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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
2018-11-01
Source PublicationACS CATALYSIS
ISSN2155-5435
Volume8Issue:11Pages:10732-10745
Abstract

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.

KeywordChlorosome Molecular Evolution Artificial Photosynthesis Supramolecular Assemblies Nadh Regeneration
DOI10.1021/acscatal.8b03105
Language英语
WOS KeywordBiocatalyzed Artificial Photosynthesis ; Redox Biocatalysis ; Light Irradiation ; Carbon-dioxide ; Porphyrin ; Efficient ; Photocatalysis ; Nicotinamide ; Conversion ; System
Funding ProjectNational Natural Science Foundation of China[21676276] ; National Natural Science Foundation of China[91534126] ; National Basic Research Program of China (973 Program)[2013CB733604]
WOS Research AreaChemistry
WOS SubjectChemistry, Physical
Funding OrganizationNational Natural Science Foundation of China ; National Basic Research Program of China (973 Program)
WOS IDWOS:000449723900087
PublisherAMER CHEMICAL SOC
Citation statistics
Document Type期刊论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/26549
Collection中国科学院过程工程研究所
Corresponding AuthorShi, Jinjun; Zhang, Songping
Affiliation1.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
Recommended Citation
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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