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Status Update on Bioelectrochemical Systems: Prospects for Carbon Electrode Design and Scale-Up

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Status Update on Bioelectrochemical Systems: Prospects for Carbon Electrode Design and Scale-Up catalysts Review Status Update on Bioelectrochemical Systems: Prospects for Carbon Electrode Design and Scale-Up Katharina Herkendell Department of Chemical and Biological Engineering, Friedrich-Alexander-Universität Erlangen-Nürnberg, Fürther Straße 244f, D-90429 Nürnberg, Germany; [email protected] Abstract: Bioelectrochemical systems (BES) employ enzymes, subcellular structures or whole elec- troactive microorganisms as biocatalysts for energy conversion purposes, such as the electrosynthesis of value-added chemicals and power generation in biofuel cells. From a bioelectrode engineering viewpoint, customizable nanostructured carbonaceous matrices have recently received considerable scientific attention as promising electrode supports due to their unique properties attractive to bio- electronics devices. This review demonstrates the latest advances in the application of nano- and micro-structured carbon electrode assemblies in BES. Specifically, in view of the gradual increase in the commercial applicability of these systems, we aim to address the stability and scalability of different BES designs and to highlight their potential roles in a circular bioeconomy. Keywords: mesoporous carbon; nanostructures; biofuel cells; bioelectrocatalysis; enzyme; bioenergy; bioelectrode; electrosynthesis; microorganisms; waste valorization; bioeconomy 1. Current Developments Citation: Herkendell, K. Status Bioelectrochemical systems (BES) are made of biocatalytic assemblies capable of con- Update on Bioelectrochemical Systems: Prospects for Carbon verting electrical into chemical energy or vice-versa. The advantages of biocatalysts in Electrode Design and Scale-Up. electrochemical conversion are numerous and include the possibility to work under mild Catalysts 2021, 11, 278. https:// operating conditions with high substrate selectivity accompanied with resilience to the doi.org/10.3390/catal11020278 presence of impurities, and the ability to seamlessly integrate decentralized energy con- version concepts [1–9]. The substitution or complementation of chemically catalyzed Academic Editor: Barbara Mecheri processes with biocatalysis are envisaged to make a multidimensional impact in the bioe- conomy [10–13], where the latter has been defined by the European Commission as “the Received: 31 January 2021 production of renewable biological resources and the conversion of these resources and Accepted: 15 February 2021 waste streams into value added products, such as food, feed, bio-based products and bioen- Published: 19 February 2021 ergy” [14]. From a general standpoint, BES may play a major role in a circular bioeconomy: (i) as biodegradable tools, (ii) consequential to their assembly from renewable or recycled Publisher’s Note: MDPI stays neutral resources, and (iii) by their conjugation to energy reco99very processes. with regard to jurisdictional claims in In regard to the first contribution (i), single-use and short-lifetime BES devices demon- published maps and institutional affil- strate clear opportunities in plastic/electronic waste reduction, which may be applied to iations. biodegradable medical implants, environmental sensors, and wearable devices [15]. These include, for example, cellulose-fiber-based sensors and fuel cell components [16,17], or degradable fuel cell stacks [18]. In terms of the second role suggested for the BES (ii), intensive efforts are currently Copyright: © 2021 by the author. invested in developing practical approaches reducing the environmental impact of BES Licensee MDPI, Basel, Switzerland. components by using renewable or recycled materials and energy resources. For ex- This article is an open access article ample, Hernandez-Flores et al. introduced an agar-containing membrane for microbial distributed under the terms and electrosynthesis cells, which was discovered to be a low-cost and sustainable replacement conditions of the Creative Commons for conventional membranes, and also resulted in a safer pretreatment procedure [14]. Attribution (CC BY) license (https:// In another interesting recycling approach reported, high-performance microbial fuel cell creativecommons.org/licenses/by/ electrodes were produced from waste tires [19]. 