Author ORCID Identifier

https://orcid.org/0000-0002-3841-5573

Date of Award

Spring 2024

Document Type

Thesis (Ph.D.)

Department or Program

Engineering Sciences

First Advisor

William J. Scheideler

Second Advisor

Jifeng Liu

Third Advisor

Weiyang Li

Abstract

Emerging energy technologies have the potential to fill gaps in performance and reliability but currently lack the capabilities to do this at a commercial scale. 3D printing has the ability to fabricate engineered lattice structures with broadly tunable surface area and optimal geometries for maximizing electrochemical performance, and perovskite solar cells (PSCs) have the potential to deliver terawatt-scale power via low-cost manufacturing. However, neither of these technologies has yet to achieve fully scalable manufacture. 3D printed energy storage devices lack an understanding of how 3D lattice type influences the specific capacity when employed in supercapacitors, and PSC fabrication is limited by the lack of rapid, reliable, large-area deposition methods with additive patterning capabilities.

Here we present methods for scaling fabrication of critical perovskite solar cell materials as well as 3D lattice structures for energy storage applications. We characterize the electrical conductivity of 3D lattices of varying size, structure, and porosity to guide additively manufactured electrode design in energy storage devices, optimizing the design for specific applications. We also use high-speed (60 m/min) flexographic printing to deposit both ultrathin NiOx hole transport layers (HTLs) and MA0.6FA0.4PbI3 perovskite absorbers. By engineering precursor rheology for rapid film leveling, we print both materials with high uniformity and ultralow pinhole densities using the fastest reported processes for both NiOx and perovskite deposition. Flexographic printing of these materials delivers high-resolution patterning (< 3 μm line edge roughness) and precise thickness control, allowing scalably printed 50 μm features over large areas (140 cm2), while obviating damaging scribing steps. Integrating these highly uniform printed NiOx HTLs and perovskite absorbers into planar PSCs, we improve photovoltaic conversion efficiency, reaching the highest performance yet reported for any roll-printed perovskite cells (20.4%). This study therefore establishes 3D printing and flexography as scalable approaches to manufacture precisely designed lattice structures for supercapacitor applications and pattern high-quality perovskite solar cell materials, enhancing performance of both energy storage and energy harvesting devices via scalable manufacturing.

Available for download on Tuesday, April 29, 2025

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