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Title: Versatile Surface Functionalization of Metal-Organic Frameworks through Direct Metal Coordination with a Phenolic Lipid Enables Diverse Applications

Journal Article · · Advanced Functional Materials
 [1];  [2];  [3];  [1];  [4];  [1];  [1];  [5]; ORCiD logo [6]
  1. Univ. of New Mexico, Albuquerque, NM (United States). Dept. of Chemical and Biological Engineering
  2. Univ. of Cambridge (United Kingdom). Melville Lab. for Polymer Synthesis, Dept. of Chemistry
  3. City Univ. of Hong Kong, Hong Kong (China). Joint Lab. for Energy and Environmental Catalysis School of Energy and Environment
  4. Monash Univ., Melbourne, VIC (Australia). Dept. of Mechanical and Aerospace Engineering
  5. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Advanced Materials Lab.
  6. Univ. of New Mexico, Albuquerque, NM (United States). Dept. of Chemical and Biological Engineering; Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Advanced Materials Lab.

Abstract A novel strategy for the versatile functionalization of the external surface of metal‐organic frameworks (MOFs) has been developed based on the direct coordination of a phenolic‐inspired lipid molecule DPGG (1,2‐dipalmitoyl‐sn‐glycero‐3‐galloyl) with metal nodes/sites surrounding MOF surface. X‐ray diffraction and Argon sorption analysis prove that the modified MOF particles retain their structural integrity and porosity after surface modification. Density functional theory calculations reveal that strong chelation strength between the metal sites and the galloyl head group of DPGG is the basic prerequisite for successful coating. Due to the pH‐responsive nature of metal‐phenol complexation, the modification process is reversible by simple washing in weak acidic water, showing an excellent regeneration ability for water‐stable MOFs. Moreover, the colloidal stability of the modified MOFs in the nonpolar solvent allows them to be further organized into 2 dimensional MOF or MOF/polymer monolayers by evaporation‐induced interfacial assembly conducted on an air/water interface. Finally, the easy fusion of a second functional layer onto DPGG‐modified MOF cores, enabled a series of MOF‐based functional nanoarchitectures, such as MOFs encapsulated within hybrid supported lipid bilayers (so‐called protocells ), polyhedral core‐shell structures, hybrid lipid‐modified‐plasmonic vesicles and multicomponent supraparticles with target functionalities, to be generated. for a wide range of applications.

Research Organization:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA)
Grant/Contract Number:
AC04-94AL85000
OSTI ID:
1464182
Alternate ID(s):
OSTI ID: 1422236
Report Number(s):
SAND-2017-12256J; 658659; TRN: US1902370
Journal Information:
Advanced Functional Materials, Vol. 28, Issue 16; ISSN 1616-301X
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 68 works
Citation information provided by
Web of Science

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The Chemistry of Reticular Framework Nanoparticles: MOF, ZIF, and COF Materials journal February 2020
ZD2-Engineered Gold Nanostar@Metal-Organic Framework Nanoprobes for T 1 -Weighted Magnetic Resonance Imaging and Photothermal Therapy Specifically Toward Triple-Negative Breast Cancer journal October 2018
Modular Metal–Organic Polyhedra Superassembly: From Molecular‐Level Design to Targeted Drug Delivery journal January 2019
SupraCells: Living Mammalian Cells Protected within Functional Modular Nanoparticle‐Based Exoskeletons journal April 2019
Phenolische Bausteine für die Assemblierung von Funktionsmaterialien journal December 2018
Phenolic Building Blocks for the Assembly of Functional Materials journal February 2019
Shape control of core–shell MOF@MOF and derived MOF nanocages via ion modulation in a one-pot strategy journal January 2018
DOX-assisted functionalization of green tea polyphenol nanoparticles for effective chemo-photothermal cancer therapy journal January 2019

Figures / Tables (9)