Abstract
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.
| Original language | English |
|---|---|
| Journal | ACS Applied Energy Materials |
| DOIs | |
| Publication status | Accepted/In press - Jan 1 2019 |
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Keywords
- ammonia synthesis
- metal chalcogenide-based catalyst
- metal-organic framework
- molecular layer deposition
- nitrate photoreduction
ASJC Scopus subject areas
- Chemical Engineering (miscellaneous)
- Energy Engineering and Power Technology
- Electrochemistry
- Materials Chemistry
- Electrical and Electronic Engineering
Cite this
Vapor-Phase Fabrication and Condensed-Phase Application of a MOF-Node-Supported Iron Thiolate Photocatalyst for Nitrate Conversion to Ammonium. / 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.
In: ACS Applied Energy Materials, 01.01.2019.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Vapor-Phase Fabrication and Condensed-Phase Application of a MOF-Node-Supported Iron Thiolate Photocatalyst for Nitrate Conversion to Ammonium
AU - Choi, Hyeju
AU - Peters, Aaron W.
AU - Noh, Hyunho
AU - Gallington, Leighanne C.
AU - Platero-Prats, Ana E.
AU - Destefano, Matthew R.
AU - Rimoldi, Martino
AU - Goswami, Subhadip
AU - Chapman, Karena W.
AU - Farha, Omar K.
AU - Hupp, Joseph T.
PY - 2019/1/1
Y1 - 2019/1/1
N2 - 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.
AB - 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.
KW - ammonia synthesis
KW - metal chalcogenide-based catalyst
KW - metal-organic framework
KW - molecular layer deposition
KW - nitrate photoreduction
UR - http://www.scopus.com/inward/record.url?scp=85076243398&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85076243398&partnerID=8YFLogxK
U2 - 10.1021/acsaem.9b01664
DO - 10.1021/acsaem.9b01664
M3 - Article
AN - SCOPUS:85076243398
JO - ACS Applied Energy Materials
JF - ACS Applied Energy Materials
SN - 2574-0962
ER -