4.0/). Catalysts 2021, 11, 278. https://doi.org/10.3390/catal11020278 https://www.mdpi.com/journal/catalysts Catalysts 2021, 11, 278 2 of 18 conventional membranes, and also resulted in a safer pretreatment procedure [14]. In an- Catalysts 2021, 11, 278 2 of 17 other interesting recycling approach reported, high-performance microbial fuel cell elec- trodes were produced from waste tires [19]. With this in mind, it is expected that the biggest contribution of the BES to circular processesWith lies this in in the mind, energy it is recovery expected area that (iii) the [15,20,21] biggest contribution. As sketched of in the Figure BES to1, circularthe two processesmajor contributing lies in the systems energy recognized recovery area in the (iii) field [15 ,of20 BES,,21]. are: As sketched(A) biofuel in cells, Figure enabling1, the twosustainable major contributing power generation systems from recognized organic waste, in the fieldsewage of BES,sludge, are: or (A) lignocellulosic biofuel cells, bio- en- ablingmass [14,21,22] sustainable, and power (B) bioelectrosynthesis generation from organic cells utilizing waste, sewage electrical sludge, energy or lignocellulosicto biocatalyze biomasschemical [ 14transformations.,21,22], and (B) bioelectrosynthesisBioelectrosynthesis cells can utilizingbe optimal electrically achieved energy by to using biocatalyze a feed chemicalof surplus transformations. renewable energy Bioelectrosynthesis for the on-site production can be optimally of value achieved-added chemicals by using a (VAC feed ofs) surplussuch as renewablehydrogen, energymethane, for methanol, the on-site formate, production or ofbicarbonate value-added [23 chemicals–26]. For both (VACs) the such bio- asfuel hydrogen, and the electrosynthesis methane, methanol, cell formate,cases, a orscalable bicarbonate bioelectrocatalytic [23–26]. For bothproduction the biofuel that and re- thequires electrosynthesis high stability celland cases, efficiency a scalable of the bioelectrocatalytic microscopic electrode production processes that is requiresessential. high stability and efficiency of the microscopic electrode processes is essential. Figure 1. Illustration of the two main bioelectrochemical systems used for the production of power and value value-added-added chemicals chemicals and and their their basic basic operation operation principles: principles: (A ()A In) Inthe the biofuel biofuel cell cell assembly assembly the biocatalyzed oxidation oxidation of of substrates substrates on on the the anode anode occurring occurring simultaneously simultaneously with with the the cathodic cathodic reduction ofof anan oxidizeroxidizer accountsaccounts forfor thethe generationgeneration ofof anan electricelectric power;power; ( B(B)) the the bioelectrosynthesis bioelectrosynthe- cellsis cell converts converts the the power power it is it fed is fed from from renewable renewable sources sources to value-addedto value-added chemicals chemicals via via biocatalyzed biocata- cathodiclyzed cathodic transformations. transformations. In the process process of of designing designing a aBES, BES, one one may may select select a biocatalyst a biocatalyst from from a constantly a constantly ex- expandingpanding pool pool of of options options [27] [27. ].Depending Depending on on the the targeted targeted substrate, substrate, product, product, and process specifications,specifications, broad broad possibilities possibilities to to select select from from exist, exist, and and these these include include,, for example: for example: pu- purifiedrified redox redox enzymes enzymes such such as as oxidoreductases, oxidoreductases, unpurified unpurified “crude” “crude” extracts extracts of microbial cells, organelles suchsuch as chloroplasts or mitochondria, oror wholewhole cellscells suchsuch asas electroactiveelectroactive bacteria, archaea or or eukaryotes eukaryotes in in mono mono-- or or co co-cultures,-cultures, given given they they can can be be immobilized immobilized in ina way a way that that allows allows them them to to effectively effectively exchange exchange electrons electrons with with an an electrode electrode surface in aa receivingreceiving (cathodic) or ejectingejecting (anodic)(anodic) mannermanner [[1,27,28]1,27,28].. TheseThese areare typicallytypically integratedintegrated into assemblies representing thethe fourfour mainmain BESBES categories,categories, whichwhich consistconsist ofof enzymatic fuel cells, microbial fuel cells, enzymatic electrosynthesis cells, and microbial electrosynthesiselectrosynthesis cells.cells. While microbialmicrobial systemssystems are are generally generally considered considered more more stable stable and and reliable reliable in in terms terms of energyof energy or VACor VAC recovery recovery from from organic organic wastes wastes and and wastewater wastewater streams, streams, enzymatic enzymatic systems sys- benefittems benefit from from high efficiencieshigh efficiencies due to due the to lack the oflack membranes of membranes and metabolicand metabolic processes processes that increasethat increase the inherentthe inherent overpotentials overpotentials and and limited limited efficiencies efficiencies associated associated with with whole-cell whole- microbial systems [29–31]. Outside of these main categories, biomimetic systems are further
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