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Title: Rapid desolvation-triggered domino lattice rearrangement in a metal–organic framework

Abstract

Topological transitions between significantly different phases typically require extreme conditions to collectively break chemical bonds and overcome the stress caused to the original structure by altering its correlated bond environment. In this work, we present a case system that can achieve rapid rearrangement of the whole lattice of a metal–organic framework (MOF) through a ‘domino’ alteration of the bond connectivity under mild conditions. The system transforms from a disordered amorphous MOF with low porosity to a highly porous and crystalline isomer within 40 seconds upon activation (solvent exchange and desorption), resulting in a significant increase in surface area, from 725 to 2,749 m2/g–1. Spectroscopic measurements show that this counter-intuitive lattice rearrangement involves a metastable intermediate that results from solvent removal on coordinatively unsaturated metal sites. In conclusion, this amorphous–crystalline switch between two topological distinct MOFs is shown to be reversible over four cycles through activation and re-immersion in polar solvents.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3]; ORCiD logo [4];  [2];  [2];  [5];  [6];  [2];  [7];  [6];  [8]; ORCiD logo [9]; ORCiD logo [10]; ORCiD logo [11]; ORCiD logo [8];  [8];  [4]; ORCiD logo [2]
  1. National Tsing Hua University, Hsinchu (Taiwan); Academia Sinica, Taipei Taiwan)
  2. Texas A & M Univ., College Station, TX (United States)
  3. Univ. of Texas at Dallas, Richardson, TX (United States)
  4. Stockholm Univ. (Sweden)
  5. National Tsing Hua University, Hsinchu (Taiwan)
  6. Chung Yuan Christian University, Taoyuan City (Taiwan)
  7. Columbia Univ., New York, NY (United States)
  8. Academia Sinica, Taipei (Taiwan)
  9. Chung Yuan Christian University, Taoyuan City (Taiwan); National Taiwan Normal University, Taipei (Taiwan)
  10. National Tsing Hua University, Hsinchu (Taiwan); Chung Yuan Christian University, Taoyuan City (Taiwan)
  11. Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Univ. of Texas at Dallas, Richardson, TX (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
OSTI Identifier:
1643793
Grant/Contract Number:  
SC0019902; FG02-08ER46491; SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Nature Chemistry
Additional Journal Information:
Journal Volume: 12; Journal Issue: 1; Journal ID: ISSN 1755-4330
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Coordination chemistry; Metal–organic frameworks

Citation Formats

Lo, Sheng-Han, Feng, Liang, Tan, Kui, Huang, Zhehao, Yuan, Shuai, Wang, Kun-Yu, Li, Bing-Han, Liu, Wan-Ling, Day, Gregory S., Tao, Songsheng, Yang, Chun-Chuen, Luo, Tzuoo-Tsair, Lin, Chia-Her, Wang, Sue-Lein, Billinge, Simon J. L., Lu, Kuang-Lieh, Chabal, Yves J., Zou, Xiaodong, and Zhou, Hong-Cai. Rapid desolvation-triggered domino lattice rearrangement in a metal–organic framework. United States: N. p., 2019. Web. doi:10.1038/s41557-019-0364-0.
Lo, Sheng-Han, Feng, Liang, Tan, Kui, Huang, Zhehao, Yuan, Shuai, Wang, Kun-Yu, Li, Bing-Han, Liu, Wan-Ling, Day, Gregory S., Tao, Songsheng, Yang, Chun-Chuen, Luo, Tzuoo-Tsair, Lin, Chia-Her, Wang, Sue-Lein, Billinge, Simon J. L., Lu, Kuang-Lieh, Chabal, Yves J., Zou, Xiaodong, & Zhou, Hong-Cai. Rapid desolvation-triggered domino lattice rearrangement in a metal–organic framework. United States. https://doi.org/10.1038/s41557-019-0364-0
Lo, Sheng-Han, Feng, Liang, Tan, Kui, Huang, Zhehao, Yuan, Shuai, Wang, Kun-Yu, Li, Bing-Han, Liu, Wan-Ling, Day, Gregory S., Tao, Songsheng, Yang, Chun-Chuen, Luo, Tzuoo-Tsair, Lin, Chia-Her, Wang, Sue-Lein, Billinge, Simon J. L., Lu, Kuang-Lieh, Chabal, Yves J., Zou, Xiaodong, and Zhou, Hong-Cai. Mon . "Rapid desolvation-triggered domino lattice rearrangement in a metal–organic framework". United States. https://doi.org/10.1038/s41557-019-0364-0. https://www.osti.gov/servlets/purl/1643793.
@article{osti_1643793,
title = {Rapid desolvation-triggered domino lattice rearrangement in a metal–organic framework},
author = {Lo, Sheng-Han and Feng, Liang and Tan, Kui and Huang, Zhehao and Yuan, Shuai and Wang, Kun-Yu and Li, Bing-Han and Liu, Wan-Ling and Day, Gregory S. and Tao, Songsheng and Yang, Chun-Chuen and Luo, Tzuoo-Tsair and Lin, Chia-Her and Wang, Sue-Lein and Billinge, Simon J. L. and Lu, Kuang-Lieh and Chabal, Yves J. and Zou, Xiaodong and Zhou, Hong-Cai},
abstractNote = {Topological transitions between significantly different phases typically require extreme conditions to collectively break chemical bonds and overcome the stress caused to the original structure by altering its correlated bond environment. In this work, we present a case system that can achieve rapid rearrangement of the whole lattice of a metal–organic framework (MOF) through a ‘domino’ alteration of the bond connectivity under mild conditions. The system transforms from a disordered amorphous MOF with low porosity to a highly porous and crystalline isomer within 40 seconds upon activation (solvent exchange and desorption), resulting in a significant increase in surface area, from 725 to 2,749 m2/g–1. Spectroscopic measurements show that this counter-intuitive lattice rearrangement involves a metastable intermediate that results from solvent removal on coordinatively unsaturated metal sites. In conclusion, this amorphous–crystalline switch between two topological distinct MOFs is shown to be reversible over four cycles through activation and re-immersion in polar solvents.},
doi = {10.1038/s41557-019-0364-0},
journal = {Nature Chemistry},
number = 1,
volume = 12,
place = {United States},
year = {Mon Dec 02 00:00:00 EST 2019},
month = {Mon Dec 02 00:00:00 EST 2019}
}

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