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    One-dimensional carbon-based materials and electrode architecture for advanced flexible Li-ion batteries = 고성능 유연 리튬 이온배터리를 위한 1차원 탄소기반 재료 및 전극구조 설계 연구

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    https://www.riss.kr/link?id=T16950392

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    국문 초록 (Abstract) kakao i 다국어 번역

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    유연 리튬이온전지의 가장 중요한 요소는 변형된 상태에서도 에너지 저장 성능을 유지해야 한다는 것이다. 하지만, 기존에 사용되던 리튬이온전지들은 특히 구리나 알루미늄 집전체와 같은 구성품들로 인하여 잘 구부러지지 않기 때문에 유연성을 얻기가 힘든 상황이다. 따라서, 금속 집전체를 사용하지 않는 탄소기반의 독립된 전극을 제조하는 기술은 유연 리튬이온전지의 유연성 한계를 극복하기 위한 유망한 기술 중 하나이다. 하지만, 독립된 유연전극은 세 가지 주요한 문제를 동반한다: (1) 제한된 활물질의 종류에 의한 낮은 비용량, (2) 금속 집전체를 사용한 전극과 비교하여 낮은 전기 전도도, 그리고 (3) 반복되는 변형 조건을 버티기 어려운 약한 기계적 물성. 이러한 관점에서, 1차원 현상을 갖는 탄소 재료를 활용하여 매우 유연한 독립된 전극을 제조하는 것은 위에 언급된 한계들을 극복하기 위해 진행되어야 하는 중요한 연구 분야 중 하나이다. 본 연구에서는 유연소자에 적용하기 위하여, 1차원 탄소 재료들의 개질과 그들을 활용한 독립된 유연 전극의 제조에 대한 접근 전략을 중점적으로 진행하였다. 챕터 2에서는 아연 산화/황화물이 증착된 황-도핑 탄소나노섬유의 복합 구조가 보고되었으며, 이는 전기방사 방법과 뒤이은 원자층 증착법에 의하여 제조되었다. 이러한 독특한 복합 구조를 형성함으로써, 아연 산화/황화물의 뛰어난 확산 특성과 황-도핑 탄소나노섬유의 높은 전기전도도의 장점을 동시에 달성할 수 있었다. - 192 특히, 아연 산화/황화물의 충전 및 방전 반응 동안 리튬이온의 매우 가역적인 변환 및 합금화 반응이 확인되었다. 더하여, 아연 산화물과 아연 황화물의 계면에서 리튬이온의 수송을 촉진할 수 있는 격자의 변형이 확인되었다. 챕터 3에서 다공성 탄소 매트릭스의 하이드록시 기능화를 통하여 단백질의 도움을 받은 유연하고 구리가 없는 음극을 개발하였다. 아연산화물 나노입자와 글루타민산을 개질 요소로 이용하여, 풍부한 하이드록시기와 잘 발달된 메조기공을 갖는 질소-도핑 탄소나노섬유를 성공적으로 합성하였다. 이러한 특징은 에너지 저장 성능을 향상 시킬 수 있도록 리튬이온 확산성 및 전기전도도를 크게 향상시켰다. 또한, 하이드록시 기능화된 탄소나노섬유 표면 작용기로 인하여 유연성이 크게 향상되었음을 확인할 수 있었다. 챕터 4에서는 매우 유연한 리튬이온전지용 음극 개발을 위해 코발트 산화물이 복합화된 메조기공 탄소나노섬유의 양자점을 통해 유도된 탄소나노주머니의 효과가 제안되었다. 메조기공을 갖는 탄소나노섬유와 탄소 나노주머니에 의해 성장이 제한된 코발트 산화물 나노입자는 탄소 양자점과 코발프 전구체에 의하여 성공적으로 제조되었다. 최적화된 샘플을 이용하여 제조된 유연전극은 차기 산화공정을 통하여 메조기공이 잘 발달되었음을 확인하였고, 높은 메조기공 부피율을 보였다. 이러한 유연전극은 변형된 상태에서도 뛰어난 에너지 저장성능을 보였다. 챕터 5는 수계 기반 연속 스프레이 전극 설계 시스템을 이용하여 매우 유연한 독립된 전극을 보고하였다. 최적화된 유연 전극은 탄소나노섬유 뼈대에 실리콘 나노입자와 탄소나노튜브 얽힘구조를 갖는 독특한 복합구조를 나타냈으며, 이를 통하여 물리적 및 전기화학 특성의 큰 향상을 보고하였다. 특히, 최적화된 유연전극은 강하게 결합되어있는 탄소나노섬유 뼈대, 실리콘 나노입자, 탄소나노튜브 망으로 인하여 3,000회의 유연성 평가 이후에도 구조적 안정성 및 전기화학 특성을 유지할 수 있었다. 따라서, 이러한 탄소나노섬유 개질 전략과 이를 이용한 독립된 유연전극 설계 연구는 유연 리튬이자전지 적용이 가능한 유력 후보가 될 수 있을 것으로 판단된다.
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    유연 리튬이온전지의 가장 중요한 요소는 변형된 상태에서도 에너지 저장 성능을 유지해야 한다는 것이다. 하지만, 기존에 사용되던 리튬이온전지들은 특히 구리나 알루미늄 집전체와 같은...

