Research progress on the hierarchical structure and mechanical behaviors of phloem fibers
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摘要: 韧皮纤维是一种重要的非木质植物纤维，具有较好的力学性能和环境友好性，被广泛用于增强复合材料。在韧皮纤维细胞壁中，螺旋结构的纤维素被半纤维素、果胶、木质素等无定形基质聚合物包裹。随着纤维素微纤丝角度变化，形成了多薄层/壁层的细胞壁结构。这种不同层级细胞壁的组装构筑，对于韧皮纤维力学性能的产生与力学行为的表现均具有重要影响。本文总结了以麻为代表的韧皮纤维在组织层级、细胞层级、细胞壁层级及分子层级的结构特点；重点分析了不同微观尺度的构造特征对单轴拉伸过程中纤维力学行为的影响；最后对韧皮纤维层级结构与力学行为研究存在的问题及未来发展方向提出了建议和展望，以期为韧皮纤维的利用及多尺度仿生结构的构建提供新思路。Abstract: Phloem fiber (or Bast fiber), a kind of non-woody plant fiber, is widely used to reinforce composites due to its good mechanical properties and eco-friendliness. In the cell wall of phloem fiber, abundant cellulose microfibrils with the helical structure are embedded in an amorphous matrix composed of hemicellulose, pectin, and lignin. The variation of the cellulose microfibril angle forms a highly ordered hierarchical structure of the cell wall. The assembly structure and compositions at different scales are of great significance for mechanisms and principles of the excellent mechanical performance of phloem fiber. This work summarized the structural characteristics of phloem fibers represented by hemp and flax at the tissue level, cell wall level, ultrastructural level, and molecular level. The emphasis was focused on the underlying interactions at different levels which generated the special mechanical behavior of the phloem fibers during the axial stretching process. Finally, the existing problems were pointed out, and the development trends of future research were prospected. The extracted concepts may provide new ideas for improving the utilization of phloem fiber and serve as inspiration for biomimetic applications.
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Key words:
- bast fiber /
- cell wall /
- fracture failure /
- crystalline cellulose /
- mechanical behavior /
- plant fiber
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图 1 不同植物来源韧皮纤维的多层级结构示意图：((a)、(b)) 成熟亚麻茎秆横截面显微构造及局部放大图[2]；((c)、(d)) 青檀幼茎树皮横截面显微构造及局部放大图(未发表图片)；(e) 亚麻纤维束及其横断面SEM图像[14]；(f) 纤维束与细胞壁模型；(g) 亚麻单根纤维横截面示意图，细胞壁层厚度和不同化学成分的相对含量；((h)~(j)) 微纤丝、基元纤丝、纤维素示意图
Figure 1. Hierarchical structure of the different phloem fibers: ((a), (b)) Anatomical structure of the mature flax and the magnified view of the fiber bundles[2]; ((c), (d)) Anatomical structure of the juvenile bark of the wingceltis (P. tatarinowii) and the magnified view of the fiber bundles (unpublished images); (e) Flax fiber bundles and SEM image of the transverse section[14]; (f) Schematic of fiber bundles and the cell wall of the single phloem fiber; (g) Relative chemical content of different cell wall compositions in the flax cell wall, with marks about the thickness of different cell wall layers; ((h)-(j)) Schematic of microfibrils, element fibrils, and cellulose molecular chain
Vc—Vascular cambium; Ph—Phloem; Phf—Phloem fibers; Xyl—Xylem; NCP—Non-cellulosic polysaccharides (Hemicellulose, pectin, etc.); Other—Wax, proteins, minerals, etc.; Gn—Newly deposited layer of the gelatinous cell wall
图 2 韧皮纤维的多种缺陷及位错对断裂行为的影响：(a) 韧皮纤维中的缺陷可以分为两大类，即表面或整体的“不连续性”和“不均匀性”，如表面杂质、裂纹、层间分离、位错和扭曲[1]；((b)、(c)) 亚麻纤维束扭结带的电镜图及二次谐波成像图[18]；((d)、(e)) 亚麻的断裂行为，裂纹由表面大缺陷开始沿纤维纵向扩展，断面出现分丝帚化[20]
