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Catalysts
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Enzymatic Bioelectrocatalysis
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Enzymatic Bioelectrocatalysis

A special issue of Catalysts (ISSN 2073-4344). This special issue belongs to the section "Biocatalysis".

Deadline for manuscript submissions: closed (31 March 2021) | Viewed by 31131

Printed Edition Available!
A printed edition of this Special Issue is available here.

Special Issue Editors

Dr. Elisabeth Lojou

E-Mail Website
Guest Editor
National Center for Scientific Research (CNRS), Aix Marseille, University, BIP, UMR 7281, 31 Chemin Aiguier, 13009 Marseille, France
Interests: bioelectrochemistry; redox protein; redox enzyme; hydrogenase; multi copper oxidase; electrode nanostructuration; biofuel cells
Dr. Xinxin Xiao

E-Mail Website
Guest Editor
Department of Chemistry and Bioscience, Aalborg University, Fredrik Bajers Vej 7H, 9220 Aalborg, Denmark
Interests: nanoporous gold; glucose biosensor; biofuel cell; bioelectrochemistry; biocatalysis; electro-catalysis

Special Issue Information

Dear colleagues,

Featuring a mild process and high selectivity, enzyme bioelectrocatalysis employing oxidoreductases immobilized on conductive surfaces is increasingly playing a vital role in a wide scope of applications. Enzyme bioelectrocatalysis is the core for devices such as biosensors and biofuel cells, which are drawing considerable attention towards sustainable sensing and energy production. A wide range of sophisticated reactions, such as chiral compound synthesis and CO2 and N2 fixation, can be accomplished with enzyme bioelectrocatalysis. Last but not least, redox enzymes are sources of inspiration for new non-noble metal electrocatalysts.

Fundamental investigations are required to alleviate the main limitations of enzyme bioelectrocatalysis, i.e., low catalytic efficiency and weak stability. In addition to the investigation of mechanisms of enzyme electrocatalysis, the molecular basis knowledge of the efficient electronic communication between enzymes and a conductive electrode is a mandatory step. Electrochemistry coupling with other in situ spectroscopic methods, as well as theoretical modeling, is expected to bring forth a fundamental understanding of enzyme conformation and dynamics on the electrode. Nanostructured electrodes and materials are significantly pushing enzyme bioelectrocatalysis forward but need further investigation to determine the molecular basis for bioelectrocatalysis optimization and stabilization. New enzyme identification in biodiversity and enzyme engineering will certainly enhance the toolbox of bioelectrochemists for high performance. Enzyme cascade broadens the scope of biocatalysis, which has also seen tremendous progress recently.

The Special Issue will focus on fundamentals, developments, and applications of enzyme bioelectrocatalysis. Reviews and original research papers are accepted. Potential topics include but are not limited to:

  • Bioengineered enzymes for bioelectrocatalysis;
  • Enzyme bioelectrocatalysis enabled high-value products, such as achiral ketone reduction for chiral alcohols and CO2 and N2 fixation;
  • Enzyme immobilization for improved bioelectrocatalysis;
  • Enzymatic biofuel cells;
  • Enzymatic biosensors;
  • Fundamentals of enzyme bioelectrochemistry;
  • Strategies for enzyme stabilization;
  • In situ and in operando techniques for enzyme bioelectrode characterization;
  • Cell design for bioelectrocatalytic reaction, such as fluidic cells;
  • Biodevices based on enzyme bioelectrocatalysis;
  • Enzyme cascade for bioelectrocatalysis;
  • Reaction media such as ionic liquid for enzyme bioelectrocatalysis;
  • Nanomaterials in enzyme bioelectrocatalysis;
  • Theoretical modeling of bioelectrocatalysis.

Dr. Elisabeth Lojou
Dr. Xinxin Xiao
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Catalysts is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • Bioelectrochemistry
  • Bioengineering
  • Biofuel cell
  • Biosensor
  • CO2 fixation
  • Direct electron transfer
  • Electron transfer
  • Enzyme bioelectrocatalysis
  • Enzyme cascade
  • Enzyme immobilization
  • Enzyme stability
  • Fluidic bioelectrocatalysis
  • In situ spectroscopies coupled to electrochemistry
  • Mediated electron transfer
  • NADH regeneration
  • Nanomaterials
  • N2 fixation
  • Protein film voltammetry
  • Theoretical modeling

Published Papers (7 papers)

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Editorial

Jump to: Review

2 pages, 154 KiB  
Editorial
Enzymatic Bioelectrocatalysis
by Elisabeth Lojou and Xinxin Xiao
Catalysts 2021, 11(11), 1373; https://doi.org/10.3390/catal11111373 - 14 Nov 2021
Cited by 4 | Viewed by 1570
Abstract
Enzymatic bioelectrocatalysis relies on immobilizing oxidoreductases on electrode surfaces, leading to different applications, such as biosensors [...] Full article
(This article belongs to the Special Issue Enzymatic Bioelectrocatalysis)

