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Title: Impact of linker engineering on the catalytic activity of metal–organic frameworks containing Pd(II)–bipyridine complexes

Abstract

A series of mixed-linker bipyridyl metal–organic framework (MOF)-supported palladium(II) catalysts were used to elucidate the electronic and steric effects of linker substitution on the activity of these catalysts in the context of Suzuki–Miyaura cross-coupling reactions. m-6,6'-Me 2bpy-MOF-PdCl 2 exhibited 110- and 496-fold enhancements in activity compared to nonfunctionalized m-bpy-MOF-PdCl 2 and m-4,4'-Me 2bpy-MOF-PdCl 2, respectively. Furthermore, this result clearly demonstrates that the stereoelectronic properties of metal-binding linker units are critical to the activity of single-site organometallic catalysts in MOFs and highlights the importance of linker engineering in the design and development of efficient MOF catalysts.

Authors:
 [1];  [2];  [1];  [1];  [2];  [2];  [1]
  1. Iowa State Univ., Ames, IA (United States); Ames Lab., Ames, IA (United States)
  2. Iowa State Univ., Ames, IA (United States)
Publication Date:
Research Org.:
Ames Lab., Ames, IA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1337683
Report Number(s):
IS-J-9087
Journal ID: ISSN 2155-5435
Grant/Contract Number:  
AC02-07CH11358
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 6; Journal Issue: 9; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; bipyridyl linker; heterogeneous catalysis; isoreticular metal−organic frameworks; single-site catalyst; structure−activity relationship; Suzuki−Miyaura cross-coupling

Citation Formats

Li, Xinle, Van Zeeland, Ryan, Maligal-Ganesh, Raghu V., Pei, Yuchen, Power, Gregory, Stanley, Levi, and Huang, Wenyu. Impact of linker engineering on the catalytic activity of metal–organic frameworks containing Pd(II)–bipyridine complexes. United States: N. p., 2016. Web. doi:10.1021/acscatal.6b01753.
Li, Xinle, Van Zeeland, Ryan, Maligal-Ganesh, Raghu V., Pei, Yuchen, Power, Gregory, Stanley, Levi, & Huang, Wenyu. Impact of linker engineering on the catalytic activity of metal–organic frameworks containing Pd(II)–bipyridine complexes. United States. doi:10.1021/acscatal.6b01753.
Li, Xinle, Van Zeeland, Ryan, Maligal-Ganesh, Raghu V., Pei, Yuchen, Power, Gregory, Stanley, Levi, and Huang, Wenyu. Tue . "Impact of linker engineering on the catalytic activity of metal–organic frameworks containing Pd(II)–bipyridine complexes". United States. doi:10.1021/acscatal.6b01753. https://www.osti.gov/servlets/purl/1337683.
@article{osti_1337683,
title = {Impact of linker engineering on the catalytic activity of metal–organic frameworks containing Pd(II)–bipyridine complexes},
author = {Li, Xinle and Van Zeeland, Ryan and Maligal-Ganesh, Raghu V. and Pei, Yuchen and Power, Gregory and Stanley, Levi and Huang, Wenyu},
abstractNote = {A series of mixed-linker bipyridyl metal–organic framework (MOF)-supported palladium(II) catalysts were used to elucidate the electronic and steric effects of linker substitution on the activity of these catalysts in the context of Suzuki–Miyaura cross-coupling reactions. m-6,6'-Me2bpy-MOF-PdCl2 exhibited 110- and 496-fold enhancements in activity compared to nonfunctionalized m-bpy-MOF-PdCl2 and m-4,4'-Me2bpy-MOF-PdCl2, respectively. Furthermore, this result clearly demonstrates that the stereoelectronic properties of metal-binding linker units are critical to the activity of single-site organometallic catalysts in MOFs and highlights the importance of linker engineering in the design and development of efficient MOF catalysts.},
doi = {10.1021/acscatal.6b01753},
journal = {ACS Catalysis},
number = 9,
volume = 6,
place = {United States},
year = {2016},
month = {8}
}

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Works referencing / citing this record:

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  • Calbo, Joaquín; Golomb, Matthias J.; Walsh, Aron
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journal, May 2017

  • Majeed, Maitham H.; Shayesteh, Payam; Wallenberg, L. Reine
  • Chemistry - A European Journal, Vol. 23, Issue 35
  • DOI: 10.1002/chem.201700777

Redox-active metal–organic frameworks for energy conversion and storage
journal, January 2019

  • Calbo, Joaquín; Golomb, Matthias J.; Walsh, Aron
  • Journal of Materials Chemistry A, Vol. 7, Issue 28
  • DOI: 10.1039/c9ta04680a