Figure 2. Different defects present in the phloem fibers and the influence of dislocation on the fracture: (a) Schematic illustration of different kinds of defects present in plant fibers divided between discontinuities and inhomogeneities at the surface or in bulk: Surface impurities, cracks, interlaminar decohesion, dislocations, and twisting[1]; ((b), (c)) SEM images and SHG images of kink-band regions in flax fibers[18]; ((d), (e)) Fracture behavior of a flax fiber, the cracks started from surface defects, extended longitudinally along the fiber, and the fibrillation occurred at the fractured ends[20]
图 3 韧皮纤维细胞壁超微构造：(a) 不同生长阶段的亚麻韧皮纤维细胞壁具有不同厚度的G层与Gn层[2]；(b) 亚麻韧皮纤维细胞壁层形成示意图及不同壁层的压弹模量[32]；(c) 成熟大麻初生韧皮纤维显示多壁层结构[33]；(d) 野梧桐(M. japonicus)韧皮纤维显示出厚-薄交替多层结构[36]
Figure 3. Ultrastructure of bast fiber cell wall: (a) Cell walls of flax phloem fibers at different growth stages showed different thicknesses of G and Gn layers[2]; (b) Atomic force microscopy (AFM) peak-force quantitative nano-mechanical (PF-QNM) mapping of the indentation modulus of developing flax fibers at top, middle, and bottom parts of the stem[32]; (c) Multilayered structure in the mature hemp primary phloem fibers[33]; (d) Multilayered structure in the phloem fibers of M. japonicas[36]
P—Primary wall; S1—Secondary wall; pf——Phloem fiber; L—Lignified layer; G—Gelatinous layer
图 4 纵向加载时具有不同微纤丝排列取向的细胞壁显示不同力学行为：(a) I—亚麻韧皮纤维断面显示微纤丝轴向取向[53]，II—山茱萸胶质纤维中G层内部到外部微纤丝取向逐渐变化[56]；(b) 细胞壁模拟设计概述[57]；(c) 3D打印圆柱的实验应力-应变曲线与形变构造[57]；(d) 基于有限元模拟的基质、微纤丝与纤维的相对应变能密度(SED)[57]
Figure 4. Cell wall layers with different microfibril orientations display different mechanical behavior under longitudinal loading: (a) I—Fracture surfaces of a flax fiber showing axial orientation of microfibrils[53]; II—Gradual change in microfibril orientation from the inner to outer parts of the G-layer in Cornaceae spp.[56]; (b) Overview of model design[57]; (c) Experimental stress-strain curves and deformed configurations of 3D-printed cylinders[57]; (d) Relative strain energy density (SED) adsorption in matrix, fibers, and fibrils from the finite element simulations[57]
S1—Inner secondary wall; S2—Middle secondary wall; S3—Outer secondary wall; ref.—Reference fibrils without S1 and S3 layer; vert.—Fibrils adding vertial S1 and S3 layer; horiz.—Fibrils adding horizontal S1 and S3 layer
图 5 (a) Iβ型纤维素结构示意图[60]；(b) 拉伸过程中纤维素分子链不同自由度的响应程度[61]；(c) 分子杠杆机制[65]；((d)~(f)) 使用分子动力学模拟Iβ纤维素在3个正交方向和3种应变速率下的单轴拉伸变形的结构示意图[69]
Figure 5. (a) Crystal structure of cellulose Iβ[60]; (b) Response to tensile strain in different degrees of freedom[61]; (c) A molecular scale leverage effect[65]; ((d)-(f)) Schematic of cellulose Iβ deformation under uniaxial tensile at three orthogonal directions with three different strain rates by using molecular dynamics (MD) simulations[69]
FⅡ—Tension parallel to the cellulose axis; ${{F}_{\bot }} $—Compression perpendicular to the cellulose axis
图 6 ((a)~(d)) 基于大麻韧皮纤维拉伸行为提出的假设[80]；(e) 微纤丝与半纤维素间界面的结构与相互作用机制[82]
Figure 6. ((a)-(d)) Schematic assumption based on the complex tensile behavior of hemp fiber[80]; (e) Structure and mechanics of the interfaces between hemicellulose and microfibrils[82]
ε12—Shear strain; ε2—Extensional across the interface; A—Attachment point between hemicellulose and cellulose before slip; A'—Attachment point between hemicellulose and cellulose after slip
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