基于非共价化学的绿色生物可循环肽材料

doi:10.11949/0438-1157.20231293

摘要/Abstract

摘要：

作为一种生物分子构建单元，肽具有生物相容性、可降解性、多功能性和序列可调性等特性。利用肽分子的非共价化学，可以实现具有多尺度结构的新型材料的可控构建，为开发生态友好、生物可降解和生物再利用的绿色生物可循环材料提供了新策略。然而，如何利用肽非共价化学策略进行单分子设计，并实现绿色生物可循环材料的可控构建和功能化应用，面临着重要挑战。本文从肽分子间的弱相互作用力协同角度，介绍肽非共价化学的策略，并详细阐述实现绿色生物可循环肽材料可控构建的单分子设计策略。最后，对基于非共价化学的绿色生物可循环肽材料在仿生光合成和光催化、药物递送和疾病诊疗以及可加工材料等领域的应用进行综述。

关键词: 非共价化学, 肽, 制备, 安全, 生物可循环性

Abstract:

Peptides, as a class of biomolecular building units, have biocompatibility, biodegradability, versatility, and sequence diversity, and can form novel materials with multi-scale structures through noncovalent chemistry. The emergence of these peptide based noncovalent chemical materials provides a method for developing eco-friendly, biodegradable and biorecyclable green biorecyclable materials. However, achieving controllable construction and functionalization of materials from single molecule design through noncovalent chemistry of peptides remains a challenge. Therefore, the article first introduced what noncovalent chemistry of peptides is, mainly describing weak intermolecular interactions. Then, it summarized how to achieve controllable construction of peptide materials from single molecule design, mainly introducing three design strategies. Finally, the applications of peptide-based materials, including biomimetic photosynthesis and photocatalysis, drug delivery and disease diagnosis and therapy, as well as processable materials, were reviewed.

Key words: noncovalent chemistry, peptides, preparation, safety, biorecyclability

中图分类号:

TQ 028.8

常蕊, 邢蕊蕊, 闫学海. 基于非共价化学的绿色生物可循环肽材料[J]. 化工学报, 2024, 75(4): 1317-1332.

Rui CHANG, Ruirui XING, Xuehai YAN. Green and biorecyclable materials based on peptide noncovalent chemistry[J]. CIESC Journal, 2024, 75(4): 1317-1332.

图/表 12

图1 基于肽非共价化学的从单分子设计到肽材料的可控构建及应用

Fig.1 Controlled construction and application of peptide materials from single molecule design based on peptide noncovalent chemistry

图2 操纵肽的非共价相互作用促进多尺度结构的形成[21]（1 Å =0.1 nm）

Fig.2 Manipulating noncovalent interactions of peptides to promote the formation of multiscale structures[21]

图3 Fmoc-FF自组装形成的β-折叠纳米纤维向α-螺旋纳米纤维转变的机理图[24]

Fig.3 Mechanism diagram of the transition from β-sheet nanofibers to α-helix nanofibers formed by Fmoc-FF self-assembly[24]

图4 （a）FF的分子结构；（b）Cyclo-（Leu-Phe）自组装形成超分子纤维状水凝胶示意图[35]；（c）两亲肽分子KFE8的嵌段异手性类似物及形成组装体的负染透射电子显微镜（TEM）图像[36]

Fig.4 (a) Molecular structure of FF; (b) Schematic diagram of supramolecular fibrous hydrogel formed by self-assembly of Cyclo-(Leu-Phe)[35]; (c) Negative-stain transmission electron microscopy (TEM) images of block heterochiral analogs of the amphipathic peptide KFE8 and the formation of assemblies[36]

图5 （a）微球结构的扫描电子显微镜（SEM）图[39]；（b）纤维束的TEM图[40]；（c）交叉偏振器下正交光纤维束交叉点处各向异性光致发光的消光（如箭头所示）[40]；（d）纤维束和J聚集体的圆二色谱[40]；（e）Z-HF、Zn2+和Ce6分子结构；（f）Z-HF/Zn2+/Ce6纳米颗粒的粒径和SEM图[42]；（g）TP5和ICG的分子结构；（h）纳米纤维的TEM图和原子力显微镜（AFM）图[43]

