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Title
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Plasma-catalytic ammonia reforming of methane over Cu-based catalysts for the production of HCN and H2 at reduced temperature
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Author
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Abstract
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| Industrial production of HCN from NH3 and CH4 not only uses precious Pt or Pt−Rh catalysts but also requires extremely high temperatures (∼1600 K). From an energetic, operational, and safety perspective, a drastic decrease in temperature is highly desirable. Here, we report ammonia reforming of methane for the production of HCN and H2 at 673 K by the combination of CH4/NH3 plasma and a supported Cu/silicalite-1 catalyst. 30% CH4 conversion has been achieved with 79% HCN selectivity. Catalyst characterization and plasma diagnostics reveal that the excellent reaction performance is attributed to metallic Cu active sites. In addition, we propose a possible reaction pathway, viz. E-R reactions with N, NH, NH2, and CH radicals produced in the plasma, for the production of HCN, based on density functional theory calculations. Importantly, the Cu/silicalite-1 catalyst costs less than 5% of the commercial Pt mesh catalyst. |
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Language
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English
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Source (journal)
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ACS catalysis. - -
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Publication
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2021
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ISSN
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2155-5435
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DOI
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10.1021/ACSCATAL.0C04940
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Volume/pages
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11
:3
(2021)
, p. 1765-1773
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ISI
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000618540300057
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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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