Enhanced Solar Energy Harvest and Electron Transfer through Intra- and Intermolecular Dual Channels in Chlorosome-Mimicking Supramolecular Self-Assemblies | |
Ji, Xiaoyuan1,2,3; Wang, Jie1,4; Kang, Yong1; Mei, Lin2; Su, Zhiguo1; Wang, Shaomin4; Ma, Guanghui1; Shi, Jinjun3; Zhang, Songping1 | |
刊名 | ACS CATALYSIS |
2018-11-01 | |
卷号 | 8期号:11页码:10732-10745 |
关键词 | Chlorosome Molecular Evolution Artificial Photosynthesis Supramolecular Assemblies Nadh Regeneration |
ISSN号 | 2155-5435 |
DOI | 10.1021/acscatal.8b03105 |
英文摘要 | The direct connection between a photosensitizer and an electron mediator, achieved by a precise arrangement based on chlorosome, provides photosynthetic bacteria the maximum efficiency in solar energy conversion. Herein, this study reports the fabrication of a biomimicking chlorosome for biocatalyzed artificial photosynthesis through self-assembly of simple molecules to functional systems. TCPP/EY(x)c/Rh8-x macromolecules, synthesized through a sequential amidation were found to self-assemble into chlorosome-mimicking reaction of porphyrin (TCPP), eosin Y (EY), and [Cp*RhCl2](2), supra molecular assemblies through noncovalent interactions. Intraand intermolecular dual channels for enhancing electron transfer were constructed in TCPP/EYx/Rh8-x supramolecular assemblies. In addition, the energy band structure of TCPP/EY4/Rh-4 supramolecular assemblies also made a perfect coordination with oxidation and reduction potentials of an electron donor and NAD+, which led to a fast and oriented electron transfer along the electron donor, TCPP/EY4/Rh-4 and NAD(+). In comparison with a system using free components, the yield of NADH photoregeneration was improved from 15% to 91% by TCPP/EY4/Rh-4 supramolecular assemblies; when this NADH photoregeneration process was coupled with dehydrogenases, 38 mu M methanol was synthesized from CO, after 2 h of visible light irradiation, which was about 12-fold higher than that obtained using free components. The chlorosome-inspired TCPP/ EYx/Rh8-x supramolecular assemblies with intra- and intermolecular electron transfer dual channels represents a landmark for implementing highly effective solar energy conversion and selective methanol synthesis from CO2 in a green and sustainable manner. |
资助项目 | National Natural Science Foundation of China[21676276] ; National Natural Science Foundation of China[91534126] ; National Basic Research Program of China (973 Program)[2013CB733604] |
WOS关键词 | Biocatalyzed Artificial Photosynthesis ; Redox Biocatalysis ; Light Irradiation ; Carbon-dioxide ; Porphyrin ; Efficient ; Photocatalysis ; Nicotinamide ; Conversion ; System |
WOS研究方向 | Chemistry |
语种 | 英语 |
出版者 | AMER CHEMICAL SOC |
WOS记录号 | WOS:000449723900087 |
资助机构 | National Natural Science Foundation of China ; National Basic Research Program of China (973 Program) |
内容类型 | 期刊论文 |
源URL | [http://ir.ipe.ac.cn/handle/122111/26548] |
专题 | 中国科学院过程工程研究所 |
通讯作者 | Shi, Jinjun; Zhang, Songping |
作者单位 | 1.Chinese Acad Sci, Inst Proc Engn, State Key Lab Biochem Engn, Beijing 100190, Peoples R China 2.Sun Yat Sen Univ, Sch Pharmaceut Sci Shenzhen, Guangzhou 510275, Guangdong, Peoples R China 3.Harvard Med Sch, Brigham & Womens Hosp, Ctr Nanomed, Boston, MA 02115 USA 4.Zhengzhou Univ, Coll Chem & Mol Engn, Zhengzhou 450001, Henan, Peoples R China |
推荐引用方式 GB/T 7714 | Ji, Xiaoyuan,Wang, Jie,Kang, Yong,et al. Enhanced Solar Energy Harvest and Electron Transfer through Intra- and Intermolecular Dual Channels in Chlorosome-Mimicking Supramolecular Self-Assemblies[J]. ACS CATALYSIS,2018,8(11):10732-10745. |
APA | Ji, Xiaoyuan.,Wang, Jie.,Kang, Yong.,Mei, Lin.,Su, Zhiguo.,...&Zhang, Songping.(2018).Enhanced Solar Energy Harvest and Electron Transfer through Intra- and Intermolecular Dual Channels in Chlorosome-Mimicking Supramolecular Self-Assemblies.ACS CATALYSIS,8(11),10732-10745. |
MLA | Ji, Xiaoyuan,et al."Enhanced Solar Energy Harvest and Electron Transfer through Intra- and Intermolecular Dual Channels in Chlorosome-Mimicking Supramolecular Self-Assemblies".ACS CATALYSIS 8.11(2018):10732-10745. |
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