><mrow><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mn>1</mn></msub></mrow></math></span>, <span><math><mrow><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mn>2</mn></msub></mrow></math></span> and <span><math><mrow><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mn>3</mn></msub></mrow></math></span> (in ascending order of frequency), <span><math><mrow><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mn>2</mn></msub></mrow></math></span> at <span><math><mrow><msub><mi>f</mi><mn>2</mn></msub></mrow></math></span> = 5.2 ∼ 6.2 MHz and <span><math><mrow><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mn>3</mn></msub></mrow></math></span> at <span><math><mrow><msub><mi>f</mi><mn>3</mn></msub></mrow></math></span> = 42 ∼ 50 MHz were correlated to <span><math><mrow><mi>c</mi></mrow></math></span>. The <span><math><mrow><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mn>3</mn></msub></mrow></math></span> was decreasing with increasing <span><math><mrow><mi>c</mi></mrow></math></span> in both cases, which was influenced by the plasma macromolecular concentrations, while the <span><math><mrow><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mn>2</mn></msub></mrow></math></span> was increased with increasing <em>c</em> in WB case but was hardly changed in LLPB case because the <span><math><mrow><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mn>2</mn></msub></mrow></math></span> is influenced by the blood cell concentrations and the shape changes of blood cell membranes. Heparin concentration <span><math><mrow><mi>c</mi></mrow></math></span> is estimated by the linear regression formula <span><math><mrow><msup><mrow><mi>c</mi></mrow><mrow><mi>P</mi><mi>R</mi><mi>E</mi></mrow></msup><mo>=</mo><msub><mi>a</mi><mn>1</mn></msub><msub><mrow><mo>(</mo><mi>Δ</mi><mi>ε</mi></mrow><mn>2</mn></msub><mo>-</mo><msubsup><mrow><mi>Δ</mi><mi>ε</mi></mrow><mrow><mn>2</mn></mrow><mrow><mi>c</mi><mo>=</mo><mn>0</mn></mrow></msubsup><mrow><mo>)</mo><mo>+</mo></mrow><msub><mi>a</mi><mn>2</mn></msub><mrow><mo>(</mo><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mn>3</mn></msub><mo>-</mo><msubsup><mrow><
{"title":"Real-time prediction of heparin concentration in blood extracorporeal circulation by relaxation time distribution (RTD)","authors":"Soichiro Ueno , Daisuke Kawashima , Katsuhiro Matsuura , Hiromichi Obara , Ryou Tanaka , Masahiro Takei","doi":"10.1016/j.bioelechem.2025.108912","DOIUrl":"10.1016/j.bioelechem.2025.108912","url":null,"abstract":"<div><div>Heparin concentration <span><math><mrow><mi>c</mi></mrow></math></span> in a blood extracorporeal circulation has been real-timely predicted based on the relaxation strength <span><math><mrow><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mi>m</mi></msub></mrow></math></span> at relaxation frequency <span><math><mrow><msub><mi>f</mi><mi>m</mi></msub></mrow></math></span> extracted by relaxation time distribution (RTD). The simulated extracorporeal circulation was conducted to optimize the number of <span><math><mrow><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mi>m</mi></msub></mrow></math></span> for the prediction of <em>c</em> using the porcine whole blood (WB) and low-leukocyte and −platelet blood (LLPB) under the condition of the gradual increment of <span><math><mrow><mi>c</mi></mrow></math></span> from 0 to 8 U/mL with constant flow rate and blood temperature. The