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
收藏
页码：8695 / 8700
页数：11
相关论文
共 33 条
  • [11] Passivation of copper surfaces for selective-area ALD using a thiol self-assembled monolayer
    Farm, Elina
    Vehkamaki, Marko
    Ritala, Mikko
    Leskela, Markku
    [J]. SEMICONDUCTOR SCIENCE AND TECHNOLOGY, 2012, 27 (07)
  • [12] The Chemistry and Applications of Metal-Organic Frameworks
    Furukawa, Hiroyasu
    Cordova, Kyle E.
    O'Keeffe, Michael
    Yaghi, Omar M.
    [J]. SCIENCE, 2013, 341 (6149) : 974 - +
  • [13] Regioselective Atomic Layer Deposition in Metal-Organic Frameworks Directed by Dispersion Interactions
    Gallington, Leighanne C.
    Kim, In Soo
    Liu, Wei-Guang
    Yakovenko, Andrey A.
    Platero-Prats, Ana E.
    Li, Zhanyong
    Wang, Timothy C.
    Hupp, Joseph T.
    Farha, Omar K.
    Truhlar, Donald G.
    Martinson, Alex B. F.
    Chapman, Karena W.
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2016, 138 (41) : 13513 - 13516
  • [14] Titania-supported bimetallic catalysts for photocatalytic reduction of nitrate
    Gao, WL
    Jin, RC
    Chen, MX
    Guan, XX
    Zeng, HS
    Zhang, FX
    Guan, NJ
    [J]. CATALYSIS TODAY, 2004, 90 (3-4) : 331 - 336
  • [15] Reductive activation in periplasmic nitrate reductase involves chemical modifications of the Mo-cofactor beyond the first coordination sphere of the metal ion
    Jacques, Julien G. J.
    Fourmond, Vincent
    Arnoux, Pascal
    Sabaty, Monique
    Etienne, Emilien
    Grosse, Sandrine
    Biaso, Frederic
    Bertrand, Patrick
    Pignol, David
    Leger, Christophe
    Guigliarelli, Bruno
    Burlat, Benedicte
    [J]. BIOCHIMICA ET BIOPHYSICA ACTA-BIOENERGETICS, 2014, 1837 (02): : 277 - 286
  • [16] Targeted Single-Site MOF Node Modification: Trivalent Metal Loading via Atomic Layer Deposition
    Kim, In Soo
    Borycz, Joshua
    Platero-Prats, Ana E.
    Tussupbayev, Samat
    Wang, Timothy C.
    Farha, Omar K.
    Hupp, Joseph T.
    Gagliardi, Laura
    Chapman, Karena W.
    Cramer, Christopher J.
    Martinson, Alex B. F.
    [J]. CHEMISTRY OF MATERIALS, 2015, 27 (13) : 4772 - 4778
  • [17] Synthetic Access to Atomically Dispersed Metals in Metal-Organic Frameworks via a Combined Atomic-Layer-Deposition-in-MOF and Metal-Exchange Approach
    Klet, Rachel C.
    Wang, Timothy C.
    Fernandez, Laura E.
    Truhlar, Donald G.
    Hupp, Joseph T.
    Farha, Omar K.
    [J]. CHEMISTRY OF MATERIALS, 2016, 28 (04) : 1213 - 1219
  • [18] Selective photocatalytic reduction of nitrate to nitrogen molecules in an aqueous suspension of metal-loaded titanium(IV) oxide particles
    Kominami, H
    Nakaseko, T
    Shimada, Y
    Furusho, A
    Inoue, H
    Murakami, S
    Kera, Y
    Ohtani, B
    [J]. CHEMICAL COMMUNICATIONS, 2005, (23) : 2933 - 2935
  • [19] Metal-Organic Framework Thin Films as Platforms for Atomic Layer Deposition of Cobalt Ions To Enable Electrocatalytic Water Oxidation
    Kung, Chung-Wei
    Mondloch, Joseph E.
    Wang, Timothy C.
    Bury, Wojciech
    Hoffeditz, William
    Klahr, Benjamin M.
    Klet, Rachel C.
    Pellin, Michael J.
    Farha, Omar K.
    Hupp, Joseph T.
    [J]. ACS APPLIED MATERIALS & INTERFACES, 2015, 7 (51) : 28223 - 28230
  • [20] Sintering-Resistant Single-Site Nickel Catalyst Supported by Metal Organic Framework
    Li, Zhanyong
    Schweitzer, Neil M.
    League, Aaron B.
    Bernales, Varinia
    Peters, Aaron W.
    Getsoian, Andrew Bean
    Wang, Timothy C.
    Miller, Jeffrey T.
    Vjunov, Aleksei
    Fulton, John L.
    Lercher, Johannes A.
    Cramer, Christopher J.
    Gagliardi, Laura
    Hupp, Joseph T.
    Farha, Omar K.
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2016, 138 (06) : 1977 - 1982
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