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1.
ACS Appl Mater Interfaces ; 15(23): 27809-27820, 2023 Jun 14.
Article in English | MEDLINE | ID: mdl-37256681

ABSTRACT

Lithium-ion battery (LIB) performance can be significantly affected by the nature of the complex electrode microstructure. The carbon binder domain (CBD) present in almost all LIB electrodes is used to enhance mechanical stability and facilitate electronic conduction, and understanding the CBD phase microstructure and how it affects the complex coupled transport processes is crucial to LIB performance optimization. In this work, the influence of microporosity in the CBD phase has been studied in detail for the first time, enabling insight into the relationships between the CBD microstructure and the battery performance. To investigate the effect of the CBD pore size distributions, a random field method is used to generate in silico a multiple-phase electrode structure, including bimodal pore size distributions seen in practice and microporous CBD with a tunable pore size and variable transport properties. The distribution of macropores and the microporous CBD phase substantially affected simulated battery performance, where battery specific capacity improved as the microporosity of the CBD phase increased.

2.
ACS Nano ; 15(12): 18624-18632, 2021 Dec 28.
Article in English | MEDLINE | ID: mdl-34870983

ABSTRACT

Lithium-ion battery electrodes are on course to benefit from current research in structure re-engineering to allow for the implementation of thicker electrodes. Increasing the thickness of a battery electrode enables significant improvements in gravimetric energy density while simultaneously reducing manufacturing costs. Both metrics are critical if the transition to sustainable transport systems is to be fully realized commercially. However, significant barriers exist that prevent the use of such microstructures: performance issues, manufacturing challenges, and scalability all remain open areas of research. In this Perspective, we discuss the challenges in adapting current manufacturing processes for thick electrodes and the opportunities that pore engineering presents in order to design thicker and better electrodes while simultaneously considering long-term performance and scalability.

3.
Faraday Discuss ; 182: 97-111, 2015.
Article in English | MEDLINE | ID: mdl-26212555

ABSTRACT

Co-electrolysis of carbon dioxide and steam has been shown to be an efficient way to produce syngas, however further optimisation requires detailed understanding of the complex reactions, transport processes and degradation mechanisms occurring in the solid oxide cell (SOC) during operation. Whilst electrochemical measurements are currently conducted in situ, many analytical techniques can only be used ex situ and may even be destructive to the cell (e.g. SEM imaging of the microstructure). In order to fully understand and characterise co-electrolysis, in situ monitoring of the reactants, products and SOC is necessary. Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) is ideal for in situ monitoring of co-electrolysis as both gaseous and adsorbed CO and CO2 species can be detected, however it has previously not been used for this purpose. The challenges of designing an experimental rig which allows optical access alongside electrochemical measurements at high temperature and operates in a dual atmosphere are discussed. The rig developed has thus far been used for symmetric cell testing at temperatures from 450 °C to 600 °C. Under a CO atmosphere, significant changes in spectra were observed even over a simple Au|10Sc1CeSZ|Au SOC. The changes relate to a combination of CO oxidation, the water gas shift reaction, carbonate formation and decomposition processes, with the dominant process being both potential and temperature dependent.

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