experimental results show that among the three relaxation strengths <span><math><mrow><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mn>1</mn></msub></mrow></math></span>, <span><math><mrow><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mn>2</mn></msub></mrow></math></span> and <span><math><mrow><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mn>3</mn></msub></mrow></math></span> (in ascending order of frequency), <span><math><mrow><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mn>2</mn></msub></mrow></math></span> at <span><math><mrow><msub><mi>f</mi><mn>2</mn></msub></mrow></math></span> = 5.2 ∼ 6.2 MHz and <span><math><mrow><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mn>3</mn></msub></mrow></math></span> at <span><math><mrow><msub><mi>f</mi><mn>3</mn></msub></mrow></math></span> = 42 ∼ 50 MHz were correlated to <span><math><mrow><mi>c</mi></mrow></math></span>. The <span><math><mrow><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mn>3</mn></msub></mrow></math></span> was decreasing with increasing <span><math><mrow><mi>c</mi></mrow></math></span> in both cases, which was influenced by the plasma macromolecular concentrations, while the <span><math><mrow><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mn>2</mn></msub></mrow></math></span> was increased with increasing <em>c</em> in WB case but was hardly changed in LLPB case because the <span><math><mrow><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mn>2</mn></msub></mrow></math></span> is influenced by the blood cell concentrations and the shape changes of blood cell membranes. Heparin concentration <span><math><mrow><mi>c</mi></mrow></math></span> is estimated by the linear regression formula <span><math><mrow><msup><mrow><mi>c</mi></mrow><mrow><mi>P</mi><mi>R</mi><mi>E</mi></mrow></msup><mo>=</mo><msub><mi>a</mi><mn>1</mn></msub><msub><mrow><mo>(</mo><mi>Δ</mi><mi>ε</mi></mrow><mn>2</mn></msub><mo>-</mo><msubsup><mrow><mi>Δ</mi><mi>ε</mi></mrow><mrow><mn>2</mn></mrow><mrow><mi>c</mi><mo>=</mo><mn>0</mn></mrow></msubsup><mrow><mo>)</mo><mo>+</mo></mrow><msub><mi>a</mi><mn>2</mn></msub><mrow><mo>(</mo><msub><mrow><mi>Δ</mi><mi>ε</mi></mrow><mn>3</mn></msub><mo>-</mo><msubsup><mrow><","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"163 ","pages":"Article 108912"},"PeriodicalIF":4.8,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143035352","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}
A micro-nano sharkskin like film (Cu-MNS-FA) was synthesized on copper surface through chemical etching followed by formate passivation, and its anticorrosive, antibacterial and thermal conductivity properties were investigated. Results show that after 7 d of exposure to nature, Pseudomonas aeruginosa and Desulfovibrio vulgaris seawater, the charge transfer resistance of Cu-MNS-FA is more than three times higher than that of unmodified copper. In particular, in D. vulgaris seawater, the Rct value of modified copper is 7 times higher than that of unmodified copper after the same exposure duration. The counts of sessile cells, specifically P. aeruginosa and D. vulgaris, on the surface of modified copper are reduced by > 88 % after 3 days of immersion. Furthermore, thermal conductivity remains 10 % higher than that of untreated copper after 7 d of immersion. This film improves the performance characteristics of copper in seawater heat exchange systems.
