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

被引：36

作者：

Choi, Hyeju ^{[1
]}

Peters, Aaron W. ^{[1
]}

Noh, Hyunho ^{[1
]}

Gallington, Leighanne C. ^{[2
]}

Platero-Prats, Ana E. ^{[2
]}

DeStefano, Matthew R. ^{[1
]}

Rimoldi, Martino ^{[1
]}

Goswami, Subhadip ^{[1
]}

Chapman, Karena W. ^{[3
]}

Farha, Omar K. ^{[1
]}

Hupp, Joseph T. ^{[1
]}

机构：

[1] Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA

[2] Argonne Natl Lab, Adv Photon Source, Xray Sci Div, Argonne, IL 60439 USA

[3] SUNY Stony Brook, Dept Chem, 100 Nicolls Rd, Stony Brook, NY 11794 USA

来源：

ACS APPLIED ENERGY MATERIALS | 2019年 / 2卷 / 12期

基金：

美国国家科学基金会;

关键词：

nitrate photoreduction; metal-organic framework; ammonia synthesis; molecular layer deposition; metal chalcogenide-based catalyst; ATOMIC-LAYER-DEPOSITION; METAL-ORGANIC FRAMEWORK; HYDROGEN EVOLUTION; MOLYBDENUM SULFIDE; THIN-FILMS; REDUCTION; WATER; GROWTH;

D O I：

10.1021/acsaem.9b01664

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

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.

引用

页码：8695 / 8700

页数：11

共 33 条

[1] Fabrication of Thin Films of α-Fe2O3 via Atomic Layer Deposition Using Iron Bisamidinate and Water under Mild Growth Conditions
Avila, Jason R.
Kim, Dong Wook
Rimoldi, Martino
Farha, Omar K.
Hupp, Joseph T.
[J]. ACS APPLIED MATERIALS & INTERFACES, 2015, 7 (30) : 16138 - 16142
[2] Real-Time Observation of Atomic Layer Deposition Inhibition: Metal Oxide Growth on Self-Assembled Alkanethiols
Avila, Jason R.
DeMarco, Erica J.
Emery, Jonathan D.
Farha, Omar K.
Pellin, Michael J.
Hupp, Joseph T.
Martinson, Alex B. F.
[J]. ACS APPLIED MATERIALS & INTERFACES, 2014, 6 (15) : 11891 - 11898
[3] Molecular Layer Deposition for Surface Modification of Lithium-Ion Battery Electrodes
Ban, Chunmei
George, Steven M.
[J]. ADVANCED MATERIALS INTERFACES, 2016, 3 (21):
[4] The Postsynthetic Renaissance in Porous Solids
Cohen, Seth M.
[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2017, 139 (08) : 2855 - 2863
[5] Postsynthetic Methods for the Functionalization of Metal-Organic Frameworks
Cohen, Seth M.
[J]. CHEMICAL REVIEWS, 2012, 112 (02) : 970 - 1000
[6] The relationship between structure and function for the sulfite reductases
Crane, BR
Getzoff, ED
[J]. CURRENT OPINION IN STRUCTURAL BIOLOGY, 1996, 6 (06) : 744 - 756
[7] Photocatalytic nitrate reduction in water: Managing the hole scavenger and reaction by-product selectivity
Doudrick, K.
Yang, T.
Hristovski, K.
Westerhoff, P.
[J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 2013, 136 : 40 - 47
[8] Mechanism of the six-electron reduction of nitrite to ammonia by cytochrome c nitrite reductase
Einsle, O
Messerschmidt, A
Huber, R
Kroneck, PMH
Neese, F
[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2002, 124 (39) : 11737 - 11745
[9] How a century of ammonia synthesis changed the world
Erisman, Jan Willem
Sutton, Mark A.
Galloway, James
Klimont, Zbigniew
Winiwarter, Wilfried
[J]. NATURE GEOSCIENCE, 2008, 1 (10) : 636 - 639
[10] The chemical reduction of nitrate in aqueous solution
Fanning, JC
[J]. COORDINATION CHEMISTRY REVIEWS, 2000, 199 : 159 - 179

← 1 2 3 4 →