Microbial electrosynthesis (MES) has recently emerged as a novel biotechnology platform for value-added product generation from waste CO2 stream. Integrating MES technology with renewable energy sources for both CO2 valorization and renewable energy storage is regarded as one type of artificial photosynthesis and a perfect example of circular bioeconomy. However, several challenges remain to be addressed to scale-up MES as a feasible process for chemical production, which include enhanced production rate, reduced energy consumption and excellent resistance to external fluctuations. To fill these knowledge gaps, different in-depth approaches were proposed in this dissertation by optimizing the cathode architecture, CO2 flow rates and utilizing efficient photoelectrode to improve MES performance and stability. A novel cathode design, made of conductive hollow fiber membrane, was developed in this dissertation to improve CO2 availability at MES cathode surface via direct CO2 delivery to chemolithoautotrophs through the pores in the hollow fibers. By modifying the hollow fiber surface with carbon nanotubes (CNTs), higher bioproduct formation was achieved with excellent faradaic efficiencies, which could be attributed to the improved surface area for bacterial adhesion and the reduction of cathodic electron transfer resistance. Since CO2 flow rate from industrial facilities typically varies over time, this hollow-fiber architecture was also applied to test the resistance of MES systems to CO2 flow rate fluctuation. Stepwise increase of CO2 flow rates from 0.3 ml/min to 10 ml/min was tested and the effect of CO2 flow rate fluctuations was evaluated in terms of biochemical generation and microbial community. MES was further integrated with renewable energy supply for both energy storage and CO2 transformation into biofuels and biochemicals. Stable MES photoanode, based on molybdenum-doped bismuth vanadate deposited on fluorine-doped tin oxide glass (FTO/BiVO4/Mo), was prepared for efficient solar energy harvesting and overpotential reduction for oxygen evolution reaction (OER), which contributed to one of the highest solar-to-biochemical conversion efficiencies ever reported for photo-assisted MES systems. The applied nature of this dissertation with fundamental insights is of great importance to bring MES one step closer to full-scale applications and enable MES technology to be economically more viable for renewable energy storage and CO2 valorization.

Biomass is a valuable and limited resource that should be used efficiently. The potential of replacing fossil-based products with bio-based ones produced in biobased industrial systems is huge. One important aim of increasing the share of biobased products is to improve the sustainability of systems for production and consumption. Therefore, it is important to evaluate what solutions are available to improve the sustainability performance of bio-based industrial systems, and if they also bring negative impacts. The thesis focuses on assessing the role of biogas solutions in developing sustainable bio-based systems. Such assessments are often quite narrow in their scope and focus on quantitative environmental or economic aspects. This thesis aims at also including feasibility related aspects involving the contextual conditions that are assessed more qualitatively. Biogas solutions are identified as a versatile approach to treat organic materials which are generated in large volumes in bio-based industrial systems. The results show that biogas solutions in bio-based industrial systems (i) improve circular flows of energy and nutrients, (ii) are especially viable alternatives when the quality of the by-product streams become poorer, and (iii) may improve the profitability of the bio-based industrial system. To perform better assessments of these systems, it seems valuable to broaden the set of indicators assessed and include feasibility-related indicators, preferably through the involvement of relevant stakeholders as they contribute with different perspectives and can identify aspects that influence the sustainability in different areas. Future studies could benefit from applying those broader assessments on more cases to build on a more generalisable knowledge base.

