Direct Electrochemistry of Proteins and Enzymes

Ferapontova, Elena E.; Shleev, Sergey; Ruzgas, Tautgirdas; Stoica, Leonard; Christenson, Andreas; Tkac, Jan; Yaropolov, A. I.; Gorton, Lo

doi:10.1016/s1871-0069(05)01016-5

Cited by 69 publications

(60 citation statements)

References 427 publications

Supporting

Mentioning

Contrasting

Unclassified

Order By: Relevance

“…In this form of electron transfer, the redox enzymes that possess tightly bound cofactors in the active site, can deliver the electrons directly at the electrode. The first reports on DET were published over 30 years ago [13] and recent reports are also available on a wide range of enzymes [14][15][16][17][18]. DET has been reported for about 40 redox enzymes, including laccase, peroxidases and complex multi-cofactor-containing enzymes [13].…”

Section: Direct Electron Transfer (Det)mentioning

confidence: 99%

“…The first reports on DET were published over 30 years ago [13] and recent reports are also available on a wide range of enzymes [14][15][16][17][18]. DET has been reported for about 40 redox enzymes, including laccase, peroxidases and complex multi-cofactor-containing enzymes [13]. Most extensively studied and best characterized enzymes for DET belong to the group of peroxidases [19][20][21][22][23][24][25][26][27][28][29].…”

Section: Direct Electron Transfer (Det)mentioning

confidence: 99%

See 1 more Smart Citation

Enzymatic Electrosynthesis: An Overview on the Progress in Enzyme- Electrodes for the Production of Electricity, Fuels and Chemicals

Satyawali¹

2013

J Microbial Biochem Technol

View full text Add to dashboard Cite

Recent interest in the field of biocommodities production through bioelectrochemical systems has generated interest in the enzyme catalyzed redox reactions. Enzyme catalyzed electrodes are well established as sensors and power generators. However, a paradigm shift in recent science towards the production of useful chemicals has changed the face of biofuel cells, keeping the fuels or chemicals production in the upfront. This review article comprehensively presents the progress in the field of enzyme-electrodes for the production of electricity, fuels and chemicals with an aim to represent a practical outline for understanding the use of single or multiple redox enzymes as electrocatalysts for their electron transfer onto electrodes. It also provides the state-of-the-art information regarding the different existing processes to fabricate enzyme electrodes. Successfully-achieved electroenzymatic anodic and cathodic reactions are further discussed, together with their potential applications. Particular focus was made on the novel single/multiple enzyme systems towards product synthesis and other applications. Finally, techno-economic and environmental elements for industrial processing with enzyme catalyzed bioelectrochemical system (e-BES) are anticipated, in order to provide useful strategies for further development of this technology.

show abstract

Section: Direct Electron Transfer (Det)mentioning

confidence: 99%

Section: Direct Electron Transfer (Det)mentioning

confidence: 99%

Enzymatic Electrosynthesis: An Overview on the Progress in Enzyme- Electrodes for the Production of Electricity, Fuels and Chemicals

Satyawali¹

2013

J Microbial Biochem Technol

View full text Add to dashboard Cite

show abstract

“…132 Among them are copper oxidases (laccases, tyrosinase, billirubin oxidase), heme-containing enzymes (cytochrome C peroxidase, fructose dehydrogenase, cellobiose dehydrogenase) and some ironsulphur cluster containing hydrogenases. 133 However, even for these enzymes a proper orientation of the biomolecule on the suitable electrode surface is necessary for the establishment of effective ET.…”

