本研究結合仿生設計原理和積層製造技術，系統性地設計多種仿生複合材料，旨在透過優化生物材料的結構以提升機械性能，並找到其中的關連性。因傳統複合材料在製程上存在限制的設計自由度，難以製造較為複雜的幾何形狀，並且在複合材料的製造上存在相對脆弱的界面，易導致材料整體的失效。因此，受自然界中生物保護組織結構的啟發，我們從中獲取設計靈感，並利用先進的多材料3D列印技術改善原有問題。
這項研究的一個主要目標是探索植物和動物保護組織的結構與性能之間的關係，以利用自然結構的複雜性和多功能性來克服傳統複合材料所面臨的限制。論文中介紹了對Elaeocarpus ganitrus果核的研究結果，揭示了其優越的抗斷裂性和功能梯度材料特性。儘管密度僅為1 g/cm3，這些直徑20毫米的果核能夠承受高壓縮載荷。透過micro-CT進行的三維結構定量分析顯示，果核具有梯度微觀結構，其中包含硬度和剛性的梯度，由於其分層細胞結構所產生的增韌機制，果核能夠承受高達5000 N的載荷, 此種梯度設計策略在開發功能性梯度和分級材料的設計上具有應有潛力。
本研究亦調查了鯊魚皮齒的機械性能，並深入探討其功能適應及增強保護機制。在類琺瑯質外層中進行的奈米壓痕測試顯示，側面區域表現出最低的硬度（分別為3.9 GPa和4.2 GPa）和較低的彈性模量（分別為49 GPa和69 GPa）。而與底棲環境密切接觸的區域，如吻部、腹部和胸鰭，則具備較高的硬度和較低的彈性模量。吻部、腹部和胸鰭區域的硬度值分別為4.8 GPa、4.7 GPa和4.7 GPa。透過以上研究結果可歸結出，鯊魚皮齒類琺瑯質外層區域中，單向氟磷灰石晶體導致了機械性能的增強。這些結果說明White-spotted bamboo shark皮齒具有功能適應，其優化設計可提供增強的保護，透過三維重建可生成具有不同重疊機制和錐角的模型，藉由多材料3D列印技術進行製造，模仿嵌入在柔軟皮膚中的堅硬皮齒。這些以3D列印製成的皮齒模型可應用於流體流動模擬，並研究不同皮齒表面圖案的防污性能，以探究不同皮齒形狀和圖案對減少阻力的效果。此研究對於改進管道流體的運輸效率以及建立有效的防污策略具有重要意義。
這項研究涵蓋3D列印界面上的優化，以實現具備複雜界面仿生結構的複合材料的3D列印。其中包含多材料界面在拉伸、剪切和奈米尺度上的機械性能，以及界面材料厚度和列印方向對機械性質之影響，提供如何調節複合材料的剛度、強度和斷裂伸長率等性能特點的模型設計策略。
本研究介紹了由珠母層啟發之交錯複合材料的設計和受力變形行為。透過3D列印、多項機械性質試驗和分析計算，系統性地調查了tablet長寬比和交錯設計對複合材料硬化現象的影響。研究發現，複合材料中的硬化現象是可調節的，並且能夠增強複合材料的韌性和強度。總結來說，這項研究為生物材料結構與性能間的關係提供了更多發展性，同時為開發擁有更高機械性能的先進複合材料提供了重要的基礎和依據。

This thesis aims to contribute to the field of composite materials by incorporating bio-inspired design principles and additive manufacturing technique. The motivation behind this research lies in the limitations of conventional composites, which struggle to achieve complex geometries restricting design freedom, and exhibit weak interfaces between mechanically mismatched materials. Here we draw design inspiration from biological protective tissues found in nature and utilize state-of-the-art multimaterial 3D printing technology to overcome these challenges.
One of the key objectives is to explore the structure-property relationship of protective tissues in plants and animals that can address the limitations of conventional composites by leveraging the complexity and multifunctionality of natural structures. We present findings on the Elaeocarpus ganitrus endocarp, revealing its outstanding fracture tolerance and functionally graded material properties. Despite possessing a low density of 1 g/cm³, the 20 mm-sized endocarps showcase remarkable resilience against substantial compression forces. Micro-CT-based 3D structural analyses unveil a gradient microarchitecture inherent to the endocarp. Moreover, the endocarp's hardness and stiffness display a gradient profile. Leveraging the toughening mechanisms arising from its layered cellular structure, these endocarps demonstrate an impressive capacity to endure elevated loads of up to 5000 N. The gradient design principles established through this investigation offer valuable insights for the creation of functionally gradient and graded materials. Similarly, the mechanical properties of shark-skin denticles are investigated, uncovering their functional adaptations and enhanced protection. The nanoindentation tests on the denticle enameloid region showed that the flank regions exhibit the lowest hardness (3.9 GPa, and 4.2 GPa) and reduced elastic modulus (49 GPa, and 69 GPa). Whereas the regions likely to be in close contact with the benthic environment, like the snout, belly, and pectoral fins, showed higher values of hardness and reduced elastic modulus. The hardness values in the snout, belly, and pectoral fin regions were 4.8 GPa, 4.7 GPa, and 4.7 GPa, respectively. The enhanced mechanical properties concur with the unidirectional fluoroapatite crystals in the enameloid region. These results reveal functional adaptations of the denticles in white-spotted bamboo sharks that are optimized to provide enhanced protection. In addition, the three-dimensional reconstruction of the denticles of several shark species can be used to generate desired patterns with various overlapping and crown angles and 3D-print with multimaterial 3D-printing technique mimicking stiff denticle embedded in the soft skin. The 3D-printed denticle patterns can be used to study the fluid flow in tunnel experiments and study the antifouling of various denticle surface patterns. Importantly, the denticle 3D-models can be utilized to carry on fluid flow simulations and study the drag reduction of various denticle shapes and patterns. Furthermore, the thesis delves into optimizing polyjet printed interfaces for 3D printing complex interface composites capable of mimicking biological architectures. The study investigates the tensile, shear, and nano-mechanical properties of multimaterial stiff-soft interfaces. The thickness of the interfacial material and the orientation of the printed composites are examined, providing insights into tuning the stiffness, strength, and elongation at break of the composites.
Finally, the design and deformation behavior of nacre-inspired staggered composites are explored. Utilizing 3D printing, testing, and computation, the study investigates the impact of tablet aspect ratio and interlocking designs on the hardening phenomena observed in these composites. The hardening phenomena discovered here is tunable and is capable of enhancing the toughness and strength of the composites. Overall, the findings provide valuable insights into the structure-property relationships of biological materials and offer guidance for the development of advanced composite designs with enhanced mechanical performance.

