兰州大学机构库 >化学化工学院
A porous rhodium(III)-porphyrin metal-organic framework as an efficient and selective photocatalyst for CO2 reduction
Liu, Jiewei1; Fan, Yan-Zhong1; Li, Xin1; Wei, Zhangwen1; Xu, Yao-Wei1; Zhang, Li1; Su, Cheng-Yong1,2
Indexed BySCIE
2018-09-05
Source PublicationAPPLIED CATALYSIS B-ENVIRONMENTAL
ISSN0926-3373
Volume231Pages:173-181
AbstractA rhodium(III)-porphyrin zirconium metal-organic framework (Rh-PMOF-1(Zr)) has been prepared from the self-assembly of a Rh-based metalloporphyrin tetracarboxylic ligand Rh(TCPP)CI (TCPP = tetrakis(4-carboxyphenyl)porphyrin) with ZrCl4. The framework of Rh-PMOF-1 is stable up to 270 degrees C as disclosed by the variable-temperature powder X-ray diffraction (VT-PXRD) measurements, and possesses good chemical stability over a wide range of solvents including water. The single-crystal structural analysis reveals that Rh-PMOF-1 contains 3D channels (1.9 x 1.9 nm(2)), and the Rh-porphyrin units are exposed to the cavities. The calculation based on the N-2 adsorption at 77 K shows Rh-PMOF-1(Zr) has a high BET surface area (3015 m(2)g(-1)). The luminescence decay of Rh-PMOF-1 is well fitted to a tri-exponential curve featuring a long average lifetime of 207 mu s at 298 K under vacuum, which represents a rare example of room-temperature phosphorescence of Rh-porphyrin complexes. Under 1 atm, it displays CO2 uptake up to 42, 53 and 98 cm(3)g(-1) at 308, 298 and 273 K, respectively. Catalytic results show that, under the visible light (>= 400 nm) irradiation without any additional photosensitizer, Rh-PMOF-1 is powerful to catalyze CO2 reduction to the formate ion with up to 99% selectivity, and can be recycled and reused for 3 runs. Theoretical study was further carried out to reveal the energy levels of the frontier orbitals of Rh-PMOF-1 and the preferred binding sites of CO2 in the framework.
KeywordRhodium(III)-porphyrin Metal-organic frameworks Photocatalysls CO2 Reduction Room-temperature phosphorescence
DOI10.1016/j.apcatb.2018.02.055
First Inst
Language英语
Project NumberNSFC Projects [21773314, 21573291, 21720102007] ; STP Project of Guangzhou [201707010168] ; Fundamental Research Funds for the Central Universities
Funding Project国家自然科学基金项目
Funding OrganizationNSFC
WOS Research AreaChemistry ; Engineering
WOS SubjectChemistry, Physical ; Engineering, Environmental ; Engineering, Chemical
WOS IDWOS:000430762300018
PublisherELSEVIER
Original Document TypeArticle
Citation statistics
Cited Times:41[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.lzu.edu.cn/handle/262010/196849
Collection化学化工学院
Corresponding AuthorZhang, Li; Su, Cheng-Yong
Affiliation1.Sun Yat Sen Univ, Sch Chem, Lehn Inst Funct Mat, MOE Lab Bloinorgan & Synthet Chem, Guangzhou 510275, Guangdong, Peoples R China
2.Lanzhou Univ, State Key Lab Appl Organ Chem, Lanzhou 730000, Gansu, Peoples R China
First Author AffilicationSchool of Physical Sicence and Technology
Corresponding Author AffilicationSchool of Physical Sicence and Technology;  College of Chemistry and Chemical Engineering
Recommended Citation
GB/T 7714
Liu, Jiewei,Fan, Yan-Zhong,Li, Xin,et al. A porous rhodium(III)-porphyrin metal-organic framework as an efficient and selective photocatalyst for CO2 reduction[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2018,231:173-181.
APA Liu, Jiewei.,Fan, Yan-Zhong.,Li, Xin.,Wei, Zhangwen.,Xu, Yao-Wei.,...&Su, Cheng-Yong.(2018).A porous rhodium(III)-porphyrin metal-organic framework as an efficient and selective photocatalyst for CO2 reduction.APPLIED CATALYSIS B-ENVIRONMENTAL,231,173-181.
MLA Liu, Jiewei,et al."A porous rhodium(III)-porphyrin metal-organic framework as an efficient and selective photocatalyst for CO2 reduction".APPLIED CATALYSIS B-ENVIRONMENTAL 231(2018):173-181.
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