Tesis por compendio / [ES] El envasado activo es una de las tecnologías emergentes más relevantes de la industria alimentaria. Su objetivo es interactuar con el espacio de cabeza del envase para controlar las reacciones enzimáticas, químicas, físicas y microbiológicas que deterioran los alimentos por medio de la absorción o liberación. La actual tesis doctoral trata originalmente del desarrollo y la caracterización de estructuras de envasado de alimentos activas y biodegradables mono y multicapa basadas en materiales de polihidroxialcanoatos (PHA) electroestirados derivados de estrategias de bioeconomía circular. Con el fin de dotar con propiedades activas los materiales de envasado, se incorporaron a los PHA aceites esenciales, extractos naturales, nanopartículas metálicas o combinaciones de los mismos mediante electrospinning de soluciones. Las fibras resultantes de PHA por electrospinning se recocieron para obtener monocapas continuas que, posteriormente, se combinaron con películas de polímeros biodegradables fundidas, sopladas o fundidas con disolventes y/o con revestimientos de barrera de nanocristales de celulosa bacteriana (CNC) para desarrollar novedosos sistemas multicapa con propiedades antimicrobianas y de barrera. Estos sistemas multicapas basados en PHA presentaron un buen rendimiento térmico y mecánico, así como altas propiedades de barrera a los vapores y gases. Las películas activas también mostraron mejores propiedades antioxidantes y una alta actividad antimicrobiana contra las bacterias transmitidas por los alimentos tanto en sistemas abiertos como, lo que es más importante, en sistemas cerrados, que pueden imitar las condiciones de envasado en casos reales. Por lo tanto, los materiales y prototipos desarrollados en este trabajo pueden ser muy prometedores como materiales de envasado, para constituir bandejas, flow packs y tapas, siendo completamente renovables y también biodegradables, con una potencial capacidad de aumentar tanto la calidad, como la seguridad de los productos alimenticios en el nuevo contexto de la Bioeconomía Circular. / [CA] L'envasament actiu és una de les tecnologies emergents més rellevants de la indústria alimentària. El seu objectiu és interactuar amb l'espai de cap de l'envàs per controlar les reaccions enzimàtiques, químiques, físiques i microbiològiques que deterioren els aliments per mitjà de l'absorció o alliberament. L'actual tesi doctoral tracta originalment de el desenvolupament i la caracterització d'estructures d'envasat d'aliments actives i biodegradables mono i multicapa basades en materials de polihidroxialcanoatos (PHA) electroestirados derivats d'estratègies de bioeconomia circular. Per tal de dotar amb propietats actives dels materials d'envasat, es van incorporar als PHA olis essencials, extractes naturals, nanopartícules metàl·liques o combinacions dels mateixos mitjançant electrospinning de solucions. Les fibres resultants de PHA per electrospinning es recocieron per obtenir monocapes contínues que, posteriorment, es van combinar amb pel·lícules de polímers biodegradables foses, bufades o foses amb dissolvents i / o amb revestiments de barrera de nanocristalls de cel·lulosa bacteriana (CNC) per desenvolupar nous sistemes multicapa amb propietats antimicrobianes i de barrera. Aquests sistemes multicapes basats en PHA van presentar un bon rendiment tèrmic i mecànic, així com altes propietats de barrera als vapors i gasos. Les pel·lícules actives també van mostrar millors propietats antioxidants i una alta activitat antimicrobiana contra bacteris transmeses pels aliments tant en sistemes oberts com, el que és més important, en sistemes tancats, que poden imitar les condicions d'envasament en casos reals. Per tant, els materials i prototips desenvolupats poden ser molt prometedors com materials d'envasat, per constituir safates, flow packs i tapes, sent completament renovables i també biodegradables, amb la capacitat potencial final d'augmentar tant la qualitat, com la seguretat de els productes alimentaris en el nou context de l'Bioeconomia Circular. / [EN] Active packaging is one of the most relevant emerging technologies in the food industry. It aims to interact with the packaging headspace to control the enzymatic, chemical, physical, and microbiological reactions that deteriorate food through scavenging or releasing means. The current PhD thesis originally deals with the development and characterization of mono and multilayer active and biodegradable food packaging structures based on electrospun polyhydroxyalkanoates (PHA) materials derived from circular bioeconomy strategies. In order to provide the packaging materials with active properties, essential oils, natural extracts, metallic nanoparticles or combinations thereof were incorporated into PHA by solution electrospinning. The resultant electrospun PHA mats were annealed to obtain continuous monolayers that were, thereafter, combined with cast-extruded, blown or solvent-casted biodegradable polymer films and/or barrier coatings of bacterial cellulose nanocrystals (CNCs) to develop novel multilayer systems with antimicrobial and barrier properties. These PHA-based multilayers systems presented good thermal and mechanical