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Title: Topologically guided tuning of Zr-MOF pore structures for highly selective separation of C6 alkane isomers

Abstract

As an alternative technology to energy intensive distillations, adsorptive separation by porous solids offers lower energy cost and higher efficiency. Herein we report a topology-directed design and synthesis of a series of Zr-based metal-organic frameworks with optimized pore structure for efficient separation of C6 alkane isomers, a critical step in the petroleum refining process to produce gasoline with high octane rating. Zr 6O 4(OH) 4(bptc) 3 adsorbs a large amount of n-hexane but excluding branched isomers. The n-hexane uptake is ~70% higher than that of a benchmark adsorbent, zeolite-5A. A derivative structure, Zr 6O 4(OH) 8(H 2O) 4(abtc) 2, is capable of discriminating all three C6 isomers and yielding a high separation factor for 3-methylpentane over 2,3-dimethylbutane. This property is critical for producing gasoline with further improved quality. Multicomponent breakthrough experiments provide a quantitative measure of the capability of these materials for separation of C6 alkane isomers. A detailed structural analysis reveals the unique topology, connectivity and relationship of these compounds.

Authors:
 [1]; ORCiD logo [2];  [3]; ORCiD logo [4];  [5];  [6]; ORCiD logo [7];  [8];  [6];  [1];  [1]; ORCiD logo [9];  [6];  [10];  [3]; ORCiD logo [2];  [1]
  1. Rutgers Univ., Piscataway, NJ (United States). Department of Chemistry and Chemical Biology
  2. King Abdullah University of Science and Technology, Thuwal (Saudi Arabia). Advanced Membranes and Porous Materials Center, Physical Sciences and Engineering Division
  3. Peking University, Beijing (China). College of Chemistry and Molecular Engineering
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  5. Wake Forest University, Winston-Salem, NC (United States). Department of Physics
  6. Univ. of Texas-Dallas, Richardson, TX (United States). Department of Materials Science & Engineering
  7. Samara University (Russia). Samara Center for Theoretical Materials Science (SCTMS
  8. Rutgers Univ., Piscataway, NJ (United States). Department of Chemistry and Chemical Biology; South China University of Technology, Guangzhou (China). School of Chemistry and Chemical Engineering
  9. Samara University (Russia). Samara Center for Theoretical Materials Science (SCTMS; Università degli Studi di Milano, Milano (Italy). Dipartimento di Chimica
  10. Wake Forest University, Winston-Salem, NC (United States). Department of Physics; Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Department of Chemistry
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1436677
DOE Contract Number:
AC02-05CH11231; FG02-08ER46491
Resource Type:
Journal Article
Resource Relation:
Journal Name: Nature Communications; Journal Volume: 9; Journal Issue: 1
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Wang, Hao, Dong, Xinglong, Lin, Junzhong, Teat, Simon J., Jensen, Stephanie, Cure, Jeremy, Alexandrov, Eugeny V., Xia, Qibin, Tan, Kui, Wang, Qining, Olson, David H., Proserpio, Davide M., Chabal, Yves J., Thonhauser, Timo, Sun, Junliang, Han, Yu, and Li, Jing. Topologically guided tuning of Zr-MOF pore structures for highly selective separation of C6 alkane isomers. United States: N. p., 2018. Web. doi:10.1038/s41467-018-04152-5.
Wang, Hao, Dong, Xinglong, Lin, Junzhong, Teat, Simon J., Jensen, Stephanie, Cure, Jeremy, Alexandrov, Eugeny V., Xia, Qibin, Tan, Kui, Wang, Qining, Olson, David H., Proserpio, Davide M., Chabal, Yves J., Thonhauser, Timo, Sun, Junliang, Han, Yu, & Li, Jing. Topologically guided tuning of Zr-MOF pore structures for highly selective separation of C6 alkane isomers. United States. doi:10.1038/s41467-018-04152-5.
Wang, Hao, Dong, Xinglong, Lin, Junzhong, Teat, Simon J., Jensen, Stephanie, Cure, Jeremy, Alexandrov, Eugeny V., Xia, Qibin, Tan, Kui, Wang, Qining, Olson, David H., Proserpio, Davide M., Chabal, Yves J., Thonhauser, Timo, Sun, Junliang, Han, Yu, and Li, Jing. Tue . "Topologically guided tuning of Zr-MOF pore structures for highly selective separation of C6 alkane isomers". United States. doi:10.1038/s41467-018-04152-5. https://www.osti.gov/servlets/purl/1436677.
@article{osti_1436677,
title = {Topologically guided tuning of Zr-MOF pore structures for highly selective separation of C6 alkane isomers},
author = {Wang, Hao and Dong, Xinglong and Lin, Junzhong and Teat, Simon J. and Jensen, Stephanie and Cure, Jeremy and Alexandrov, Eugeny V. and Xia, Qibin and Tan, Kui and Wang, Qining and Olson, David H. and Proserpio, Davide M. and Chabal, Yves J. and Thonhauser, Timo and Sun, Junliang and Han, Yu and Li, Jing},
abstractNote = {As an alternative technology to energy intensive distillations, adsorptive separation by porous solids offers lower energy cost and higher efficiency. Herein we report a topology-directed design and synthesis of a series of Zr-based metal-organic frameworks with optimized pore structure for efficient separation of C6 alkane isomers, a critical step in the petroleum refining process to produce gasoline with high octane rating. Zr6O4(OH)4(bptc)3 adsorbs a large amount of n-hexane but excluding branched isomers. The n-hexane uptake is ~70% higher than that of a benchmark adsorbent, zeolite-5A. A derivative structure, Zr6O4(OH)8(H2O)4(abtc)2, is capable of discriminating all three C6 isomers and yielding a high separation factor for 3-methylpentane over 2,3-dimethylbutane. This property is critical for producing gasoline with further improved quality. Multicomponent breakthrough experiments provide a quantitative measure of the capability of these materials for separation of C6 alkane isomers. A detailed structural analysis reveals the unique topology, connectivity and relationship of these compounds.},
doi = {10.1038/s41467-018-04152-5},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {Tue May 01 00:00:00 EDT 2018},
month = {Tue May 01 00:00:00 EDT 2018}
}