    유연 리튬이온전지의 가장 중요한 요소는 변형된 상태에서도 에너지 저장 성능을 유지해야 한다는 것이다. 하지만, 기존에 사용되던 리튬이온전지들은 특히 구리나 알루미늄 집전체와 같은 구성품들로 인하여 잘 구부러지지 않기 때문에 유연성을 얻기가 힘든 상황이다. 따라서, 금속 집전체를 사용하지 않는 탄소기반의 독립된 전극을 제조하는 기술은 유연 리튬이온전지의 유연성 한계를 극복하기 위한 유망한 기술 중 하나이다. 하지만, 독립된 유연전극은 세 가지 주요한 문제를 동반한다: (1) 제한된 활물질의 종류에 의한 낮은 비용량, (2) 금속 집전체를 사용한 전극과 비교하여 낮은 전기 전도도, 그리고 (3) 반복되는 변형 조건을 버티기 어려운 약한 기계적 물성. 이러한 관점에서, 1차원 현상을 갖는 탄소 재료를 활용하여 매우 유연한 독립된 전극을 제조하는 것은 위에 언급된 한계들을 극복하기 위해 진행되어야 하는 중요한 연구 분야 중 하나이다. 본 연구에서는 유연소자에 적용하기 위하여, 1차원 탄소 재료들의 개질과 그들을 활용한 독립된 유연 전극의 제조에 대한 접근 전략을 중점적으로 진행하였다. 챕터 2에서는 아연 산화/황화물이 증착된 황-도핑 탄소나노섬유의 복합 구조가 보고되었으며, 이는 전기방사 방법과 뒤이은 원자층 증착법에 의하여 제조되었다. 이러한 독특한 복합 구조를 형성함으로써, 아연 산화/황화물의 뛰어난 확산 특성과 황-도핑 탄소나노섬유의 높은 전기전도도의 장점을 동시에 달성할 수 있었다. - 192 특히, 아연 산화/황화물의 충전 및 방전 반응 동안 리튬이온의 매우 가역적인 변환 및 합금화 반응이 확인되었다. 더하여, 아연 산화물과 아연 황화물의 계면에서 리튬이온의 수송을 촉진할 수 있는 격자의 변형이 확인되었다. 챕터 3에서 다공성 탄소 매트릭스의 하이드록시 기능화를 통하여 단백질의 도움을 받은 유연하고 구리가 없는 음극을 개발하였다. 아연산화물 나노입자와 글루타민산을 개질 요소로 이용하여, 풍부한 하이드록시기와 잘 발달된 메조기공을 갖는 질소-도핑 탄소나노섬유를 성공적으로 합성하였다. 이러한 특징은 에너지 저장 성능을 향상 시킬 수 있도록 리튬이온 확산성 및 전기전도도를 크게 향상시켰다. 또한, 하이드록시 기능화된 탄소나노섬유 표면 작용기로 인하여 유연성이 크게 향상되었음을 확인할 수 있었다. 챕터 4에서는 매우 유연한 리튬이온전지용 음극 개발을 위해 코발트 산화물이 복합화된 메조기공 탄소나노섬유의 양자점을 통해 유도된 탄소나노주머니의 효과가 제안되었다. 메조기공을 갖는 탄소나노섬유와 탄소 나노주머니에 의해 성장이 제한된 코발트 산화물 나노입자는 탄소 양자점과 코발프 전구체에 의하여 성공적으로 제조되었다. 최적화된 샘플을 이용하여 제조된 유연전극은 차기 산화공정을 통하여 메조기공이 잘 발달되었음을 확인하였고, 높은 메조기공 부피율을 보였다. 이러한 유연전극은 변형된 상태에서도 뛰어난 에너지 저장성능을 보였다. 챕터 5는 수계 기반 연속 스프레이 전극 설계 시스템을 이용하여 매우 유연한 독립된 전극을 보고하였다. 최적화된 유연 전극은 탄소나노섬유 뼈대에 실리콘 나노입자와 탄소나노튜브 얽힘구조를 갖는 독특한 복합구조를 나타냈으며, 이를 통하여 물리적 및 전기화학 특성의 큰 향상을 보고하였다. 특히, 최적화된 유연전극은 강하게 결합되어있는 탄소나노섬유 뼈대, 실리콘 나노입자, 탄소나노튜브 망으로 인하여 3,000회의 유연성 평가 이후에도 구조적 안정성 및 전기화학 특성을 유지할 수 있었다. 따라서, 이러한 탄소나노섬유 개질 전략과 이를 이용한 독립된 유연전극 설계 연구는 유연 리튬이자전지 적용이 가능한 유력 후보가 될 수 있을 것으로 판단된다.

