Thermodynamically Guided Synthesis of Mixed-Linker Zr-MOFs with Enhanced Tunability
Abstract
Guided by thermodynamics, we have synthesized two mixed-linker zirconium-based metal–organic frameworks (Zr-MOFs), namely, PCN-133 and PCN-134. Both of them possess a layer-pillar structure, in which the connection between Zr6 clusters and primary BTB linkers form a (3,6)-connected kdg layer that is further extended into 3D frameworks by auxiliary DCDPS/TCPP linkers (BTB = benzene tribenzoate, DCDPS = 4,4'-dicarboxydiphenyl sulfone, TCPP = tetrakis(4-carboxyphenyl)porphyrin). PCN-134 demonstrates high porosity (N2 uptake of 717 cm3·g–1 and BET surface area of 1946 cm2·g–1) and excellent chemical stability in aqueous solutions with pH values ranging from 0 to 13. More importantly, PCN-134 tolerates the partial absence of auxiliary linkers leading to structural defects during the assembly process while preserving its framework integrity. Furthermore, the defect density can be systematically controlled by tuning the occupancy of the auxiliary linker, which in turn affects the MOF properties. For instance, the dichromate uptake of PCN-134 is tuned by adjusting the BTB/TCPP ratios, which gives rise to an efficient dichromate absorbent when the TCPP molar ratio in linkers is set as 22%. Additionally, the photocatalytic reduction of Cr(VI) in aqueous solution was also performed by PCN-134–22%TCPP which exhibits excellent catalytic activity. This work not only opens up a new synthetic routemore »
- Authors:
-
- Texas A & M Univ., College Station, TX (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Gas Separations Relevant to Clean Energy Technologies (CGS)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); ConocoPhillips
- OSTI Identifier:
- 1470340
- Grant/Contract Number:
- SC0001015; EE0007049
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 138; Journal Issue: 20; Related Information: CGS partners with University of California, Berkeley; University of California, Davis; Lawrence Berkeley National Laboratory; University of Minnesota; National Energy Technology Laboratory; Texas A&M University; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; membrane; carbon capture; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing); layers; metal organic frameworks; defects; cluster chemistry; stability
Citation Formats
Yuan, Shuai, Qin, Jun-Sheng, Zou, Lanfang, Chen, Ying-Pin, Wang, Xuan, Zhang, Qiang, and Zhou, Hong-Cai. Thermodynamically Guided Synthesis of Mixed-Linker Zr-MOFs with Enhanced Tunability. United States: N. p., 2016.
Web. doi:10.1021/jacs.6b03263.
Yuan, Shuai, Qin, Jun-Sheng, Zou, Lanfang, Chen, Ying-Pin, Wang, Xuan, Zhang, Qiang, & Zhou, Hong-Cai. Thermodynamically Guided Synthesis of Mixed-Linker Zr-MOFs with Enhanced Tunability. United States. https://doi.org/10.1021/jacs.6b03263
Yuan, Shuai, Qin, Jun-Sheng, Zou, Lanfang, Chen, Ying-Pin, Wang, Xuan, Zhang, Qiang, and Zhou, Hong-Cai. Fri .
"Thermodynamically Guided Synthesis of Mixed-Linker Zr-MOFs with Enhanced Tunability". United States. https://doi.org/10.1021/jacs.6b03263. https://www.osti.gov/servlets/purl/1470340.
@article{osti_1470340,
title = {Thermodynamically Guided Synthesis of Mixed-Linker Zr-MOFs with Enhanced Tunability},
author = {Yuan, Shuai and Qin, Jun-Sheng and Zou, Lanfang and Chen, Ying-Pin and Wang, Xuan and Zhang, Qiang and Zhou, Hong-Cai},
abstractNote = {Guided by thermodynamics, we have synthesized two mixed-linker zirconium-based metal–organic frameworks (Zr-MOFs), namely, PCN-133 and PCN-134. Both of them possess a layer-pillar structure, in which the connection between Zr6 clusters and primary BTB linkers form a (3,6)-connected kdg layer that is further extended into 3D frameworks by auxiliary DCDPS/TCPP linkers (BTB = benzene tribenzoate, DCDPS = 4,4'-dicarboxydiphenyl sulfone, TCPP = tetrakis(4-carboxyphenyl)porphyrin). PCN-134 demonstrates high porosity (N2 uptake of 717 cm3·g–1 and BET surface area of 1946 cm2·g–1) and excellent chemical stability in aqueous solutions with pH values ranging from 0 to 13. More importantly, PCN-134 tolerates the partial absence of auxiliary linkers leading to structural defects during the assembly process while preserving its framework integrity. Furthermore, the defect density can be systematically controlled by tuning the occupancy of the auxiliary linker, which in turn affects the MOF properties. For instance, the dichromate uptake of PCN-134 is tuned by adjusting the BTB/TCPP ratios, which gives rise to an efficient dichromate absorbent when the TCPP molar ratio in linkers is set as 22%. Additionally, the photocatalytic reduction of Cr(VI) in aqueous solution was also performed by PCN-134–22%TCPP which exhibits excellent catalytic activity. This work not only opens up a new synthetic route toward mixed-linker MOFs, but also provides tunable control of MOF defects and, in turn, the properties.},
doi = {10.1021/jacs.6b03263},
journal = {Journal of the American Chemical Society},
number = 20,
volume = 138,
place = {United States},
year = {Fri May 06 00:00:00 EDT 2016},
month = {Fri May 06 00:00:00 EDT 2016}
}
Web of Science
Figures / Tables:
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Photosensitizer‐Anchored 2D MOF Nanosheets as Highly Stable and Accessible Catalysts toward Artemisinin Production
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