Review

Jump to: Editorial

45 pages, 5154 KiB  
Review
From Enzyme Stability to Enzymatic Bioelectrode Stabilization Processes
by Charlène Beaufils, Hiu-Mun Man, Anne de Poulpiquet, Ievgen Mazurenko and Elisabeth Lojou
Catalysts 2021, 11(4), 497; https://doi.org/10.3390/catal11040497 - 14 Apr 2021
Cited by 27 | Viewed by 7036
Abstract
Bioelectrocatalysis using redox enzymes appears as a sustainable way for biosensing, electricity production, or biosynthesis of fine products. Despite advances in the knowledge of parameters that drive the efficiency of enzymatic electrocatalysis, the weak stability of bioelectrodes prevents large scale development of bioelectrocatalysis. [...] Read more.
Bioelectrocatalysis using redox enzymes appears as a sustainable way for biosensing, electricity production, or biosynthesis of fine products. Despite advances in the knowledge of parameters that drive the efficiency of enzymatic electrocatalysis, the weak stability of bioelectrodes prevents large scale development of bioelectrocatalysis. In this review, starting from the understanding of the parameters that drive protein instability, we will discuss the main strategies available to improve all enzyme stability, including use of chemicals, protein engineering and immobilization. Considering in a second step the additional requirements for use of redox enzymes, we will evaluate how far these general strategies can be applied to bioelectrocatalysis. Full article
(This article belongs to the Special Issue Enzymatic Bioelectrocatalysis)
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26 pages, 2793 KiB  
Review
Direct Electrochemical Enzyme Electron Transfer on Electrodes Modified by Self-Assembled Molecular Monolayers
by Xiaomei Yan, Jing Tang, David Tanner, Jens Ulstrup and Xinxin Xiao
Catalysts 2020, 10(12), 1458; https://doi.org/10.3390/catal10121458 - 14 Dec 2020
Cited by 28 | Viewed by 4792
Abstract
Self-assembled molecular monolayers (SAMs) have long been recognized as crucial “bridges” between redox enzymes and solid electrode surfaces, on which the enzymes undergo direct electron transfer (DET)—for example, in enzymatic biofuel cells (EBFCs) and biosensors. SAMs possess a wide range of terminal groups [...] Read more.
Self-assembled molecular monolayers (SAMs) have long been recognized as crucial “bridges” between redox enzymes and solid electrode surfaces, on which the enzymes undergo direct electron transfer (DET)—for example, in enzymatic biofuel cells (EBFCs) and biosensors. SAMs possess a wide range of terminal groups that enable productive enzyme adsorption and fine-tuning in favorable orientations on the electrode. The tunneling distance and SAM chain length, and the contacting terminal SAM groups, are the most significant controlling factors in DET-type bioelectrocatalysis. In particular, SAM-modified nanostructured electrode materials have recently been extensively explored to improve the catalytic activity and stability of redox proteins immobilized on electrochemical surfaces. In this report, we present an overview of recent investigations of electrochemical enzyme DET processes on SAMs with a focus on single-crystal and nanoporous gold electrodes. Specifically, we consider the preparation and characterization methods of SAMs, as well as SAM applications in promoting interfacial electrochemical electron transfer of redox proteins and enzymes. The strategic selection of SAMs to accord with the properties of the core redox protein/enzymes is also highlighted. Full article
(This article belongs to the Special Issue Enzymatic Bioelectrocatalysis)
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Graphical abstract