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    다국어 초록 (Multilingual Abstract) kakao i 다국어 번역

    영어
    한국어
    Title: One-dimensional carbon-based materials and electrode architecture for advanced flexible Li-ion batteries
    The flexible lithium-ion batteries (LIBs) primarily require the electrodes to withstand repeated deformation stresses, maintaining their energy storage performance. However, owing to the rigidity of conventional electrodes, achieving deformability is difficult, mainly because of the use of a metal foil current collector (Cu and Al). Thus, developing carbon-based self-supporting electrodes without a metal current collector is a promising strategy to overcome the limitations of electrode deformability in flexible LIBs. However, self-supporting electrodes exhibit three main problems: (1) low specific capacity owing to the restricted types of active materials, (2) relatively low electrical conductivity compared with conventional electrodes with metal current collectors, and (3) poor mechanical strength for maintaining electrode structure under the repeated deformable condition. In this stream, designing highly deformable self-supporting electrode using one-dimensional materials has suggested as promising research field to overcome aforementioned limitations. In this study, advanced approaches on the modification of one-dimensional carbon materials and following construction of highly deformable self-supporting flexible electrodes for the flexible LIBs application. In chapter II, novel hybrid structure of ZnOS lamination layer on S-doped CNF matrix is reported using electrospinning method and sequential ALD process. Through the development of the novel hybrid structure, superior kinetic property of ZnOS and high electrical conductivity of S-doped CNF can be achieved. It should be noted that during the charge/discharge process of ZnOS, a highly reversible conversion and alloying reaction with Li-ion occurs. Moreover, the distorted lattice structure at the interfacial region of ZnO/ZnS can facilitate the Li-ion transportation. In chapter III, a protein-assisted bendable Cu-free anode was developed using a hydroxy-functionalized mesoporous carbon matrix. Using ZnO nanoparticles and glutamic acid as modification agents, a well-developed mesoporous CNF structure with N dopants and rich hydroxy groups was successfully synthesized. This resulted in the excellent lithium-ion diffusion kinetics and enhanced electrical conductivity for the optimized electrode, which significantly improved the energy storage performance and flexibility. In chapter IV, quantum dot-induced carbon nanopocket effect of cobalt oxide-embedded mesoporous carbon nanofibers is proposed for highly flexible LIB anodes. A mesoporous carbon nanofiber with carbon nanopocket-confined cobalt oxide was developed using carbon quantum dots and a cobalt precursor. The resultant flexible electrode exhibited well-developed mesoporous morphology during the post-oxidation process, with a high mesopore volume fraction. The optimized flexible electrode demonstrated superior lithium-ion storage capability even under the repeated deformable condition. In chapter V, the highly flexible self-supporting electrode is developed using a water-solvent-based continuously spraying-electrode architecture system. The resultant flexible electrode exhibited a novel hybrid composite structure of the carbon nanofiber framework and Si nanoparticles with a carbon nanotube interlocking network, which noticeably improved its physical and electrochemical properties. In particular, the optimized flexible electrode maintained its structural stability even after 3,000 cycles of flexibility testing because of the tight combination of the carbon nanofiber framework and Si nanoparticels with the carbon nanotube interlocking layer. Therefore, the modification strategies of carbon nanofibers and following construction of highly deformable self-supporting electrodes can be a promising candidate for the flexible LIBs application. Keywords: Flexible lithium-ion batteries, carbon-based materials, one-dimensional materials, surface engineering, flexible electrode architecture.
