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Title Page 1

초록 4

Abstract 5

Contents 6

Chapter 1. Introduction 10

Chapter 2. Results and Discussion 13

2.1. Preparation and chemical configuration of CMP 13

2.1.1. Preparation of CMP 13

2.1.2. Chemical configuration of CMP 13

2.2. Characterization of CMP 16

2.2.1. Electrical properties of CMP 16

2.2.2. Mechanical properties of CMP 19

2.3. Ink design and on-skin compatibility of CMP 22

2.3.1. CMP ink design for e-tattoo 22

2.3.2. On-skin biocompatibility of CMP e-tattoo 25

2.4. Demonstration of e-tattoo for healthcare applications 27

2.4.1. Demonstration of bioelectronics with CMP e-tattoo 27

2.4.2. CMP e-tattoo as electrochemical biosensors 32

Chapter 3. Conclusion 37

Chapter 4. Methods 38

4.1. Preparation of Pt-decorated CNTs 38

4.2. Preparation of CMP suspension 38

4.3. E-tattoo for electrical stimulation, photothermal heater, and ECG sensor 38

4.4. Fabrication of biosensor 38

4.5. Chemical characterization 39

4.6. Mechanical characterization 39

4.7. Electrical characterization 39

4.8. Biocompatibility test 39

4.9. Demonstrations 40

4.10. Experiments on human subjects 40

4.11. Statistical Analysis 40

Bibliography 41

List of Figures 7

Figure 1. CMP-based e-tattoo 11

Figure 2. Photograph of shadow mask for direct patterning of e-tattoo on skin 12

Figure 3. Schematic illustration of preparation of CMP suspension 13

Figure 4. A, Schematic configuration of LMP and CMP. B, Zeta potential and SEM image of composites 14

Figure 5. Schematic illustrations of preparing LMP suspension. Bulk LM splits into LMPs 14

Figure 6. A, Schematic illustrations of preparing CNT@Pt. B, TEM image of CNT@Pt 15

Figure 7. A, TEM image of CMP and EDS mapping of sulfur in CMP. B, Molecular structure of PSS.... 15

Figure 8. Photograph of LMP mixed with CNT@Pt without PSS. LMP and Pt-decorated CNT are not... 15

Figure 9. A, SEM images of CMP. B, Size distribution of CMP 15

Figure 10. Photograph of LED connected with CMP and LMP-based interconnects 16

Figure 11. TEM image and EDS of CMP 17

Figure 12. XPS of LMP and CMP with different composition 17

Figure 13. TEM image and Ga EDS mapping of CMP (A) and LMP (B). More Ga element is observed on... 18

Figure 14. A-B, Photograph of the resistance of CMP (435.5 Ω) (A) and LMP mixed with PSS and bare... 18

Figure 15. Sheet resistance according to CNT@Pt concentration 18

Figure 16. Schematic illustration (A) and photograph (B) of bar coating CMP suspension using Baker Type... 19

Figure 17. Normalized load applied on micro-tip as a function of normalized depth of CMP and LMP 20

Figure 18. SEM image of CMP and LMP before and after pressure compression 20

Figure 19. Scratch and peel-off test of CMP and LMP-based film by applying shear force 20

Figure 20. Schematic illustration of scratch (A) and peel-off (B) test of CMP film 21

Figure 21. A, Photographs of CMP, LMP, and LMP with PSS before and after rubbing. B-C, OM image of... 21

Figure 22. A, Photographs of CMP coated on the nitrile glove before and after strain. B, Resistance... 22

Figure 23. Schematic illustration of direct coating of CMP on skin 23

Figure 24. Zeta potential and contact angles of CMP suspension with different base solvent 23

Figure 25. Photographs of CMP and LMP suspensions. Wettability of suspension increases with the... 23

Figure 26. Contrast OM image and SEM image of coated CMP with different base solvent 24

Figure 27. OM top-view image and SEM cross-section image of coated CMP on pig skin with different... 24

Figure 28. Photograph of CMP coating on skin with different solvent 25

Figure 29. A, Photographs of ethanol-based ink immediately after preparation and after 5 days. B,... 25

