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  • Two-dimensional Conjugated Polymers with Nanofluidic Channels for Quasi-solid-state Supercapacitors and Batteries
    (2024) Liang, Jiaxing
    Thesis
    Electrochemical energy systems (EESs), like supercapacitors (SCs) and batteries, are essential for sustainable societies. Nanofluidic two-dimensional conjugated polymers (2D CPs) as functional materials advance charge transport and storage in SCs and batteries, utilizing their in-plane conjugated networks and interlayer nanoconfined fluids as charge carriers’ paths. Their persistent lamellar structures further promote durability. Integrating nanofluidic 2D CPs with quasi-solid-state (QSS) device configurations is promising to synergistically enhance the functionalities of SCs and batteries with efficient charge transport in electrodes. Meanwhile, such study is lacking. This thesis explores the applications and kinetics of nanofluidic 2D CPs in QSS SCs and batteries. Recent advancements of 2D CPs in SCs and batteries are reviewed. Layered tungstate anion-linked polyaniline (TALP), featuring in-plane electronic conductive network and intrinsic nanoconfined fluids as ionic transport path, is selected as a model material for QSS SCs and batteries. The methodologies employed in this research are outlined, and the reproducibility of TALP is examined. The research first investigates TALP-based nanofluidic 2D CPs as active materials in low-temperature QSS zinc-ion hybrid capacitors (ZIHCs). Utilizing nanoconfined supercooled water, TALP exhibits superior ionic conduction and storage at sub-zero degrees, promoting the performance of as-obtained iced ZIHCs with a maximum areal energy of 580.0 µWh cm−2 at 43.3 mW cm−2. The following chapter describes the design of miniatured QSS lithium-ion batteries (LIBs) electrodes with TALP-based 2D CPs as nanofluidic fillers. The nanofillers with confined organic solvents endow rapid cation diffusion in ultracompact electrodes for QSS LIBs, rendering high volumetric capacity (266.7 mAh cm−3). The final session reports TALP-based nanofluidic 2D CPs as artificial cathode-electrolyte interphase (CEI) for QSS dual-ion batteries (DIBs). The layered artificial CEI permits efficient anion transport on graphite cathode while accommodating its large volume change and minimizing side reactions. These enable the development of sustainable QSS DIBs with high areal performance (1.78 mAh cm−2) and long lifespan (94% capacity retention after 2000 cycles). The versatile capabilities of TALP highlight the immense potential of nanofluidic 2D CPs in QSS SCs and batteries, revealing promising avenues for their future research and development.