Biomimetic Oxygen-Evolving Photobacteria Based on Amino Acid and Porphyrin Hierarchical Self-Organization

被引:32
作者
Liu, Kai [1 ,3 ]
Zhang, Han [1 ]
Xing, Ruirui [1 ]
Zou, Qianli [1 ]
Yan, Xuehai [1 ,2 ,3 ]
机构
[1] Chinese Acad Sci, State Key Lab Biochem Engn, Beijing 100190, Peoples R China
[2] Chinese Acad Sci, Ctr Mesosci, Inst Proc Engn, Beijing 100190, Peoples R China
[3] Univ Chinese Acad Sci, Beijing 100190, Peoples R China
基金
中国国家自然科学基金;
关键词
amino acids; porphyrins; self-organization; oxygen evolution; biomimetic photosynthesis; DRIVEN WATER OXIDATION; ARTIFICIAL PHOTOSYNTHESIS; PHOTOSYSTEM-II; FUNCTIONAL MATERIALS; SURFACE MODIFICATION; CRYSTAL-STRUCTURE; ELECTRON-TRANSFER; CHEMISTRY; NANOSTRUCTURES; EVOLUTION;
D O I
10.1021/acsnano.7b08215
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Biomimetic organization provides a promising strategy to develop functional materials and understand biological processes. However, how to mimic complex biological systems using simple biomolecular units remains a great challenge. Herein, we design and fabricate a biomimetic cyanobacteria model based on self-integration of small bioinspired molecules, including amphiphilic amino acid, 3,4-dihydroxyphenylalanine (DOPA), and metalloporphyrin and cobalt oxide nanoparticles (Co3O4 NPs), with the assistance of chemical conjugation and molecular self-assembly. The assembled amino acid fiber can be modified by DOPA to form covalently bound DOPA melanin containing hydroxyl and quinone species via Schiff base reaction. The adhering template can further tune the self-assembly of metalloporphyrin and Co3O4 NPs into J-aggregation and dispersive distribution, respectively, mainly via coordination binding. Metalloporphyrin molecules in the resulting hybrid fibers capture light; quinone species accept the excited electrons, and Co3O4 NPs catalyze water oxidation. Thus, the essential components of the photosystem-II protein complex in cyanobacteria are simplified and engineered into a simple framework, still retaining a similar photosynthetic mechanism. In addition, this architecture leads to efficient coupling of antenna, quinone-type reaction center, and photocatalyst, which increases the flux of light energy from antenna to reaction center for charge separation, resulting in enhanced oxygen evolution rate with excellent sustainability.
引用
收藏
页码:12840 / 12848
页数:9
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