Derivation and Decoration of Nets with Trigonal-Prismatic Nodes: A Unique Route to Reticular Synthesis of Metal–Organic Frameworks
Abstract
Quests for advanced functionalities in metal–organic frameworks (MOFs) inevitably encounter increasing complexity in their tailored framework architectures, accompanied by heightened challenges with their geometric design. Herein, we demonstrate the feasibility of rationally exploiting topological prediction as a blueprint for predesigned MOFs. A new triangular frusta secondary building unit (SBU), {Zn4(tz)3}, was bridged by three TDC2– fragments to initially form a trigonal prismatic node, {Zn8(tz)6(TDC)3} (Htz = 1H-1,2,3-triazole and H2TDC = 2,5-thiophenedicarboxylic acid). Furthermore, the trigonal prism unit can be considered as a double SBU derived from triply bound triangular frusta. By considering theoretical derived nets for linking this trigonal-prismatic node with ditopic, tritopic, and tetratopic linkers, we have synthesized and characterized a new family of MOFs that adopt the decorated lon, jea, and xai nets, respectively. Pore sizes have also been successively increased within TPMOF-n family, which facilitates heterogeneous biomimetic catalysis with Fe–porphyrin-based TPMOF-7 as a catalyst.
- Authors:
-
- Texas A & M Univ., College Station, TX (United States); Northeast Normal Univ., Changchun (People's Republic of China)
- Northeast Normal Univ., Changchun (People's Republic of China)
- Shantou Univ., Guangdong (People's Republic of China)
- Texas A & M Univ., College Station, TX (United States)
- Nanjing Normal Univ. (People's Republic of China)
- Nanjing Normal Univ. (People's Republic of China); Northeast Normal Univ., Changchun (People's Republic of China)
- 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); National Natural Science Foundation of China (NSFC); China Postdoctoral Science Foundation; Priority Academic Program Development of Jiangsu Higher Education Institutions; Foundation of Jiangsu Collaborative Innovation Center of Biomedical Functional Materials; Science and Technology Development Planning of Jilin Province
- OSTI Identifier:
- 1387707
- Grant/Contract Number:
- SC0001015
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 138; Journal Issue: 16; 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); ligands; metal organic frameworks; mixtures; chemical structure; mathematical methods
Citation Formats
Qin, Jun-Sheng, Du, Dong-Ying, Li, Mian, Lian, Xi-Zhen, Dong, Long-Zhang, Bosch, Mathieu, Su, Zhong-Min, Zhang, Qiang, Li, Shun-Li, Lan, Ya-Qian, Yuan, Shuai, and Zhou, Hong-Cai. Derivation and Decoration of Nets with Trigonal-Prismatic Nodes: A Unique Route to Reticular Synthesis of Metal–Organic Frameworks. United States: N. p., 2016.
Web. doi:10.1021/jacs.6b01093.
Qin, Jun-Sheng, Du, Dong-Ying, Li, Mian, Lian, Xi-Zhen, Dong, Long-Zhang, Bosch, Mathieu, Su, Zhong-Min, Zhang, Qiang, Li, Shun-Li, Lan, Ya-Qian, Yuan, Shuai, & Zhou, Hong-Cai. Derivation and Decoration of Nets with Trigonal-Prismatic Nodes: A Unique Route to Reticular Synthesis of Metal–Organic Frameworks. United States. https://doi.org/10.1021/jacs.6b01093
Qin, Jun-Sheng, Du, Dong-Ying, Li, Mian, Lian, Xi-Zhen, Dong, Long-Zhang, Bosch, Mathieu, Su, Zhong-Min, Zhang, Qiang, Li, Shun-Li, Lan, Ya-Qian, Yuan, Shuai, and Zhou, Hong-Cai. Tue .
"Derivation and Decoration of Nets with Trigonal-Prismatic Nodes: A Unique Route to Reticular Synthesis of Metal–Organic Frameworks". United States. https://doi.org/10.1021/jacs.6b01093. https://www.osti.gov/servlets/purl/1387707.
@article{osti_1387707,
title = {Derivation and Decoration of Nets with Trigonal-Prismatic Nodes: A Unique Route to Reticular Synthesis of Metal–Organic Frameworks},
author = {Qin, Jun-Sheng and Du, Dong-Ying and Li, Mian and Lian, Xi-Zhen and Dong, Long-Zhang and Bosch, Mathieu and Su, Zhong-Min and Zhang, Qiang and Li, Shun-Li and Lan, Ya-Qian and Yuan, Shuai and Zhou, Hong-Cai},
abstractNote = {Quests for advanced functionalities in metal–organic frameworks (MOFs) inevitably encounter increasing complexity in their tailored framework architectures, accompanied by heightened challenges with their geometric design. Herein, we demonstrate the feasibility of rationally exploiting topological prediction as a blueprint for predesigned MOFs. A new triangular frusta secondary building unit (SBU), {Zn4(tz)3}, was bridged by three TDC2– fragments to initially form a trigonal prismatic node, {Zn8(tz)6(TDC)3} (Htz = 1H-1,2,3-triazole and H2TDC = 2,5-thiophenedicarboxylic acid). Furthermore, the trigonal prism unit can be considered as a double SBU derived from triply bound triangular frusta. By considering theoretical derived nets for linking this trigonal-prismatic node with ditopic, tritopic, and tetratopic linkers, we have synthesized and characterized a new family of MOFs that adopt the decorated lon, jea, and xai nets, respectively. Pore sizes have also been successively increased within TPMOF-n family, which facilitates heterogeneous biomimetic catalysis with Fe–porphyrin-based TPMOF-7 as a catalyst.},
doi = {10.1021/jacs.6b01093},
journal = {Journal of the American Chemical Society},
number = 16,
volume = 138,
place = {United States},
year = {Tue Apr 05 00:00:00 EDT 2016},
month = {Tue Apr 05 00:00:00 EDT 2016}
}
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Figure 1: (a) Deconstruction of TMOF into the diamond (dia) net and (b) TPMOF-1 into the lonsdaleite (lon) net. The fragments outlined in blue and red show the distinct local conformations between the two basic nets. (c) Two {Zn5(tz)6} units linked by one TDC2– fragment in TMOF, which can bemore »
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