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Multi-phase management is crucial for performance and durability of electrochemical cells such as batteries and fuel cells. In this paper we present a generic framework for describing the two-dimensional spatiotemporal evolution of gaseous, liquid and solid phases, as well as their interdependence with interfacial (electro-)chemistry and microstructure in a continuum description. The modeling domain consists of up to seven layers (current collectors, channels, electrodes, separator/membrane), each of which can consist of an arbitrary number of bulk phases (gas, liquid, solid) and connecting interfaces (two-phase or multi-phase boundaries). Bulk and interfacial chemistry is described using global or elementary kinetic reactions. Multi-phase management is coupled to chemistry and to mass and charge transport within bulk phases. The functionality and flexibility of this framework is demonstrated using four application areas in the context of post-lithium-ion batteries and fuel cells, that is, lithium-sulfur (Li-S) cells, lithium-oxygen (Li-O) cells, solid oxide fuel cells (SOFC) and polymer electrolyte membrane fuel cells (PEFC). The results are compared to models available in literature and properties of the generic framework are discussed.
Battery degradation is a complex physicochemical process that strongly depends on operating conditions and environment. We present a model-based analysis of lithium-ion battery degradation in smart microgrids, in particular, a single-family house and an office tract with photovoltaics generator. We use a multi-scale multi-physics model of a graphite/lithium iron phosphate (LiFePO4, LFP) cell including SEI formation as ageing mechanism. The cell-level model is dynamically coupled to a system-level model consisting of photovoltaics, inverter, power consumption profiles, grid interaction, and energy management system, fed with historic weather data. The behavior of the cell in terms of degradation propensity, performance, state of charge and other internal states is predicted over an annual operation cycle. As result, we have identified a peak in degradation rate during the battery charging process, caused by charging overpotentials. Ageing strongly depends on the load situation, where the predicted annual capacity fade is 1.9 % for the single-family house and only 1.3 % for the office tract.
Proton Exchange Membrane Fuel Cells (PEMFC) are energy efficient and environmentally friendly alternatives to conventional energy conversion systems in many yet emerging applications. In order to enable prediction of their performance and durability, it is crucial to gain a deeper understanding of the relevant operation phenomena, e.g., electrochemistry, transport phenomena, thermodynamics as well as the mechanisms leading to the degradation of cell components. Achieving the goal of providing predictive tools to model PEMFC performance, durability and degradation is a challenging task requiring the development of detailed and realistic models reaching from the atomic/molecular scale over the meso scale of structures and materials up to components, stack and system level. In addition an appropriate way of coupling the different scales is required.
This review provides a comprehensive overview of the state of the art in modeling of PEMFC, covering all relevant scales from atomistic up to system level as well as the coupling between these scales. Furthermore, it focuses on the modeling of PEMFC degradation mechanisms and on the coupling between performance and degradation models.
We present a novel fabrication route yielding Raney-platinum film electrodes intended as glucose oxidation anodes for potentially implantable fuel cells. Fabrication roots on thermal alloying of an extractable metal with bulk platinum at 200 °C for 48 h. In contrast to earlier works using carcinogenic nickel, we employ zinc as potentially biocompatible alloying partner. Microstructure analysis indicates that after removal of extractable zinc the porous Raney-platinum film (roughness factor ∼2700) consists predominantly of the Pt3Zn phase. Release of zinc during electrode operation can be expected to have no significant effect on physiological normal levels in blood and serum, which promises good biocompatibility. In contrast to previous anodes based on hydrogel-bound catalyst particles the novel anodes exhibit excellent resistance against hydrolytic and oxidative attack. Furthermore, they exhibit significantly lower polarization with up to approximately 100 mV more negative electrode potentials in the current density range relevant for fuel cell operation. The anodes’ amenability to surface modification with protective polymers is demonstrated by the exemplary application of an approximately 300 nm thin Nafion coating. This had only a marginal effect on the anode long-term stability and amino acid tolerance. While in physiological glucose solution after approximately 100 h of operation gradually increasing performance degradation occurs, rapid electrode polarization within 24 h is observed in artificial tissue fluid. Optimization approaches may include catalyst enhancement by adatom surface modification and the application of specifically designed protective polymers with controlled charge and mesh size.
We report the fabrication and characterization of glucose-tolerant Raney-platinum cathodes for oxygen reduction in potentially implantable glucose fuel. Fabricated by extraction of aluminum from 1 μm thin platinum–aluminum bi-layers annealed at 300 °C, the novel cathodes show excellent resistance against hydrolytic and oxidative attack. This renders them superior over previous cathodes fabricated from hydrogel-bound catalyst particles. Annealing times of 60, 120, and 240 min result in approximately 400–550 nm thin porous films (roughness factors ∼100–150), which contain platinum and aluminum in a ratio of ∼9:1. Aluminum release during electrode operation can be expected to have no significant effect on physiological normal levels, which promises good biocompatibility. Annealing time has a distinct influence on the density of trenches formed in the cathode. Higher trench densities lead to lower electrode potentials in the presence of glucose. This suggests that glucose sensitivity is governed by mixed potential formation resulting from oxygen depletion within the trenches. During performance characterization the diffusion resistance to be expected from tissue capsule formation upon electrode implantation was taken into account by placing a membrane in front of the cathode. Despite the resulting limited oxygen supply, cathodes prepared by annealing for 60 min show more positive electrode potentials than previous cathodes fabricated from hydrogel-bound activated carbon. Compared to operation in phosphate buffered saline containing 3.0 mM glucose, a potential loss of approximately 120 mV occurs in artificial tissue fluid. This can be reduced to approximately 90 mV with a protective Nafion layer that is easily electro-coated onto the Raney-platinum film.
The formation of secondary phases in the porous electrodes is a severe mechanism affecting the lifetime of solid oxide fuel cells (SOFC). It can occur via various chemical mechanisms and it has a significant influence on cell performance due to pore clogging and deactivation of active surfaces and triple-phase boundary (TPB). We present a modeling and simulation study of nickel oxide formation (reoxidation) and carbon formation (coking) within the SOFC anode. We use a 2D continuum model based on a multi-phase framework [Neidhardt et al., J. Electrochem. Soc., 159, 9 (2012)] that allows the introduction of arbitrary solid phases (here: Ni, YSZ, NiO, Carbon) plus gas phase. Reactions between the bulk phases are modeled via interface-adsorbed species and are described by an elementary kinetic approach. Published experimental data are used for parameterization and validation. Simulations allow the prediction of cell performance under critical operation conditions, like (i) a non-fuel operation test, where NiO formation is taking place (Figure 1a), or (ii) an open circuit voltage (OCV) stability test under hydrocarbon atmosphere, where solid carbon is formed (Figure 1b). Results are applied for enhanced interpretation of experimental data and for prediction of safe operation conditions.