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Title
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DFT and microkinetic comparison of ru-doped porphyrin-like graphene and nanotubes toward catalytic formic acid decomposition and formation
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Author
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Abstract
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| Immobilization of single metal atoms on a solid host opens numerous possibilities for catalyst designs. If that host is a two-dimensional sheet, sheet curvature becomes a design parameter potentially complementary to host and metal composition. Here, we use a combination of density functional theory calculations and microkinetic modeling to compare the mechanisms and kinetics of formic acid decomposition and formation, chosen for their relevance as a potential hydrogen storage medium, over single Ru atoms anchored to pyridinic nitrogen in a planar graphene flake (RuN4-G) and curved carbon nanotube (RuN4-CNT). Activation barriers are lowered and the predicted turnover frequencies are increased over RuN4-CNT relative to RuN4-CNT. The results highlight the potential of curvature control as a means to achieve high performance and robust catalysts. |
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Language
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English
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Source (journal)
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The journal of physical chemistry: C : nanomaterials and interfaces. - Washington, D.C., 2007, currens
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Publication
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Washington, D.C.
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2021
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ISSN
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1932-7447
[print]
1932-7455
[online]
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DOI
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10.1021/ACS.JPCC.1C03914
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Volume/pages
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125
:34
(2021)
, p. 18673-18683
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ISI
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000693413400013
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Full text (Publisher's DOI)
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Full text (open access)
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Full text (publisher's version - intranet only)
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