Direct ink writing of aqueous electrochemical energy storage devices
File(s)
Author(s)
Tagliaferri, Stefano
Type
Thesis
Abstract
Electrochemical energy storage devices (EESDs) will play a key role in the future development of portable and wearable electronics. The current manufacturing methods for EESDs rely on toxic and flammable solvents, raising concerns about user safety and environmental sustainability. Energy storage devices containing aqueous electrolytes are intrinsically safer; however, their low energy density and cycle life hinder commercialization.
Direct Ink Writing (DIW) is a 3D printing technique emerging as a promising manufacturing method for customizable EESDs with tailored size and enhanced performance. Inks for DIW can be formulated using water and environmentally sustainable solvents. Additionally, 3D printed EESDs present superior surface-to-volume ratios and high loading of active material, overcoming the energy density limitations of aqueous EESDs and the low rate capability of thick electrodes.
DIW has the capability to print a broad range of materials, enabling the fabrication of electrodes, electrolyte and passive components in the same manufacturing process. Nonetheless, the composition of the inks for DIW must be carefully designed to achieve structures with the desired geometry and functional properties. Therefore, in this work we investigated new ink formulations for the manufacturing of aqueous EESDs using DIW, with specific focus on aqueous graphene supercapacitors, zinc hybrid capacitors and zinc ion batteries. The printability of the inks was optimized to fabricate electrochemically-active structures with the desired degree of geometric complexity. We demonstrated that 3D printed graphene and zinc electrodes achieve superior energy density, rate capability and stability in aqueous supercapacitors and zinc hybrid capacitors. Additionally, we shed light into the charge storage and ageing mechanisms of 3D printed electrodes for aqueous supercapacitors and zinc ion batteries, using a combination of physical and electrochemical characterization tools. Finally, we successfully demonstrated an all-printed zinc-ion battery, combining interdigitated zinc anodes and manganese oxide cathodes with printable gel electrolytes.
Direct Ink Writing (DIW) is a 3D printing technique emerging as a promising manufacturing method for customizable EESDs with tailored size and enhanced performance. Inks for DIW can be formulated using water and environmentally sustainable solvents. Additionally, 3D printed EESDs present superior surface-to-volume ratios and high loading of active material, overcoming the energy density limitations of aqueous EESDs and the low rate capability of thick electrodes.
DIW has the capability to print a broad range of materials, enabling the fabrication of electrodes, electrolyte and passive components in the same manufacturing process. Nonetheless, the composition of the inks for DIW must be carefully designed to achieve structures with the desired geometry and functional properties. Therefore, in this work we investigated new ink formulations for the manufacturing of aqueous EESDs using DIW, with specific focus on aqueous graphene supercapacitors, zinc hybrid capacitors and zinc ion batteries. The printability of the inks was optimized to fabricate electrochemically-active structures with the desired degree of geometric complexity. We demonstrated that 3D printed graphene and zinc electrodes achieve superior energy density, rate capability and stability in aqueous supercapacitors and zinc hybrid capacitors. Additionally, we shed light into the charge storage and ageing mechanisms of 3D printed electrodes for aqueous supercapacitors and zinc ion batteries, using a combination of physical and electrochemical characterization tools. Finally, we successfully demonstrated an all-printed zinc-ion battery, combining interdigitated zinc anodes and manganese oxide cathodes with printable gel electrolytes.
Version
Open Access
Date Issued
2023-08-01
Date Awarded
2024-03-01
Copyright Statement
Creative Commons Attribution NonCommercial Licence
License URL
Advisor
Mattevi, Cecilia
Publisher Department
Materials
Publisher Institution
Imperial College London
Qualification Level
Doctoral
Qualification Name
Doctor of Philosophy (PhD)
Rights Embargo Date
2026-02-28