Section: Direct Electron Transfermentioning

confidence: 99%

Facilitating electron transfer in bioelectrocatalytic systems

Sekretaryova¹

2016

View full text Add to dashboard Cite

During the course of the research underlying this thesis, Alina Sekretaryova was enrolled in Forum Scientium, a multidisciplinary doctoral programme at Linköping University, Sweden Alina Sekretaryova, 2016, unless otherwise noted. Cover design by Alina Sekretaryova Linköping studies in science and technology Dissertation No. 1738 Printed in Sweden by LiU-Tryck, Linköping, Sweden, 2016 iii ABSTRACT Bioelectrocatalytic systems are based on biological entities, such as enzymes, whole cells, parts of cells or tissues, which catalyse electrochemical processes that involve the interaction between chemical change and electrical energy. In all cases, enzymes, isolated or residing inside cells or part of cells, implement biocatalysis. Electron transfer phenomena, within the protein molecules and between biological redox systems and electronics, enable the development of various bioelectrocatalytic systems, which can be used both for fundamental investigations of enzymatic biological processes by electrochemical methods and for applied purposes, such as power generation, bioremediation, chemical synthesis and biosensing.Electrical communication between the biocatalysts redox centre and an electrode is essential for the functioning of the system. This can be established using two main mechanisms: indirect electron transfer and direct electron transfer. The efficiency of the electron transfer influences important parameters such as the turnover rate of the biocatalyst, the generated current density and partially the stability of the system. These in turn determine the response time, sensitivity, detection limit and operational stability of biosensors or the power densities and current output of biofuel cells, and hence they should be carefully considered when designing bioelectrocatalytic systems.This thesis focuses on approaches that facilitate electron transfer in bioelectrocatalytic systems based on mediated and direct electron transfer mechanisms. Both fundamental aspects of electron transfer in bioelectrocatalytic systems and applications of such systems for biosensing and power generation are considered. First, a new hydrophobic mediator for oxidases, unsubstituted phenothiazine, and its improved electron transfer properties in comparison with commonly used mediators are discussed. Application of the mediator in electrochemical biosensors is demonstrated by glucose, lactate and cholesterol sensing. Utilisation of mediated biocatalytic cholesterol oxidation as the anodic reaction for the construction of a biofuel cell, acting as a power supply and an analytical device at the same time, is investigated as a "self-powered" biosensor. In addition, the enhancement of mediated bioelectrocatalysis by the employment of microelectrodes as a transducer is examined. The effect of surface roughness on the current response of the microelectrodes under conditions of convergent diffusion is considered. The applicability of the laccase-based system for total phenol analysis of weakly supported water is demonstrated. Finally, a...

show abstract

“…However, direct electron transfer between redox enzyme and electrode close to the electrode surface can be very slow due to the insulating protein shell, shielding the enzyme active site (see section 3.1.1). Therefore, from 1060 known oxidoreductases 22 only 50 -60 are able to transfer electrons directly between the active site and the electrode surface 23 due to the close distance, no longer then 10 -15 Å. 20 Efficiency of direct electron transfer depends not only on the distance between the active site of the enzyme and the electrode, but also on the properties of the electrode material and on the immobilization technique.…”

Section: 'Third-generation' Biosensorsmentioning

confidence: 99%

Novel reagentless electrodes for biosensing

Sekretaryova¹

2014

View full text Add to dashboard Cite

Analytical chemical information is needed in all areas of human activity including health care, pharmacology, food control and environmental chemistry. Today one of the main challenges in analytical chemistry is the development of methods to perform accurate and sensitive rapid analysis and monitoring of analytes in 'real' samples. Electrochemical biosensors are ideally suited for these applications.Despite the wide application of electrochemical biosensors, they have some limitations. Thus, there is a demand on improvement of biosensor performance together with a necessity of simplification required for their mass production. In this thesis the work is focused on the development of electrochemical sensors with improved performance applicable for mass production, e.g. by screen printing.Biosensors using immobilized oxidases as the bio-recognition element are among the most widely used electrochemical devices. Electrical communication between redox enzymes and electrodes can be established by using natural or synthetic electron carriers as mediators. However, sensors based on soluble electronshuttling redox couples have low operational stability due to the leakage of water-soluble mediators to the solution. We have found a new hydrophobic mediator for oxidases -unsubstituted phenothiazine. Phenothiazine and glucose oxidase, lactate oxidase or cholesterol oxidase were successfully co-immobilized in a sol-gel membrane on a screen-printed electrode to construct glucose, lactate and cholesterol biosensors, respectively. All elaborated biosensors with phenothiazine as a mediator exhibited long-term operational stability. A kinetic study of the mediator has shown that phenothiazine is able to function as an efficient mediator in oxidase-based biosensors.To improve sensitivity of the biosensors and simplify their production we have developed a simple approach for production of graphite microelectrode arrays. Arrays of microband electrodes were produced by screen printing followed by scissor cutting, which enabled the realization of microband arrays at the cut edge. The analytical performance of the system is illustrated by the detection of ascorbic acid through direct oxidation and by detection of glucose using a phenothiazine mediated glucose biosensor. Both systems showed enhanced sensitivity due to improved mass transport. Moreover, the developed approach can be adapted to automated electrode recovery.Finally, two enzyme-based electrocatalytic systems with oxidation and reduction responses, respectively, have been combined into a fuel cell generating a current as an analytical output (a so-called self-powered biosensor). This was possible as a result of the development of the phenothiazine mediated enzyme electrodes, Abstract which enabled the construction of a cholesterol biosensor with self-powered configuration. The biosensor generates a current when analyte (cholesterol) is added to the cell. The biosensor has been applied for whole plasma analysis.All developed concepts in the thesis are compatible with ...

show abstract

Direct Electrochemistry of Proteins and Enzymes

Cited by 69 publications

References 427 publications

Enzymatic Electrosynthesis: An Overview on the Progress in Enzyme- Electrodes for the Production of Electricity, Fuels and Chemicals

Enzymatic Electrosynthesis: An Overview on the Progress in Enzyme- Electrodes for the Production of Electricity, Fuels and Chemicals

Facilitating electron transfer in bioelectrocatalytic systems

Novel reagentless electrodes for biosensing

Contact Info

Product

Resources

About