Enhanced Photocatalytic Activity and Stability in Hydrogen Evolution of Mo6 Iodide Clusters Supported on Graphene Oxide

Catalytic properties of the cluster compound (TBA)2[Mo6Ii8(O2CCH3)a6] (TBA = tetrabutylammonium) and a new hybrid material (TBA)2Mo6Ii8@GO (GO = graphene oxide) in water photoreduction into molecular hydrogen were investigated. New hybrid material (TBA)2Mo6Ii8@GO was prepared by coordinative immobil...

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Published inNanomaterials (Basel, Switzerland) Vol. 10; no. 7; p. 1259
Main Authors Puche, Marta, García-Aboal, Rocío, Mikhaylov, Maxim A., Sokolov, Maxim N., Atienzar, Pedro, Feliz, Marta
Format Journal Article
LanguageEnglish
Published MDPI 28.06.2020
MDPI AG
Subjects
graphene oxide
hydrogen generation
metal cluster
molybdenum
nanocomposite
photocatalysis
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Abstract Catalytic properties of the cluster compound (TBA)2[Mo6Ii8(O2CCH3)a6] (TBA = tetrabutylammonium) and a new hybrid material (TBA)2Mo6Ii8@GO (GO = graphene oxide) in water photoreduction into molecular hydrogen were investigated. New hybrid material (TBA)2Mo6Ii8@GO was prepared by coordinative immobilization of the (TBA)2[Mo6Ii8(O2CCH3)a6] onto GO sheets and characterized by spectroscopic, analytical, and morphological techniques. Liquid and, for the first time, gas phase conditions were chosen for catalytic experiments under UV–Vis irradiation. In liquid water, optimal H2 production yields were obtained after using (TBA)2[Mo6Ii8(O2CCH3)a6] and (TBA)2Mo6Ii8@GO) catalysts after 5 h of irradiation of liquid water. Despite these remarkable catalytic performances, “liquid-phase” catalytic systems have serious drawbacks: the cluster anion evolves to less active cluster species with partial hydrolytic decomposition, and the nanocomposite completely decays in the process. Vapor water photoreduction showed lower catalytic performance but offers more advantages in terms of cluster stability, even after longer radiation exposure times and recyclability of both catalysts. The turnover frequency (TOF) of (TBA)2Mo6Ii8@GO is three times higher than that of the microcrystalline (TBA)2[Mo6Ii8(O2CCH3)a6], in agreement with the better accessibility of catalytic cluster sites for water molecules in the gas phase. This bodes well for the possibility of creating {Mo6I8}4+-based materials as catalysts in hydrogen production technology from water vapor.
AbstractList Catalytic properties of the cluster compound (TBA)2[Mo6Ii8(O2CCH3)a6] (TBA = tetrabutylammonium) and a new hybrid material (TBA)2Mo6Ii8@GO (GO = graphene oxide) in water photoreduction into molecular hydrogen were investigated. New hybrid material (TBA)2Mo6Ii8@GO was prepared by coordinative immobilization of the (TBA)2[Mo6Ii8(O2CCH3)a6] onto GO sheets and characterized by spectroscopic, analytical, and morphological techniques. Liquid and, for the first time, gas phase conditions were chosen for catalytic experiments under UV–Vis irradiation. In liquid water, optimal H2 production yields were obtained after using (TBA)2[Mo6Ii8(O2CCH3)a6] and (TBA)2Mo6Ii8@GO) catalysts after 5 h of irradiation of liquid water. Despite these remarkable catalytic performances, “liquid-phase” catalytic systems have serious drawbacks: the cluster anion evolves to less active cluster species with partial hydrolytic decomposition, and the nanocomposite completely decays in the process. Vapor water photoreduction showed lower catalytic performance but offers more advantages in terms of cluster stability, even after longer radiation exposure times and recyclability of both catalysts. The turnover frequency (TOF) of (TBA)2Mo6Ii8@GO is three times higher than that of the microcrystalline (TBA)2[Mo6Ii8(O2CCH3)a6], in agreement with the better accessibility of catalytic cluster sites for water molecules in the gas phase. This bodes well for the possibility of creating {Mo6I8}4+-based materials as catalysts in hydrogen production technology from water vapor.
