TY - GEN A1 - Bobadilla, Luis F. A1 - Azancot, Lola A1 - Luque-Alvarez, Ligia A. A1 - Torres-Sempere, Guillermo A1 - Gonzalez-Castano, Miriam A1 - Pastor-Perez, Laura A1 - Yu, Jie A1 - Ramirez Reina, Tomas A1 - Ivanova, Svetlana A1 - Centeno, Miguel Angel A1 - Odriozola, José Antonio T1 - Development of Power-to-X Catalytic Processes for CO2 Valorisation: From the Molecular Level to the Reactor Architecture T2 - Chemistry N2 - Nowadays, global climate change is likely the most compelling problem mankind is facing. In this scenario, decarbonisation of the chemical industry is one of the global challenges that the scientific community needs to address in the immediate future. Catalysis and catalytic processes are called to play a decisive role in the transition to a more sustainable and low-carbon future. This critical review analyses the unique advantages of structured reactors (isothermicity, a wide range of residence times availability, complex geometries) with the multifunctional design of efficient catalysts to synthesise chemicals using CO2 and renewable H2 in a Power-to-X (PTX) strategy. Fine-chemistry synthetic methods and advanced in situ/operando techniques are essential to elucidate the changes of the catalysts during the studied reaction, thus gathering fundamental information about the active species and reaction mechanisms. Such information becomes crucial to refine the catalyst’s formulation and boost the reaction’s performance. On the other hand, reactors architecture allows flow pattern and temperature control, the management of strong thermal effects and the incorporation of specifically designed materials as catalytically active phases are expected to significantly contribute to the advance in the valorisation of CO2 in the form of high added-value products. From a general perspective, this paper aims to update the state of the art in Carbon Capture and Utilisation (CCU) and PTX concepts with emphasis on processes involving the transformation of CO2 into targeted fuels and platform chemicals, combining innovation from the point of view of both structured reactor design and multifunctional catalysts development. Y1 - 2022 UR - https://www.mdpi.com/2624-8549/4/4/83 U6 - https://doi.org/10.3390/chemistry4040083 SN - 2624-8549 VL - 4 IS - 4 SP - 1250 EP - 1280 ER - TY - GEN A1 - Ketabchi, Elham A1 - Pastor-Perez, Laura A1 - Arellano-García, Harvey A1 - Ramirez Reina, Tomas T1 - Influence of Reaction Parameters on the Catalytic Upgrading of an Acetone, Butanol and Ethanol (ABE) Mixture: Exploring New Routes for Modern Biorefineries T2 - Frontiers in Chemistry N2 - Here we present a comprehensive study on the effect of reaction parameters on the upgrade of an acetone, butanol and ethanol mixture – key molecules and platform products of great interest within the chemical sector. Using a selected high performing catalyst, Fe/MgO-Al2O3, the variation of temperature, reaction time, catalytic loading and reactant molar ratio have been examined in this reaction. This work is aiming to not only optimise the reaction conditions previously used, but to step towards using less energy, time and material by testing those conditions and analysing the sufficiency of the results. Herein we demonstrate that this reaction is favoured at higher temperatures and longer reaction time. Also, we observe that increasing the catalyst loading had a positive effect on the product yields, while reactant ratios have shown to produce varied results due to the role of each reactant in the complex reaction network. In line with the aim of reducing energy and costs, this work showcases that the products from the upgrading route have significantly higher market value than the reactants; highlighting that this process represents an appealing route to be implemented in modern biorefineries. Y1 - 2020 UR - https://www.frontiersin.org/articles/10.3389/fchem.2019.00906/full U6 - https://doi.org/10.3389/fchem.2019.00906 SN - 2296-2646 VL - 7 ER - TY - GEN A1 - Ketabchi, Elham A1 - Pastor-Perez, Laura A1 - Ramirez Reina, Tomas A1 - Arellano-García, Harvey T1 - Catalytic upgrading of acetone, butanol and ethanol (ABE): A step ahead for the production of added value chemicals in bio-refineries T2 - Renewable Energy N2 - With the aim of moving towards sustainability and renewable energy sources, we have studied the production of long chain hydrocarbons from a renewable source of biomass to reduce negative impacts of greenhouse gas emissions while providing a suitable alternative for fossil fuel-based processes. Herein we report a catalytic strategy for Acetone, Butanol and Ethanol (ABE) upgrading using economically viable catalysts with potential impact in modern bio-refineries. Our catalysts based on transition metals such as Ni, Fe and Cu supported on MgO–Al2O3 have been proven to perform exceptionally with outstanding conversions towards the production of a broad range of added value chemicals from C2 to C15. Although all catalysts displayed meritorious performance, the Fe catalyst has shown the best results in terms conversion (89%). Interestingly, the Cu catalyst displays the highest selectivity towards long chain hydrocarbons (14%). Very importantly, our approach suppresses the utilization of solvents and additives resulting directly in upgraded hydrocarbons that are of use in the chemical and/or the transportation industry. Overall, this seminal work opens the possibility to consider ABE upgrading as a viable route in bio-refineries to produce renewably sourced added value products in an economically favorable way. In addition, the described process can be envisaged as a cross-link stream among bio and traditional refineries aiming to reduce fossil fuel sources involved and incorporate “greener” solutions. Y1 - 2020 UR - https://www.sciencedirect.com/science/article/pii/S096014812030690X?via%3Dihub U6 - https://doi.org/10.1016/j.renene.2020.04.152 SN - 1879-0682 SN - 0960-1481 VL - 156 SP - 1065 EP - 1075 ER - TY - GEN A1 - Ramirez Reina, Tomas A1 - Ketabchi, Elham A1 - Arellano-García, Harvey A1 - Pastor-Perez, Laura T1 - The Production of Long Chain Hydrocarbons through the Catalytic Upgrade of Biomass-Based Acetone, Butanol and Ethanol (ABE) T2 - 2019 AIChE Annual Meeting N2 - One of the main issues that many industrial sectors such as oil refineries have been facing nowadays is their sole dependency on fossil fuel. Not only have price fluctuations affected the products, but their environmental impact is an ever present problem that should be addressed. This has led to the search for alternatives such as biomass based processes in order to reduce the dependency on fossil fuel. Bio-refinery processes, fed by biomass, produce high value chemicals and materials with the advantage of reduced environmental drawbacks, such as CO2 emissions, when compared to the conventional refinery. For the benefit of both systems, an integration approach has been considered connecting bio-refining and conventional refining processes together. In this work we focus on the production of long chain hydrocarbons while maintaining production of chemicals that already originate from biomass such as Acetone, Butanol and Ethanol (ABE). The ABE used for this process is obtained as a product of sugar fermentation using the bacteria genus Clostridium. Through the upgrading and conversion of ABE, the products obtained will then be incorporated in the proposed integration system, connecting the conventional oil refinery to this process. A reaction involving a complex reaction network towards upgrading ABE with the aim of producing valuable products using economically viable catalysts has been carried out. The vast majority of research in this area either involves the separation of ABE after fermentation to be used in the chemical/or transportation industry that incurs large costs, or noble metal catalysts are used to upgrade this feed, which would also not be economically viable. However, our research has surpassed the necessity of noble metals, leading to a significant cost decrease that also produces outstanding results. The catalysts required for this process were synthesised successfully through the wetness incipient method and characterised by XRD, Raman, BET, TPR and N2 Isotherm. The reaction consists of the self-condensation and cross condensation of the alcohols and acetone, respectively, using a variety of active metals on basic supports as catalysts, at high temperatures and pressure in a batch reactor. The results have shown exceptional performance for the catalysts in terms of conversion and selectivity, having conversions as high as 90%. The catalysts have proven to yield a range of C3-C15 hydrocarbons identified to be of need in the chemical industry. In conclusion, our route has produced valuable chemicals proven to have a considerably higher market value than the simple alcohol reactants, useful for both the petrochemical and the transportation industries, through the use of novel and economically favourable catalysts. Y1 - 2019 UR - https://www.aiche.org/conferences/aiche-annual-meeting/2019/proceeding/paper/39f-production-long-chain-hydrocarbons-through-catalytic-upgrade-biomass-based-acetone-butanol-and SN - 978-0-8169-1112-7 ER -