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Catalyst Design and Interface Engineering for Aqueous Zinc-Iodine and Dry-Electrode Lithium-Ion Batteries

  • 정민주 (아주대학교 일반대학원)

초록/요약

The commercialization of next-generation rechargeable batteries requires both high performance electrode materials and reliable fabrication processes. This thesis presents two studies, one addressing each aspect. First, to address the sluggish iodine redox kinetics and polyiodide shuttle of aqueous zinc–iodine batteries （AZIBs）, a trimetallic single-atom catalyst （CuFeSn-NC） with Cu, Fe, and Sn atomically dispersed in a nitrogen-doped carbon framework was designed as an iodine host. Integrating the complementary functions of these three active sites addressed the limitations of monometallic catalysts, enhancing iodine conversion reversibility and suppressing the polyiodide shuttle. The CuFeSn-NC@I₂ electrode delivered reversible capacities of 255.4 and 235.2 mAh g⁻¹ at 0.5 and 1 A g⁻¹, retained ~200 mAh g⁻¹ with 99.8% Coulombic efficiency over 10,000 cycles at 5 A g⁻¹, and maintained 145–150 mAh g⁻¹ over 5,000 cycles at 10 A g⁻¹, outperforming the corresponding monometallic counterparts. Second, to mitigate the low electrode–current collector adhesion and delamination in the dry electrode process of lithium-ion batteries, current collectors were coated with an SWCNT primer by sono coating. The CMC/SWCNT and PVdF/SWCNT primers exhibited a trade-off between electrochemical performance and surface morphology. To exploit these complementary characteristics, a dual-primer strategy applying both via dual-nozzle sono coating was proposed. The resulting dual-primer current collector showed improved discharge capacity and stable cycling, even at high mass loading, improving the reliability of dry electrode fabrication. Overall, the trimetallic catalyst enhanced reversible iodine conversion, while the dual-primer current collector improved both the performance and process reliability of dry electrodes. These studies highlight the importance of both electrode material design and fabrication-process engineering for developing next-generation rechargeable batteries. Keywords: Aqueous zinc–iodine batteries, Iodine cathode, Interfacial Engineering, Single-atom catalyst, Trimetallic active sites, Dry Electrodes, Ultrasonic coating, Current Collector Primers

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목차

Chapter 1. Introduction. 1
Chapter 2. Trimetallic Atomic Catalyst for Polyiodide Regulation and Fast Redox Conversion in Durable Zinc–Iodine Batteries 3
2.1 Introduction 3
2.2 Experimental Section 6
2.2.1 Synthesis of CuFeSn-NC 6
2.2.2 Preparation of CuFeSn-NC@I₂ Cathode 6
2.2.3 Electrode Preparation 6
2.3 Material Characterizations 7
2.4 Electrochemical Measurements 7
2.5 Results and Discussion 9
2.5.1 Structural Characterization and Atomic Dispersion of CuFeSn-NC 9
2.5.2 Polyiodide Adsorption Capability of CuFeSn-NC 22
2.5.3 Electrochemical Behavior and Charge-Storage Analysis 25
2.5.4 Electrochemical Performance of CuFeSn-NC@I₂ Cathode 31
2.5.5 Discussion on the Balanced Iodine Regulation Mechanism 38
2.6 Conclusion 40
Chapter 3. Dual Primer Current Collectors Fabricated by Dual Nozzle Sono Coating for Dry Electrode Lithium-Ion Batteries 41
3.1 Introduction 41
3.2 Experimental Section 43
3.2.1 Preparation of CMC/SWCNT Primer 43
3.2.2 Preparation of PVdF/SWCNT Primer 43
3.2.3 Fabrication of Dual Primer Current Collectors 43
3.2.4 Dry Electrode Preparation 43
3.2.5 Electrochemical Measurements 44
3.3 Results and Discussion 45
3.3.1 Surface Morphology of SWCNT Primers 45
3.3.2 Optimization of Primer Type and Coating Cycles 50
3.3.3 Electrochemical Performance of Dual Primer Current Collectors 55
3.4 Conclusion 60
Chapter 4. General Conclusions 61
Reference 63

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