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    Title: One-dimensional carbon-based materials and electrode architecture for advanced flexible Li-ion batteries The flexible lithium-ion batteries (LIBs) primarily require the electrodes to withstand repeated deformation stresses, maintaining their ...

    Title: One-dimensional carbon-based materials and electrode architecture for advanced flexible Li-ion batteries
    The flexible lithium-ion batteries (LIBs) primarily require the electrodes to withstand repeated deformation stresses, maintaining their energy storage performance. However, owing to the rigidity of conventional electrodes, achieving deformability is difficult, mainly because of the use of a metal foil current collector (Cu and Al). Thus, developing carbon-based self-supporting electrodes without a metal current collector is a promising strategy to overcome the limitations of electrode deformability in flexible LIBs. However, self-supporting electrodes exhibit three main problems: (1) low specific capacity owing to the restricted types of active materials, (2) relatively low electrical conductivity compared with conventional electrodes with metal current collectors, and (3) poor mechanical strength for maintaining electrode structure under the repeated deformable condition. In this stream, designing highly deformable self-supporting electrode using one-dimensional materials has suggested as promising research field to overcome aforementioned limitations. In this study, advanced approaches on the modification of one-dimensional carbon materials and following construction of highly deformable self-supporting flexible electrodes for the flexible LIBs application. In chapter II, novel hybrid structure of ZnOS lamination layer on S-doped CNF matrix is reported using electrospinning method and sequential ALD process. Through the development of the novel hybrid structure, superior kinetic property of ZnOS and high electrical conductivity of S-doped CNF can be achieved. It should be noted that during the charge/discharge process of ZnOS, a highly reversible conversion and alloying reaction with Li-ion occurs. Moreover, the distorted lattice structure at the interfacial region of ZnO/ZnS can facilitate the Li-ion transportation. In chapter III, a protein-assisted bendable Cu-free anode was developed using a hydroxy-functionalized mesoporous carbon matrix. Using ZnO nanoparticles and glutamic acid as modification agents, a well-developed mesoporous CNF structure with N dopants and rich hydroxy groups was successfully synthesized. This resulted in the excellent lithium-ion diffusion kinetics and enhanced electrical conductivity for the optimized electrode, which significantly improved the energy storage performance and flexibility. In chapter IV, quantum dot-induced carbon nanopocket effect of cobalt oxide-embedded mesoporous carbon nanofibers is proposed for highly flexible LIB anodes. A mesoporous carbon nanofiber with carbon nanopocket-confined cobalt oxide was developed using carbon quantum dots and a cobalt precursor. The resultant flexible electrode exhibited well-developed mesoporous morphology during the post-oxidation process, with a high mesopore volume fraction. The optimized flexible electrode demonstrated superior lithium-ion storage capability even under the repeated deformable condition. In chapter V, the highly flexible self-supporting electrode is developed using a water-solvent-based continuously spraying-electrode architecture system. The resultant flexible electrode exhibited a novel hybrid composite structure of the carbon nanofiber framework and Si nanoparticles with a carbon nanotube interlocking network, which noticeably improved its physical and electrochemical properties. In particular, the optimized flexible electrode maintained its structural stability even after 3,000 cycles of flexibility testing because of the tight combination of the carbon nanofiber framework and Si nanoparticels with the carbon nanotube interlocking layer. Therefore, the modification strategies of carbon nanofibers and following construction of highly deformable self-supporting electrodes can be a promising candidate for the flexible LIBs application. Keywords: Flexible lithium-ion batteries, carbon-based materials, one-dimensional materials, surface engineering, flexible electrode architecture.