Figure 30. WST-1 assay of 3T3 fibroblast cells upon exposure to SBS, CMP coated SBS and DMSO for 3... 26

Figure 31. Live/dead staining images of 3T3 fibroblast cells at day 1. Live cells in green, with dead cells in... 26

Figure 32. A, Photograph of experimental set-up for gas-permeability test. B, Loss of weight due to... 26

Figure 33. Photograph and OM image for measuring on-skin compatibility. CMP and bulk LM were coated... 27

Figure 34. A, Schematic illustration of e-tattoo-based electrical stimulator. B, Real-time activated EMG... 27

Figure 35. A, Infrared image of heated e-tattoo with laser (wavelength: 808 nm). B, Temperature change... 28

Figure 36. Cyclic temperature variation with different laser power 28

Figure 37. A, Photograph of simultaneous electrical muscle stimulation and thermal treatment on the... 29

Figure 38. A, Schematic illustration of e-tattoo-based wireless ECG monitoring system. B, ECG signals... 30

Figure 39. Schematic illustrations of experimental set-up for ECG monitoring with CMP-based e-tattoo... 30

Figure 40. Real-time ECG monitoring with e-tattoo and carbon electrodes under mechanical deformation 31

Figure 41. A, Photograph of compressed and stretched e-tattoo. B, ECG signal under application of... 31

Figure 42. A, Photograph of CMP-based e-tattoo before and after immersion in artificial sweat, B,... 31

Figure 43. Photograph of CMP-based e-tattoo before and after washing with soap 32

Figure 44. Photograph and mechanism of CMP-based electrochemical biosensor 33

Figure 45. A, Schematic illustrations of preparation of CMP-based electrochemical biosensor. WE:... 33

Figure 46. FTIR spectra variation according to materials 34

Figure 47. Impedance of LMP and CMP electrodes immersed in 0.1 M PBS (pH 7.4) over time 34

Figure 48. Current level according to concentration of biomarkers: glucose (A), ethanol (B), and lactate... 35

Figure 49. Chronoamperometric (CA) responses of glucose (A), alcohol (B), lactate sensor (C) 35

Figure 50. Continuous monitoring of glucose level 35

Figure 51. Selectivity test of biosensor with glucose. Real-time chronoamperometric response was measured... 36

초록보기

 기존의 병원 기반 진단 및 치료를 대체하기 위한 개인 맞춤의료 서비스에 대해 관심이 높아지면서, 사용자에게 최소한의 부담을 주는 웨어러블 기기를 활용한 디지털 헬스케어가 집중적으로 연구되고 있다. 이와 관련하여 주목할 만한 기술은 맞춤형 전자피부로, 그 중에서도 전자문신은 사용자의 체형 및 신체 부위에 맞춘 디자인으로 피부에 부착되어 다양한 생체신호를 수집해 사용자의 건강상태를 파악할 수 있다. 그러나 기존의 전자문신은 초박형 지지 기판을 요구하므로 실험실이나 공장에서 일률적인 공정을 통해 제작될 수밖에 없어, 맞춤의료 서비스를 위한 사용자의 요구를 즉석에서 반영하여 신속하고 간단한 개별 맞춤제작이 불가능하다. 본 연구에서는 사용자의 목적에 따라 다양한 디자인으로 간편하게 피부에 도포하여 구현할 수 있는 새로운 차원의 전자문신을 개발하였다. 갈륨 기반 액체 금속 입자(CMP)에 백금으로 기능화된 탄소나노튜브와 고분자를 부착한 후, 입자간의 낮은 전기적 반발력과 높은 습윤성 및 빠른 증발이 가능한 CMP 현탁액을 제작하여 10초 만에 피부 위에 발릴 수 있는 전자문신을 개발하였다. CMP 전자문신의 저렴한 비용, 준비 용이성, 고유 전기 전도성, 기계적 내구성, 생체 적합성 및 기능화 용이성으로 인해 심전도 신호 측정, 전기 근육 자극기, 광열 히터 및 전기화학적 바이오센서와 같은 다양한 헬스케어 분야에 적용 가능함을 확인하였다.

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