Liu, Yiyang; (2024) Industrialization of Aqueous Zinc-ion Batteries: Mechanism, Material, Device, Industrial Chain and Commercialization Perspectives. Doctoral thesis (Ph.D), UCL (University College London).

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Abstract

The escalating concern over climate change has necessitated an unprecedented global transition towards carbon peaking and neutrality, providing both challenges and opportunities. Renewable energy sources and energy storage technologies are crucial in this effort, but their development faces complex technical and economic barriers. Within this context, aqueous zinc-ion batteries (AZIBs) have emerged as a prominent solution. Characterized by low toxicity, abundant raw materials, and potentials for high energy and power densities, AZIBs are positioned to serve applications ranging from portable electronics to grid-scale energy storage. However, their commercialization is hampered by issues from the mechanism , material, device, manufacturing and commercialization perspectives. To foster the commercialization of AZIBs, a transformative technology, it is crucial to bridge four existing gaps: transitioning from scientific discovery to technology, from technology to product development, from product to market application, and finally, from market application to large-scale industrialization. • In the gap from science to technology, many of the mechanisms related to the key components of AZIBs remain unclear; hence, more efforts are crucial to further investigate the underlying mechanisms. Meanwhile, it is imperative to identify the most suitable niche applications for this technology through rigorous analysis from a first-principles perspective, which will offer a roadmap for future industrialization. • As for the transition from technology to product, most current research on AZIBs remains at the non-scalable coin cell stage. To mature the AZIB technology into a viable product, it is essential to forge strong industrial collaborations. The establishment of pilot lines can aid in addressing the challenges that arise during the scaling-up process. • In the gap from product to market application, the target use-cases for AZIBs are ambiguous at present. To provide a quantitative analysis, a systematic approach is needed for a techno-economic analysis of AZIB applications in specific scenarios. • Once the application scenarios are defined, constructing a complete industrial value chain is the next logical step. While this may require collective effort and investment, it is generally only a matter of time. To accelerate the progress of AZIB commercialization and navigate these four critical gaps, this thesis encompasses four major contributions made during my doctoral study. These contributions span across four dimensions: mechanisms, materials, industrial chain, and economic viability. They are summarized as follows: 1). Mechanisms: This thesis first offers an in-depth discussion and introduction of the core components of all types of aqueous zinc-based energy storage devices (AZDs), including the electrodes, electrolytes, separators, and configurations. Subsequently, it combines first-principles theory with various application demands, such as high capacity, high energy, high power, and ultra-high power, to explore the most inherently suitable core component combinations in the specific application scenarios. The study finds that AZIBs are particularly well-suited for high-power applications due to their safety advantages and electrochemical performances. 2). Materials: Building upon the deep exploration in mechanisms and high-power application scenarios, this thesis has developed a composite cathode based on polyaniline (PANI) and cobalt hexacyanoferrate (CoHCF), exhibiting excellent electrochemical performances. The results showed that the PANI was well-coated on CoHCF, thereby enhancing the electrical conductivity and Zn2+ transport kinetics. As a result, the as-prepared materials demonstrated remarkable specific capacity, good cycling durability (86.15% capacity retention over 5,000 cycles at 10 A g-1), high peak energy density (312 Wh kg-1 at 500 W kg-1), and superior power density (75,294 W kg-1 at 25 Wh kg-1). The excellent electrochemical performance confirms that PANI-CoHCF composites are promising cathode candidates for AZIBs in high power applications. 3). Industrial chain: This thesis introduces and discusses the cell structure, production lines, core materials, and electronic control and system integration for AZIBs. For the first time, various insights are presented, including: a). the theoretical configuration design for AZDs; b). optimal cell internal and external structures; c). manufacturing process design and their challenges; d). the current status of the core materials and components within the industrial chain; e). how AZIB integrate with electronic control and energy storage system integration. 4). Economic viability: Based on the insights gathered on mechanisms and the industrial chain, this thesis conducts a techno-economic analysis for AZIBs and compares it with other mainstream technologies. It introduces quantitative metrics like levelized cost of electricity (LCOE), net present value (NPV), and internal rate of return (IRR) as core parameters for the first time to offer a techno-economic comparison between AZIBs and other technological pathways. This work will serve as a cornerstone, enlightening both the industrial and academic communities by setting new benchmarks and outlining future research trajectories.

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