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    목차 (Table of Contents)

    • Summary ⅰ
    • List of tables ⅶ
    • List of figures ⅷ
    • List of symbols ⅹⅶ
    • I. Introduction 1
    • Summary ⅰ
    • List of tables ⅶ
    • List of figures ⅷ
    • List of symbols ⅹⅶ
    • I. Introduction 1
    • 1. Background and thesis overview 1
    • 2. Lithium-ion batteries 9
    • 2.1 Principle of Li-ion Battery 9
    • 2.2 Components 21
    • 2.3 Flexible lithium-ion batteries 37
    • 2.4 Electrode designing 45
    • 2.5 Performance evaluation 50
    • 3. Methods 53
    • 3.1 Electrospinning 53
    • 3.2 Vacuum filtration 54
    • 3.3 Ultrasonic spraying 55
    • 4. References 56
    • II. Metal compound-laminated S-doped carbon nanofibers 59
    • 1. Introduction 59
    • 2. Experimental Section 62
    • 2.1 Synthesis of ZnO/ZnS laminated carbon nanofibers 62
    • 2.2 Characterization 63
    • 3. Results and Discussion 65
    • 4. Conclusion 84
    • 5. References 85
    • III. Tailoring surface functional groups of carbon nanofibers 89
    • 1. Introductions 89
    • 2. Experimental Section 92
    • 2.1 Synthesis of protein-assisted bendable Cu-free anode 92
    • 2.2 Characterization 93
    • 3. Results and Discussion 94
    • 4. Conclusion 111
    • 5. References 112
    • IV. Co3O4 nanoparticles embedded mesoporous carbon nanofibers using carbon
    • quantum dots 117
    • 1. Introduction 117
    • 2. Experimental Section 121
    • 2.1 Synthesis of carbon nanopocket-confined Co3O4 within mesoporous carbon
    • nanofibers 121
    • 2.2 Characterization 122
    • 3. Results and Discussion 124
    • 4. Conclusion 145
    • 5. References 146
    • V. Developing highly flexible electrode through carbon nanotube interlocking
    • network 152
    • 1. Introduction 152
    • 2. Experimental Section 156
    • 2.1 Synthesis of carbon nanotube-interlocked self-supporting electrode 156
    • 2.2 Characterization 157
    • 3. Results and Discussion 159
    • 4. Conclusion 181
    • 5. References 182
    • VI. Conclusion 188
    • Abstract in Korean 191
    • List of Publications 193
    • List of Patents 196
    • List of Awards and Scholarship 197
    • Acknowledgments
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