Abstract (Chinese) i
Abstract (English) iii
Acknowledgements v
Table of Contents vi
List of Figures ix
List of Tables xvi
CHAPTER ONE 1
Introduction 1
1.1 Composites and their limitations 1
1.2 Biological Protective tissues 3
1.3 Thesis approach and organization 4
CHAPTER TWO 8
Literature Review 8
2.1 Protective tissues in nature 8
2.1.1 Nacre 8
2.1.2 Teeth and denticles 10
2.1.3 Hard plant shells 13
2.2 Additive Manufacturing 17
CHAPTER THREE 18
Methodology 18
3.1 Biological structure reconstruction 18
3.2 Additive manufacturing 21
3.2.1 Stereolithography printing technique 22
3.2.2 PolyJet 3D printing 25
3.3 Mechanical Testing 30
3.3.1 Universal testing machine 30
3.3.2 Nanoindentation 32
CHAPTER FOUR 34
Structure and property investigation of protective tissues in nature 34
4.1 Elaeocarpus ganitrus endocarp 34
4.1.1 Materials and methods 35
4.1.2 Microscopic and tomographic structural analysis 37
4.1.3 Mechanical properties of Elaeocarpus ganitrus endocarp 40
4.1.4 Fracture morphologies and mechanisms 44
4.1.5 Conclusions 47
4.2 Shark-skin denticles 57
4.2.1 Introduction of shark-skin denticles 57
4.2.2 Materials and methods 57
4.2.3 Microstructure of white-spotted bamboo shark denticle 58
4.2.4 Elemental composition of white-spotted bamboo shark denticle 59
4.2.5 Mechanical properties of white-spotted bamboo shark denticle 59
4.2.6 Three-dimensional structure reconstruction 65
4.3 Structure-property-mechanisms of nacre 79
CHAPTER FIVE 80
Mechanical properties of polyjet 3D- printed stiff-soft interface composites 80
5.1 Introduction to polyjet 3D- printed stiff-soft interface composites 80
5.1.1 Literature review 81
5.2 Composite design and manufacturing 84
5.2.1 Design and manufacturing of tensile and shear interface composites 84
5.2.2 Composite characterization 85
5.3 Microstructure, mechanical properties and fracture mechanisms 86
5.3.1 Microstructure of the interface 86
5.3.2 Tensile interface composites 86
5.3.3 Shear interface composites 88
5.3.4 Tensile - Shear interface Composites 90
5.3.5 Fracture morphologies and mechanisms of TSICs 94
5.3.6 Nanoindentation on the stiff-soft interface 96
5.4 Conclusions 97
CHAPTER SIX 109
Nacre-inspired composites with Tunable Mechanical Properties 109
6.1 Introduction to nacre and nacre-inspired 3D-printed composites 109
6.1.1 Nacre inspired brick-and-mortar composites 109
6.2 Composite designs and manufacturing 111
6.2.1 Design and specification 111
6.2.2 3D-printing and tensile testing 112
6.2.3 Simulation procedures using 2D-LSM (lattice spring model) 113
6.3 Mechanical properties of RT and IT composites 115
6.3.1 Experimental tensile test response of RT and IT composites 115
6.3.2 Softening stages of RT and IT composite 115
6.3.3 Tunable Interface hardening in RT and IT composite 116
6.4 Fracture mechanisms and morphologies 119
6.5 LSM (Lattice spring model) simulation results 121
6.5.1 Comparison between simulation and experimental tensile response 121
6.5.2 Stress distribution at various fracture stages 122
6.6 Conclusions 124
CHAPTER SEVEN 138
Conclusions and Outlook 138
7.1 Summary and Conclusions 138
References 140

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