Catalytic properties of the cluster compound (TBA) 2 [Mo 6 I i 8 (O 2 CCH 3 ) a 6 ] (TBA = tetrabutylammonium) and a new hybrid material (TBA) 2 Mo 6 I i 8 @GO (GO = graphene oxide) in water photoreduction into molecular hydrogen were investigated. New hybrid material (TBA) 2 Mo 6 I i 8 @GO was prepared by coordinative immobilization of the (TBA) 2 [Mo 6 I i 8 (O 2 CCH 3 ) a 6 ] onto GO sheets and characterized by spectroscopic, analytical, and morphological techniques. Liquid and, for the first time, gas phase conditions were chosen for catalytic experiments under UV–Vis irradiation. In liquid water, optimal H 2 production yields were obtained after using (TBA) 2 [Mo 6 I i 8 (O 2 CCH 3 ) a 6 ] and (TBA) 2 Mo 6 I i 8 @GO) catalysts after 5 h of irradiation of liquid water. Despite these remarkable catalytic performances, “liquid-phase” catalytic systems have serious drawbacks: the cluster anion evolves to less active cluster species with partial hydrolytic decomposition, and the nanocomposite completely decays in the process. Vapor water photoreduction showed lower catalytic performance but offers more advantages in terms of cluster stability, even after longer radiation exposure times and recyclability of both catalysts. The turnover frequency (TOF) of (TBA) 2 Mo 6 I i 8 @GO is three times higher than that of the microcrystalline (TBA) 2 [Mo 6 I i 8 (O 2 CCH 3 ) a 6 ], in agreement with the better accessibility of catalytic cluster sites for water molecules in the gas phase. This bodes well for the possibility of creating {Mo 6 I 8 } 4+ -based materials as catalysts in hydrogen production technology from water vapor.
Author Puche, Marta
García-Aboal, Rocío
Mikhaylov, Maxim A.
Sokolov, Maxim N.
Atienzar, Pedro
Feliz, Marta
AuthorAffiliation 1 Instituto de Tecnología Química, Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas, Avenida de los Naranjos s/n, 46022 Valencia, Spain; mpuche@itq.upv.es (M.P.); rogarab@itq.upv.es (R.G.-A.); pedatcor@itq.upv.es (P.A.)
2 Nikolaev Institute of Inorganic Chemistry, Siberian Branch of the Russian Academy of Sciences, 3 Acad. Lavrentiev Ave., Novosibirsk 630090, Russia; mikhajlovmaks@yandex.ru (M.A.M.); caesar@niic.nsc.ru (M.N.S.)
AuthorAffiliation_xml – name: 1 Instituto de Tecnología Química, Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas, Avenida de los Naranjos s/n, 46022 Valencia, Spain; mpuche@itq.upv.es (M.P.); rogarab@itq.upv.es (R.G.-A.); pedatcor@itq.upv.es (P.A.)
– name: 2 Nikolaev Institute of Inorganic Chemistry, Siberian Branch of the Russian Academy of Sciences, 3 Acad. Lavrentiev Ave., Novosibirsk 630090, Russia; mikhajlovmaks@yandex.ru (M.A.M.); caesar@niic.nsc.ru (M.N.S.)
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Snippet Catalytic properties of the cluster compound (TBA)2[Mo6Ii8(O2CCH3)a6] (TBA = tetrabutylammonium) and a new hybrid material (TBA)2Mo6Ii8@GO (GO = graphene...
Catalytic properties of the cluster compound (TBA) 2 [Mo 6 I i 8 (O 2 CCH 3 ) a 6 ] (TBA = tetrabutylammonium) and a new hybrid material (TBA) 2 Mo 6 I i 8 @GO...
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StartPage 1259
SubjectTerms graphene oxide
hydrogen generation
metal cluster
molybdenum
nanocomposite
photocatalysis
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Title Enhanced Photocatalytic Activity and Stability in Hydrogen Evolution of Mo6 Iodide Clusters Supported on Graphene Oxide
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