16 pages, 2418 KiB  
Review
Rational Surface Modification of Carbon Nanomaterials for Improved Direct Electron Transfer-Type Bioelectrocatalysis of Redox Enzymes
by Hongqi Xia and Jiwu Zeng
Catalysts 2020, 10(12), 1447; https://doi.org/10.3390/catal10121447 - 10 Dec 2020
Cited by 12 | Viewed by 2435
Abstract
Interfacial electron transfer between redox enzymes and electrodes is a key step for enzymatic bioelectrocatalysis in various bioelectrochemical devices. Although the use of carbon nanomaterials enables an increasing number of redox enzymes to carry out bioelectrocatalysis involving direct electron transfer (DET), the role [...] Read more.
Interfacial electron transfer between redox enzymes and electrodes is a key step for enzymatic bioelectrocatalysis in various bioelectrochemical devices. Although the use of carbon nanomaterials enables an increasing number of redox enzymes to carry out bioelectrocatalysis involving direct electron transfer (DET), the role of carbon nanomaterials in interfacial electron transfer remains unclear. Based on the recent progress reported in the literature, in this mini review, the significance of carbon nanomaterials on DET-type bioelectrocatalysis is discussed. Strategies for the oriented immobilization of redox enzymes in rationally modified carbon nanomaterials are also summarized and discussed. Furthermore, techniques to probe redox enzymes in carbon nanomaterials are introduced. Full article
(This article belongs to the Special Issue Enzymatic Bioelectrocatalysis)
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29 pages, 2797 KiB  
Review
Membrane Protein Modified Electrodes in Bioelectrocatalysis
by Huijie Zhang, Rosa Catania and Lars J. C. Jeuken
Catalysts 2020, 10(12), 1427; https://doi.org/10.3390/catal10121427 - 06 Dec 2020
Cited by 7 | Viewed by 4497
Abstract
Transmembrane proteins involved in metabolic redox reactions and photosynthesis catalyse a plethora of key energy-conversion processes and are thus of great interest for bioelectrocatalysis-based applications. The development of membrane protein modified electrodes has made it possible to efficiently exchange electrons between proteins and [...] Read more.
Transmembrane proteins involved in metabolic redox reactions and photosynthesis catalyse a plethora of key energy-conversion processes and are thus of great interest for bioelectrocatalysis-based applications. The development of membrane protein modified electrodes has made it possible to efficiently exchange electrons between proteins and electrodes, allowing mechanistic studies and potentially applications in biofuels generation and energy conversion. Here, we summarise the most common electrode modification and their characterisation techniques for membrane proteins involved in biofuels conversion and semi-artificial photosynthesis. We discuss the challenges of applications of membrane protein modified electrodes for bioelectrocatalysis and comment on emerging methods and future directions, including recent advances in membrane protein reconstitution strategies and the development of microbial electrosynthesis and whole-cell semi-artificial photosynthesis. Full article
(This article belongs to the Special Issue Enzymatic Bioelectrocatalysis)
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Graphical abstract

20 pages, 3092 KiB  
Review
Recent Progress in Applications of Enzymatic Bioelectrocatalysis
by Taiki Adachi, Yuki Kitazumi, Osamu Shirai and Kenji Kano
Catalysts 2020, 10(12), 1413; https://doi.org/10.3390/catal10121413 - 03 Dec 2020
Cited by 13 | Viewed by 3142
Abstract
Bioelectrocatalysis has become one of the most important research fields in electrochemistry and provided a firm base for the application of important technology in various bioelectrochemical devices, such as biosensors, biofuel cells, and biosupercapacitors. The understanding and technology of bioelectrocatalysis have greatly improved [...] Read more.
Bioelectrocatalysis has become one of the most important research fields in electrochemistry and provided a firm base for the application of important technology in various bioelectrochemical devices, such as biosensors, biofuel cells, and biosupercapacitors. The understanding and technology of bioelectrocatalysis have greatly improved with the introduction of nanostructured electrode materials and protein-engineering methods over the last few decades. Recently, the electroenzymatic production of renewable energy resources and useful organic compounds (bioelectrosynthesis) has attracted worldwide attention. In this review, we summarize recent progress in the applications of enzymatic bioelectrocatalysis. Full article
(This article belongs to the Special Issue Enzymatic Bioelectrocatalysis)
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25 pages, 5184 KiB  
Review
Enzymatic Bioreactors: An Electrochemical Perspective
by Simin Arshi, Mehran Nozari-Asbemarz and Edmond Magner
Catalysts 2020, 10(11), 1232; https://doi.org/10.3390/catal10111232 - 24 Oct 2020
Cited by 20 | Viewed by 6066
Abstract
Biocatalysts provide a number of advantages such as high selectivity, the ability to operate under mild reaction conditions and availability from renewable resources that are of interest in the development of bioreactors for applications in the pharmaceutical and other sectors. The use of [...] Read more.
Biocatalysts provide a number of advantages such as high selectivity, the ability to operate under mild reaction conditions and availability from renewable resources that are of interest in the development of bioreactors for applications in the pharmaceutical and other sectors. The use of oxidoreductases in biocatalytic reactors is primarily focused on the use of NAD(P)-dependent enzymes, with the recycling of the cofactor occurring via an additional enzymatic system. The use of electrochemically based systems has been limited. This review focuses on the development of electrochemically based biocatalytic reactors. The mechanisms of mediated and direct electron transfer together with methods of immobilising enzymes are briefly reviewed. The use of electrochemically based batch and flow reactors is reviewed in detail with a focus on recent developments in the use of high surface area electrodes, enzyme engineering and enzyme cascades. A future perspective on electrochemically based bioreactors is presented. Full article
(This article belongs to the Special Issue Enzymatic Bioelectrocatalysis)
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