Resumen de Biomass-derived carbon materials for energy storage applications
Energy storage systems are an essential link in the implementation of renewable energies and in the development of electric vehicles, which are needed to reduce our dependence on fossil fuels and the emission of greenhouse gases. Various technologies have been proposed for energy storage based on different working principles, including lithium-ion batteries, emerging sodium-ion batteries and electric-double layer capacitors. Besides the quest for improving key aspects such as energy and power densities, current research efforts are devoted to foster the manufacturing of more environmentally friendly devices using sustainable materials. Carbon-based electrodes hold considerable promise in such terms due to their low cost, tailorable morphology and microstructure, and the possibility of processing them by direct carbonization of eco-friendly and naturally-available biomass resources. The main goal of this thesis is to develop carbon materials from biomass resources and study their applications as electrode for lithium-ion batteries, sodium-ion batteries and electric-double layer capacitors. En route towards that goal, it also aims at expanding our understanding of the microstructural changes of biomass-derived carbons with varying processing conditions and their effect on the electrochemical performance for each of these technologies. The first part of this work reports on the synthesis of graphitized carbon materials from biomass resources by means of an Fe catalyst, and the study of their electrochemical performance as anode materials for lithium-ion batteries (LIBs). Peak carbonization temperatures between 850 °C and 2000 ºC were covered to study the effect of crystallinity, surface and microstructural parameters on the anodic behavior, focusing on the first-cycle Coulombic efficiency, reversible specific capacity and rate performance. Reversible capacities of Fe-catalyzed biomass-derived carbons were compared to non-catalyzed hard carbon and soft carbons materials heated up to 2800 ºC. Moreover, in-situ characterization experiments were carried out to advance our understanding of the mechanisms responsible for catalytic graphitization. The second part of this work reports a comprehensive study on the structural evolution of hard carbons from biomass resources as a function of carbonization temperature (800 - 2000 ºC), and its correlation with electrochemical properties as anode materials for sodium-ion batteries (SIBs). Synchrotron X-ray total scattering experiments were performed and the associated atomic pair distribution function (PDF) extracted from the data to access quantitative information on local atomic arrangement in these amorphous materials at the nanoscale, as well as its evolution with increasing processing temperature. Then, electrochemical properties and the storage mechanisms involved on Na ions insertion into hard carbon structures at each characteristic potential regions were elucidated and correlated with microstructural properties. Finally, the third part of this work reports on the synthesis of nanostructured porous graphene-like materials from biomass resources using an explosion-assisted activation strategy by nitrate compounds and Ni as a graphitization catalyst. The thermal behavior during carbonization as well as the resulting microstructural and surface properties were evaluated at two different processing temperatures, 300 and 1000 ºC. Finally, their application as electrode materials for electric-double layer capacitors (EDLCs) and LIBs is investigated, with a view to their performance under high charge/discharge specific current densities experiments.