{"title":"Development of micro-nanostructured film with antibacterial, anticorrosive and thermal conductivity properties on copper surface","authors":"Li Lai, Muqiu Xia, Mengyu Fu, Yuanyuan Gao, Jiahao Sun, Guangzhou Liu, Shiqiang Chen","doi":"10.1016/j.bioelechem.2025.108905","DOIUrl":"10.1016/j.bioelechem.2025.108905","url":null,"abstract":"<div><div>A micro-nano sharkskin like film (Cu-MNS-FA) was synthesized on copper surface through chemical etching followed by formate passivation, and its anticorrosive, antibacterial and thermal conductivity properties were investigated. Results show that after 7 d of exposure to nature, <em>Pseudomonas aeruginosa</em> and <em>Desulfovibrio vulgaris</em> seawater, the charge transfer resistance of Cu-MNS-FA is more than three times higher than that of unmodified copper. In particular, in <em>D. vulgaris</em> seawater, the <em>R</em><sub>ct</sub> value of modified copper is 7 times higher than that of unmodified copper after the same exposure duration. The counts of sessile cells, specifically <em>P. aeruginosa</em> and <em>D. vulgaris</em>, on the surface of modified copper are reduced by > 88 % after 3 days of immersion. Furthermore, thermal conductivity remains 10 % higher than that of untreated copper after 7 d of immersion. This film improves the performance characteristics of copper in seawater heat exchange systems.</div></div>","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"163 ","pages":"Article 108905"},"PeriodicalIF":4.8,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143027451","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}
Pub Date : 2025-01-15DOI: 10.1016/j.bioelechem.2025.108909
Stefano Gianvittorio , Marco Malferrari , Horst Pick , Stefania Rapino , Andreas Lesch
Print-Light-Synthesis (PLS) combines the inkjet printing of a ruthenium precursor ink with the simultaneous photo-induced generation of ruthenium oxide films. During PLS, inkjet-printing generates on conductive as well as insulating substrates micrometer-thin reaction volumes that contain with high precision defined precursor loadings. Upon direct UV light irradiation, the Ru precursor converts to RuO2 while all other ink components escape in the gas phase. No post PLS processes are required, and the as-obtained RuO2 films can be immediately used as electrochemical devices. Two-dimensional RuO2 patterns with micrometric resolution and highly-controlled ruthenium loadings (few µg/cm2) are realized. Thin RuO2 films are generated on insulating substrates, such as polyimide, as well as individual RuO2 particles on conductive substrates, such as graphene layers. The RuO2 films are characterized by electron microscopy and spectroscopic techniques. The sensoristic applicability of the PLS-RuO2 electrodes is demonstrated by potentiometric pH sensing in cell cultures and amperometric detection of L-cysteine. For pH sensing the RuO2 film electrodes show Nernstian sensitivity. L-cysteine detection of RuO2-modified graphene electrodes showed an electrocatalytical effect and resulted in the possibility of selectively detecting L-Cysteine also in presence of the interfering compound uric acid.
{"title":"Print-Light-Synthesis of ruthenium oxide thin film electrodes for electrochemical sensing applications","authors":"Stefano Gianvittorio , Marco Malferrari , Horst Pick , Stefania Rapino , Andreas Lesch","doi":"10.1016/j.bioelechem.2025.108909","DOIUrl":"10.1016/j.bioelechem.2025.108909","url":null,"abstract":"<div><div>Print-Light-Synthesis (PLS) combines the inkjet printing of a ruthenium precursor ink with the simultaneous photo-induced generation of ruthenium oxide films. During PLS, inkjet-printing generates on conductive as well as insulating substrates micrometer-thin reaction volumes that contain with high precision defined precursor loadings. Upon direct UV light irradiation, the Ru precursor converts to RuO<sub>2</sub> while all other ink components escape in the gas phase. No post PLS processes are required, and the as-obtained RuO<sub>2</sub> films can be immediately used as electrochemical devices. Two-dimensional RuO<sub>2</sub> patterns with micrometric resolution and highly-controlled ruthenium loadings (few µg/cm<sup>2</sup>) are realized. Thin RuO<sub>2</sub> films are generated on insulating substrates, such as polyimide, as well as individual RuO<sub>2</sub> particles on conductive substrates, such as graphene layers. The RuO<sub>2</sub> films are characterized by electron microscopy and spectroscopic techniques. The sensoristic applicability of the PLS-RuO<sub>2</sub> electrodes is demonstrated by potentiometric pH sensing in cell cultures and amperometric detection of L-cysteine. For pH sensing the RuO<sub>2</sub> film electrodes show Nernstian sensitivity. L-cysteine detection of RuO<sub>2</sub>-modified graphene electrodes showed an electrocatalytical effect and resulted in the possibility of selectively detecting L-Cysteine also in presence of the interfering compound uric acid.</div></div>","PeriodicalId":252,"journal":{"name":"Bioelectrochemistry","volume":"163 ","pages":"Article 108909"},"PeriodicalIF":4.8,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143035350","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}
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