Vapor-Phase Fabrication and Condensed-Phase Application of a MOF-Node-Supported Iron Thiolate Photocatalyst for Nitrate Conversion to Ammonium

We describe a method for synthesizing a nitrate reduction catalyst within a metal–organic framework (MOF). The MOF NU-1000, a zirconium-based mesoporous material, is exposed by using atomic layer deposition (ALD) to a vaporous iron amidinate coordination complex and subsequently a dodecanethiol liga...

Full description

Saved in:
Bibliographic Details
Published in:ACS applied energy materials 2019-12, Vol.2 (12), p.8695-8700
Main Authors: Choi, Hyeju, Peters, Aaron W, Noh, Hyunho, Gallington, Leighanne C, Platero-Prats, Ana E, DeStefano, Matthew R, Rimoldi, Martino, Goswami, Subhadip, Chapman, Karena W, Farha, Omar K, Hupp, Joseph T
Format: Article
Language:English
Subjects:
ammonia synthesis
INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
metal chalcogenide-based catalyst
metal-organic framework
molecular layer deposition
nitrate photoreduction
Citations: Items that this one cites
Items that cite this one
Online Access:Get full text
Tags: Add Tag
No Tags, Be the first to tag this record!
Description
Summary:We describe a method for synthesizing a nitrate reduction catalyst within a metal–organic framework (MOF). The MOF NU-1000, a zirconium-based mesoporous material, is exposed by using atomic layer deposition (ALD) to a vaporous iron amidinate coordination complex and subsequently a dodecanethiol ligand to synthesize an iron thiolate cluster grafted on the zirconium oxide nodes. Structural identification of the cluster is conducted through X-ray absorption spectroscopy (XAS) and differential envelope density (DED) analyses. Once submerged in an aqueous solution containing nitrate (30 ppm of N) and irradiated with light, the MOF/iron thiolate cluster assembly can photochemically transform the nitrate to ammonium ions. We suggest that sequential, self-limiting, atomic (metal ion), and molecular (ligand) deposition onto the reactive nodes of chemically and thermally stable MOFs could prove to be a versatile and attractive method for obtaining nature-inspired chemical catalysts.
ISSN:2574-0962
2574-0962
DOI:10.1021/acsaem.9b01664