Thesis Advisor白硕
Degree Grantor中国科学院大学
Degree Discipline化学工程

太阳能高效利用是人们长期以来研究的热点课题之一,虽然取得了重要的研究成果,但依然存在着效率过低、成本过高等问题,制约着太阳能的高效利用。然而在自然界中,光合系统则能够持续高效地实现太阳能的转化和利用,这其中通过分子自组装形成的蛋白质/色素复合体是关键结构之一,此复合体不仅高效地完成光能捕获、电子和能量传递,且最终实现物质合成的功能。因此,通过仿生自然界光转换过程,构建类似于自然界光转换复合体是提高光转化效率、降低成本的有效途径之一。如何通过简单的生物分子结构设计和组装,以实现光能的高效利用是目前研究的热点和难点。在本课题中我们合理地设计与筛选了由几个氨基酸组成的短肽作为自组装基元,通过改变组装条件调控短肽的自组装行为,实现对自组装结构的精准设计和调控。在对短肽自组装规律的理解基础之上,进一步研究其调控卟啉等色素分子的有序组装能力,构筑了与天然捕光体系具有类似结构和功能的组装体。主要取得如下研究结果:(1)采用多孔CaCO3微粒作为模板,结合酶促缩合反应构建了多级组织的肽笼。其中多孔CaCO3微粒用作热蛋白酶(Thermolysin)的载体,并作为催化剂以实现Fmoc-Y和L-NH2在水/正己烷乳液的限域空间中发生缩合反应,并限定短肽Fmoc-YL-NH2的自组装行为,使其仅在CaCO3表面上自组装。在去除CaCO3模板后即可获得由纤维组成的肽笼,以期实现对多种功能性分子的有效负载(如卟啉类)。(2)利用卟啉作为掺杂剂制备了芳香短肽水凝胶,实现了有效的太阳能-电子能量转换。芳香短肽的长程有序组装不仅可以起到光电子受体和导体的作用,而且促进捕光天线卟啉分子产生光电子。同时,卟啉的掺杂可以有效地降低肽类水凝胶的阻抗,促进光电子的传输。光电流测试结果表明,卟啉掺杂的肽水凝胶具有良好的光响应性能。;Efficient use of solar energy is one of the hot topics that people have been studying for a long time. Although important research results have been achieved, there are still problems such as low efficiency and high cost, which restricts the efficient using of solar energy. However, the protein/pigment complex formed by molecular self-assembly in nature is the key light capture unit, which completes the light energy harvesting, electron and energy transfer and final material synthesis. Therefore, biomimicking the natural light conversion process is one of the effective ways to improve light conversion efficiency and reducing cost. How to realize the efficient utilization of light energy through simple molecular design and structure assembly has become a hot and challenging research topic at present. In this thesis, short peptides consisting of several amino acids were selected as the self-assembling building unit, and the self-assembly behavior of the peptides was regulated by changing the assembly conditions, so as to achieve the precise design and preparation of the self-assembly structure. Based on the understanding of the self-assembly rule of short peptides, the ordered assembly ability of porphyrin and other pigment molecules was further studied, and the assembly with similar structure and function as that of natural photosynthetic system was constructed. The main results of the study are as follows:(1) A short peptide cage with hierarchical organization was constructed by using porous CaCO3 microparticles as templates in combination with enzyme-catalyzed condensation reaction. The porous CaCO3 microparticles were used as the carrier of thermolysin, which could be used as catalyzers for the condensation of Fmoc-Y and L-NH2 in water/n-hexane emulsion to yield the short peptide Fmoc-YL-NH2 for self-assembly. The condensation of Fmoc-Y and L-NH2 in the confined space of water/n-hexane emulsion allow the resulting Fmoc-YL-NH2 for self-assembly only confined on the surface of CaCO3. The peptide cage composed of nanofibrils can finally be obtained by removing the CaCO3 template, which has great potential application in the encapsulation of active cargos (such as porphyrin).(2) Light-harvesting hybrid hydrogels were prepared by self-assembly of aromatic short peptides with porphyrin as a dopant, and effective solar energy conversion was achieved. The long-range ordered assembly of aromatic short peptides can act as photoelectron receptor and conductor and promote photoelectron generation from light-harvesting antenna (porphyrins). At the same time, the doping of porphyrin can effectively reduce the impedance of peptide hydrogels and promote photoelectron transfer. The results of photocurrent measurement show that the porphyrin-doped peptide hydrogels have good photo-response properties.

Document Type学位论文
Recommended Citation
GB/T 7714
冯璐. 短肽自组装水凝胶卟啉掺杂及光电性质研究[D]. 中国科学院大学,2019.
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短肽自组装水凝胶卟啉掺杂及光电性质研究.(4454KB)学位论文 限制开放CC BY-NC-SAApplication Full Text
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