CAS OpenIR  > 生化工程国家重点实验室
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

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.

WOS HeadingsScience & Technology ; Physical Sciences ; Technology
Indexed BySCI
WOS KeywordNicotinamide Adenine-dinucleotide ; Visible-light ; Carbon-dioxide ; Solar-energy ; Photothermal Therapy ; System ; Regeneration ; Methanol ; Photocatalyst ; Conversion
WOS Research AreaChemistry ; Energy & Fuels ; Materials Science
WOS SubjectChemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary
Funding OrganizationNational 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 IDWOS:000397605300031
Citation statistics
Cited Times:22[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
AffiliationChinese Acad Sci, Inst Proc Engn, State Key Lab Biochem Engn, Beijing 100190, Peoples R China
Recommended Citation
GB/T 7714
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.
Files in This Item:
File Name/Size DocType Version Access License
Integration of funct(1298KB)期刊论文出版稿限制开放CC BY-NC-SAApplication Full Text
Related Services
Recommend this item
Usage statistics
Export to Endnote
Google Scholar
Similar articles in Google Scholar
[Ji, Xiaoyuan]'s Articles
[Liu, Cuicui]'s Articles
[Wang, Jie]'s Articles
Baidu academic
Similar articles in Baidu academic
[Ji, Xiaoyuan]'s Articles
[Liu, Cuicui]'s Articles
[Wang, Jie]'s Articles
Bing Scholar
Similar articles in Bing Scholar
[Ji, Xiaoyuan]'s Articles
[Liu, Cuicui]'s Articles
[Wang, Jie]'s Articles
Terms of Use
No data!
Social Bookmark/Share
All comments (0)
No comment.

Items in the repository are protected by copyright, with all rights reserved, unless otherwise indicated.