Porphyrin/SiO2/Cp*Rh(bpy)Cl Hybrid Nanoparticles Mimicking Chloroplast with Enhanced Electronic Energy Transfer for Biocatalyzed Artificial Photosynthesis

doi:10.1002/adfm.201705083

CAS OpenIR > 生化工程国家重点实验室

	*Porphyrin/SiO2/CpRh(bpy)Cl Hybrid Nanoparticles Mimicking Chloroplast with Enhanced Electronic Energy Transfer for Biocatalyzed Artificial Photosynthesis**
	Ji, Xiaoyuan 1,2,3; Wang, Jie 1,4; Mei, Lin 5; Tao, Wei 3; Barrett, Austin 3; Su, Zhiguo 1; Wang, Shaomin 4; Ma, Guanghui 1; Shi, Jinjun 3; Zhang, Songping 1
	2018-02-28
发表期刊	ADVANCED FUNCTIONAL MATERIALS
ISSN	1616-301X
卷号	28 期号:9
摘要	A biocatalyzed artificial photosynthesis system (APS) based on porphyrin/SiO2/CpRh(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 (CpRh(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.
关键词	Artificial Photosynthesis Chloroplast Mimicks Intermolecular Electron Transfer Intramolecular Electron Transfer Sol-gel Reactions
文章类型	Article
WOS标题词	Science & Technology ; Physical Sciences ; Technology
DOI	10.1002/adfm.201705083
收录类别	SCI
语种	英语
关键词[WOS]	SOLAR-ENERGY ; MESOPOROUS ORGANOSILICA ; NATURAL PHOTOSYNTHESIS ; REDOX BIOCATALYSIS ; MOLECULAR WIRES ; CHARGE-TRANSFER ; CO2 ; PHOTOCATALYSIS ; SYSTEM ; INTEGRATION
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
WOS类目	Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter
项目资助者	National Natural Science Foundation of China(21676276 ; National Basic Research Program of China (973 Program)(2013CB733604) ; 91534126)
WOS记录号	WOS:000426154500009
引用统计
文献类型	期刊论文
条目标识符	http://ir.ipe.ac.cn/handle/122111/24003
专题	生化工程国家重点实验室
作者单位	1.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
推荐引用方式 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).