performance as well as high barrier properties to vapors and gases. The active films also showed improved antioxidant properties and high antimicrobial activity against food-borne bacteria in both open and, more importantly, closed systems, which can mimic real case use packaging conditions. Therefore, the here-developed materials and prototypes can be very promising as packaging materials, to constitute trays, flow packs and lids, being completely renewable and also biodegradable, with the final potential capacity to increase both quality and safety of food products in the new Circular Bioeconomy context. / Al programa Santiago Grisolía de la Generalitat Valenciana (0001426013N810001A201) por concederme la beca Predoctoral. Al proyecto EU H2020 YPACK “High Performance Polyhydroxyalkanoates Based Packaging to Minimise Food Waste” (Grant agreement 773872) de la Comisión Europea. Al proyecto RTI2018-097249-B-C21 financiado por el Ministerio de Ciencia e Innovación de España. A la Unidad Asociada IATA-UJI en “Polymer Technology”. / Figueroa López, KJ. (2021). Biodegradable Mono and Multilayer Materials with Antimicrobial Capacity Based on Circular Bioeconomy of Application Interest in Food Packaging [Tesis doctoral]. Universitat Politècnica de València. https://doi.org/10.4995/Thesis/10251/168439 / TESIS / Compendio

Durch die Nutzung des fischfutterbedingten Nährstoffeintrags für die kombinierte Produktion von Fischen und Pflanzen können Aquaponiksysteme eine nachhaltige Erweiterung von Kreislaufanlagen der Aquakultur (RAS) darstellen. Herkömmliche Aquakulturfutter zielen jedoch auf Fischproduktion mit geringer Umweltbelastung ab und sind somit nicht für die Aquaponik optimiert. Daher weist RAS-Wasser häufig Mängel im Profil gelöster anorganischer Pflanzennährstoffe auf. So war es Ziel dieser Arbeit, die Auswirkungen unterschiedlicher Proteinquellen auf die Nährstoffdynamik in RAS durch Fütterungsversuche mit Afrikanischem Raubwels und Nil-Tilapia zu untersuchen, bei denen Wachstum, gelöste anorganische Nährstoffkonzentrationen im RAS-Wasser und die Ausscheidung von Nährstoffen über den Kot verfolgt wurden. Der Fokus lag auf nachhaltigen alternativen Proteinquellen zu marinem Fischmehl und terrestrischen Pflanzenproteinen: Larvenmehl der Schwarzen Soldatenfliege (BSFM), Welsschlachtabfallmehl (CM), Geflügelschlachtabfallmehl (PM) und Geflügelblutmehl (PBM). Experimentalfutter, die phosphorreiches PM und CM enthielten, förderten erhöhte Ausscheidung von löslichem reaktivem Phosphor, erzeugten die besten gelösten N:P-Verhältnisse im RAS-Wasser verglichen mit einer Hydroponik-Nährlösung und ermöglichten in Kombination mit PBM besseres Wachstum beim Wels als ein vergleichbares kommerzielles Futter. In Futtern basierend auf einer einzigen Proteinquelle führte PM bei Wels und insbesondere bei Tilapia zu ähnlichem Wachstum verglichen mit marinem Fischmehl, wohingegen BSFM und PBM bei beiden Arten Wachstumsleistung beeinträchtigte. Meta-Analysen aller Versuche legen nahe, dass höherer Phosphor-, Kalium- und Magnesiumgehalt im Futter erhöhte Ausscheidung dieser Elemente in gelöster Form bedingt, was sie zu Zielnährstoffen in Aquaponikfuttern macht, während die Optimierung des Protein zu Energie-Verhältnisses im Futter die gelösten N:P- und N:K-Verhältnisse im RAS-Wasser verbessern kann. / By using the nutrient input from fish feeds for the combined production of fish and plants, aquaponic systems can be a sustainable extension of recirculating aquaculture systems (RAS). However, conventional aquaculture feeds are optimized for fish production and reduced environmental impact rather than aquaponics. Hence, RAS water is often characterized by deficiencies regarding its dissolved inorganic plant nutrient profile. Therefore, this thesis aimed to explore the effect of purposeful dietary protein choice on nutrient dynamics in RAS through four systematic feeding trials involving African catfish and Nile tilapia in which growth performance, dissolved inorganic nutrient concentrations in RAS water and solid fecal nutrient excretion were tracked. Focus was on sustainable alternative protein sources to marine fish meal and terrestrial plant proteins: black soldier fly larvae meal (BSFM), catfish by-product meal (CM), poultry by-product meal (PM) and poultry blood meal (PBM). Experimental diets including phosphorus-rich PM and CM supported increased excretion of soluble reactive phosphorus, produced the most favorable dissolved N:P ratios in RAS water when compared to a renowned hydroponic nutrient solution, and, combined with PBM, enabled better growth performance in African catfish than a comparable commercial diet. In single protein source diets, PM produced similar growth performance in African catfish and particularly Nile tilapia versus marine fish meal, whereas BSFM and PBM impaired growth performance in both species. Meta-analyses covering all trials suggest that higher dietary phosphorus, potassium and magnesium content leads to their increased excretion in dissolved form, making them target nutrients for aquaponic feed formulation, while the optimization of the dietary protein to energy ratio can further improve dissolved N:P and N:K ratios in RAS water.