Fig.5 (a) Scanning electron microscopy (SEM) image of microsphere structure[39]; (b) TEM image of fiber bundles[40]; (c) Extinction of anisotropic photoluminescence (as denoted by arrows) at the cross-points of orthogonal fiber bundles under crossed polarizers[40]; (d) Circular dichroism of fiber bundles and J-aggregates[40]; (e) Molecular structure of Z-HF, Zn2+, and Ce6; (f) Particle size and SEM image of Z-HF/Zn2+/Ce6 nanoparticles[42]; (g) Molecular structure of TP5 and ICG; (h) TEM image and atomic force microscopy (AFM) image of nanofibers[43]

图6 其他分子修饰肽形成缀合物的分子结构

Fig.6 The molecular structure of other molecules modifying peptides to form conjugates

表1 基于非共价化学设计肽材料的三种策略的优缺点及应用范围

Table 1 Advantages， disadvantages， and application scope of three strategies for designing peptide materials based on noncovalent chemistry

策略名称	构筑基元	优势	不足	应用范围
特定肽序列的自组装	肽序列	简单、易操作	受限于自身具备的性质及结构赋予的性质	疾病相关蛋白纤维化的机理研究、生物光学和光电设备、3D组织培养
其他分子调控肽自组装	其他分子、肽序列	增加新功能和结构	易泄漏、装封率不可控	光催化、成像、光动力/热治疗、免疫治疗
其他分子与肽生成缀合物的自组装	其他分子-肽缀合物	增加稳定性、可控装封率	缀合物需分离提纯，或需引用连接剂，过程复杂	光动力/热治疗、成像、载药、化疗

图7 集光分子卟啉和肽在“益生元汤”中的分子演变示意图[55]

Fig.7 Schematic diagram of molecular evolution of light harvesting molecular porphyrin and peptides in “prebiotic soup”[55]

图8 （a）戊二醛（GA）辅助CDP交联自组装过程示意图；（b）肽基纳米球的粒径、电位和TEM图[61]

Fig.8 (a) Schematic diagram of glutaraldehyde (GA)-assisted CDP cross-linking self-assembly process; (b) Particle size, potential, and TEM image of peptide based nanospheres[61]

图9 （a）TPP-G-FF自组装形成纳米点示意图；（b）纳米点的粒径和AFM图；（c）纳米点在不同激光功率照射下的温升曲线；（d）激光连续照射10 min内小鼠肿瘤部位的红外热成像图；（e）不同组小鼠的肿瘤体积变化[46]

Fig.9 (a) Schematic diagram of TPP-G-FF self-assembled into nanodots; (b) Particle size and AFM image of nanodots; (c) Temperature elevation curves of nanodots under different laser power irradiation; (d) Infrared thermal images of mouse tumor sites within 10 min of continuous laser irradiation; (e) Changes in tumor volume in different groups of mice[46]

图10 （a）各治疗组肿瘤引流淋巴结成熟DCs (CD11c+CD80+CD86+)的比例及小鼠脾细胞中CD3+CD45+、CD3+CD4+、CD3+CD8+T细胞百分比的代表性流式细胞术图；（b）小鼠肿瘤中HIF-1α和CD31阳性区域的代表性H&E和IF染色图[62]

Fig.10 (a) Representative flow cytometry images of the ratio of mature DCs (CD11c+CD80+CD86+) in tumor-draining lymph nodes and the percentage of CD3+CD45+, CD3+CD4+, and CD3+CD8+T cells in mouse spleen cells in each treatment group; (b) Representative H&E and IF staining images of HIF-1α and CD31 positive areas in mouse tumor[62]

图11 （a）通过加热熔融和淬火冷却的方法制造生物玻璃示意图；（b）原位XRD谱图和原位拉曼光谱作为温度的函数；（c）3D打印机的示意图和印刷玻璃结构的照片；（d）玻璃珠在堆肥土壤中的降解图片；（e）玻璃珠在小鼠皮肤的解剖照片[75]

Fig.11 (a) Schematic diagram of manufacturing bioglass through heating, melting, and quenching and cooling methods; (b) In situ XRD and in situ Raman spectra as a function of temperature; (c) Schematic diagram of 3D printer and photos of printed glass architecture; (d) Image of degradation of glass beads in composting soil; (e) Anatomical photos of glass beads on mouse skin[75]

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