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|a The striking influence of oxophilicity differences in heterometallic Mo?Mn oxide cluster reactions with water
|h [electronic resource]
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|a Washington, D.C. :
|b United States. Department of Energy. Office of Science ;
|a Oak Ridge, Tenn. :
|b Distributed by the Office of Scientific and Technical Information, U.S. Department of Energy,
|c 2020.
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|a Size: Article No. 054301 :
|b digital, PDF file.
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|a Published through Scitech Connect.
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|a 02/07/2020.
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|a "Journal ID: ISSN 0021-9606."
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|a ": US2212400."
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|a Mason, Jarrett L. ; Gupta, Ankur K. ; McMahon, Abbey J. ; Folluo, Carley N. ; Raghavachari, Krishnan ; Jarrold, Caroline Chick ;
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|a Indiana Univ., Bloomington, IN (United States)
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|a Mixed-metal oxides have proven to be effective catalysts for the hydrogen evolution reaction, often outperforming either of the binary metal oxides. The reactivity of Mn<sub>x</sub>MoO<sub>y</sub><sup>-</sup> (x = 1, 2; y = 3, 4) clusters toward H<sub>2</sub>O was investigated via time-of-flight mass spectrometry with clear evidence of cluster oxidation and corresponding H<sub>2</sub> production, specifically for Mn<sub>x</sub>MoO<sub>3</sub><sup>-</sup> (x = 1, 2) clusters. Unlike previously studied MoxOy- clusters, which assumed a broad distribution of stoichiometries (typically x ? y ? 3x), both MnMoOy- and Mn<sub>2</sub>MoO<sub>y</sub><sup>-</sup> preferentially formed y = 3 and 4 compositions in significant quantities under our source conditions. The electronic and molecular structures of the Mn<sub>x</sub>MoO<sub>y</sub> (x = 1, 2; y = 3, 4) anion and neutral clusters were probed with anion photoelectron spectroscopy and analyzed with supporting density functional theory calculations. Our studies suggest that both metal centers are involved in initial cluster?water complex formation, while Mo is the center that undergoes oxidation; hence, reactivity terminates when Mo is saturated in its highest oxidation state of +6. Across these four clusters, Mn remains relatively reduced and is stable in a high-spin electronic configuration. The preferential reactivity of water molecules toward the Mo center rather than Mn is rationalized by the much lower relative oxophilicity of Mn.
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|b FG02-07ER15889.
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|a 37 inorganic, organic, physical, and analytical chemistry
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|a Chemistry
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|a Physics
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|a Stoichiometry
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|a Photoelectron spectroscopy
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|a Mass spectrometry
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|a Isomerism
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|a Free energy
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|a Catalysts and catalysis
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|a Et al
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|a Inorganic, organic, physical, and analytical chemistry
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|a United States.
|b Department of Energy.
|b Office of Science.
|4 spn.
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|a United States.
|b Department of Energy.
|b Chicago Operations Office.
|f res.
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|a United States.
|b Department of Energy.
|b Office of Scientific and Technical Information
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|u https://www.osti.gov/servlets/purl/1800418
|z Full Text (via OSTI)
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|a .b128300991
|b 02-28-23
|c 12-08-22
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|p Can circulate
|a University of Colorado Boulder
|b Online
|c Online
|d Online
|e E 1.99:1800418
|h Superintendent of Documents classification
|i web
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