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Porphyrin/SiO2/Cp*Rh(bpy)Cl Hybrid Nanoparticles Mimicking Chloroplast with Enhanced Electronic Energy Transfer for Biocatalyzed Artificial Photosynthesis
Ji, Xiaoyuan1,2,3; Wang, Jie1,4; Mei, Lin5; Tao, Wei3; Barrett, Austin3; Su, Zhiguo1; Wang, Shaomin4; Ma, Guanghui1; Shi, Jinjun3; Zhang, Songping1
2018-02-28
Source PublicationADVANCED FUNCTIONAL MATERIALS
ISSN1616-301X
Volume28Issue:9
Abstract

A biocatalyzed artificial photosynthesis system (APS) based on porphyrin/SiO2/Cp*Rh(bpy)Cl hybrid nanoparticles (TCPP/SiO2/Rh HNPs) to mimic chloroplasts in green plant is reported. The TCPP/SiO2/Rh HNPs are fabricated via sol-gel reaction of silica precursors functionalized with photosensitizer (porphyrin, TCPP) and electron mediator (Cp*Rh(bpy)Cl, M); while the integration of enzyme and coenzyme nicotinamide adenine dinucleotide (NAD)(H), on the outer surface of the HNPs is achieved through electro-static-interaction-driven assembling under the entanglement of a negatively charged polyelectrolyte. The chloroplast-mimicking, highly integrated APS exhibits remarkably superior performance over a free system such that the regeneration of NADH is improved from 11% to 75%, and the synthesis of formic acid from CO2 increased from 15 to 100 mu mol. Based on the detailed investigations into the photochemical and electrochemical properties, it is speculated that the covalent linking of the photosensitizer and electron mediator via silicon hydride bonds, and the formed SiO2 network through sol-gel reaction, may form intramolecular and intermolecular electron transfer chains to direct more efficient electron transfer from TCPP to M. Such intramolecular and intermolecular electrons and energy transfer, cooperated with the integrated biocatalytic process, lead to the significantly enhanced overall reaction efficiency. Moreover, the integrated APS also allows facile recycling of expensive M, enzymes, and cofactors.

KeywordArtificial Photosynthesis Chloroplast Mimicks Intermolecular Electron Transfer Intramolecular Electron Transfer Sol-gel Reactions
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences ; Technology
DOI10.1002/adfm.201705083
Indexed BySCI
Language英语
WOS KeywordSolar-energy ; Mesoporous Organosilica ; Natural Photosynthesis ; Redox Biocatalysis ; Molecular Wires ; Charge-transfer ; Co2 ; Photocatalysis ; System ; Integration
WOS Research AreaChemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
WOS SubjectChemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter
Funding OrganizationNational Natural Science Foundation of China(21676276 ; National Basic Research Program of China (973 Program)(2013CB733604) ; 91534126)
WOS IDWOS:000426154500009
Citation statistics
Cited Times:11[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/24003
Collection生化工程国家重点实验室
Affiliation1.Chinese Acad Sci, Inst Proc Engn, State Key Lab Biochem Engn, Beijing 100190, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, 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
5.Sun Yat Sen Univ, Sch Pharmaceut Sci Shenzhen, Guangzhou 510275, Guangdong, Peoples R China
Recommended Citation
GB/T 7714
Ji, Xiaoyuan,Wang, Jie,Mei, Lin,et al. Porphyrin/SiO2/Cp*Rh(bpy)Cl Hybrid Nanoparticles Mimicking Chloroplast with Enhanced Electronic Energy Transfer for Biocatalyzed Artificial Photosynthesis[J]. ADVANCED FUNCTIONAL MATERIALS,2018,28(9).
APA Ji, Xiaoyuan.,Wang, Jie.,Mei, Lin.,Tao, Wei.,Barrett, Austin.,...&Zhang, Songping.(2018).Porphyrin/SiO2/Cp*Rh(bpy)Cl Hybrid Nanoparticles Mimicking Chloroplast with Enhanced Electronic Energy Transfer for Biocatalyzed Artificial Photosynthesis.ADVANCED FUNCTIONAL MATERIALS,28(9).
MLA Ji, Xiaoyuan,et al."Porphyrin/SiO2/Cp*Rh(bpy)Cl Hybrid Nanoparticles Mimicking Chloroplast with Enhanced Electronic Energy Transfer for Biocatalyzed Artificial Photosynthesis".ADVANCED FUNCTIONAL MATERIALS 28.9(2018).
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