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Integration of functionalized two-dimensional TaS2 nanosheets and an electron mediator for more efficient biocatalyzed artificial photosynthesis
Ji, Xiaoyuan; Liu, Cuicui; Wang, Jie; Su, Zhiguo; Ma, Guanghui; Zhang, Songping
2017
发表期刊JOURNAL OF MATERIALS CHEMISTRY A
ISSN2050-7488
卷号5期号:11页码:5511-5522
摘要A visible light active photocatalytic system based on two-dimensional (2D) TaS2 nanosheets with an integrated electron mediator (M) was developed for solar fuel production from CO2 in a biocatalyzed artificial photosynthesis system. The integration of M to TaS2 was realized through sequential functionalization by pegylation with lipoic acid conjugated PEG (LA-PEG), surface assembly of graphene (GR), and final integration of M. The photocatalytic activities of the resultant photocatalysts with different degrees of functionalization were evaluated by the photo-regeneration efficiency of NADH from NAD+ under visible light irradiation. Compared with non-functionalized TaS2 nanosheets that could only regenerate 39.7 +/- 1.9% of NAD+ to NADH in the presence of dispersed M, the wholly integrated photocatalyst termed as TaS2-PEG-GR-M exhibited significantly improved efficiency with a NADH regeneration yield up to 83.9 +/- 2.2%, which was higher than most of the reported values. This NADH photo-regeneration process was then coupled with formate dehydrogenase (FateDH) catalyzed synthesis of formic acid from CO2. By using TaS2-PEG-GR-M as a catalyst for NADH photoregeneration, the formic acid concentration reached 101.4 +/- 3.5 mM, which was about 2.5-fold higher than that obtained with the non-functionalized TaS2 nanosheets. Based on detailed investigations of the photochemical and electrochemical properties, the photo-induced electron transfer mechanism involved in the TaS2 nanosheets-based artificial photosynthesis system is discussed. The significantly enhanced reaction efficiency of the artificial photosynthesis system using the integrated TaS2-PEG-GRM as the photocatalyst was considered to be mainly benefited from the increased hydrophilicity, elimination of electron back-flow and recombination of photogenerated electrons and holes, as well as the shortened distance of electron transfer. The integrated TaS2-PEG-GR-M photocatalytic system also avoided contamination of M to the reaction system, and allowed reuse of the expensive M. The whole photocatalytic system retained 83% of its original activity after 10 cycles of reuse. The present research highlights the development of a new class of 2D transition metal dichalcogenide-based integrated photocatalysts for the efficient and direct formation of solar fuels and chemicals from CO2.
文章类型Article
WOS标题词Science & Technology ; Physical Sciences ; Technology
DOI10.1039/c7ta00002b
收录类别SCI
语种英语
关键词[WOS]NICOTINAMIDE ADENINE-DINUCLEOTIDE ; VISIBLE-LIGHT ; CARBON-DIOXIDE ; SOLAR-ENERGY ; PHOTOTHERMAL THERAPY ; SYSTEM ; REGENERATION ; METHANOL ; PHOTOCATALYST ; CONVERSION
WOS研究方向Chemistry ; Energy & Fuels ; Materials Science
WOS类目Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary
项目资助者National Natural Science Foundation of China(21676276 ; National Basic Research Program of China (973 Program)(2013CB733604) ; National Key Scientific Instrument and Equipment Development Project(2013YQ14040508) ; 21376249)
WOS记录号WOS:000397605300031
引用统计
被引频次:5[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.ipe.ac.cn/handle/122111/22103
专题生化工程国家重点实验室
作者单位Chinese Acad Sci, Inst Proc Engn, State Key Lab Biochem Engn, Beijing 100190, Peoples R China
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Ji, Xiaoyuan,Liu, Cuicui,Wang, Jie,et al. Integration of functionalized two-dimensional TaS2 nanosheets and an electron mediator for more efficient biocatalyzed artificial photosynthesis[J]. JOURNAL OF MATERIALS CHEMISTRY A,2017,5(11):5511-5522.
APA Ji, Xiaoyuan,Liu, Cuicui,Wang, Jie,Su, Zhiguo,Ma, Guanghui,&Zhang, Songping.(2017).Integration of functionalized two-dimensional TaS2 nanosheets and an electron mediator for more efficient biocatalyzed artificial photosynthesis.JOURNAL OF MATERIALS CHEMISTRY A,5(11),5511-5522.
MLA Ji, Xiaoyuan,et al."Integration of functionalized two-dimensional TaS2 nanosheets and an electron mediator for more efficient biocatalyzed artificial photosynthesis".JOURNAL OF MATERIALS CHEMISTRY A 5.11(2017):5511-5522.
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