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Mechanistic aspects of the Andrussow process over Pt–Rh gauzes. Pathways of formation and consumption of HCN

Paper ID Volume ID Publish Year Pages File Format Full-Text
42029 45908 2010 9 PDF Available
Title
Mechanistic aspects of the Andrussow process over Pt–Rh gauzes. Pathways of formation and consumption of HCN
Abstract

Reaction pathways governing HCN selectivity in the oxidative coupling of methane and ammonia were investigated over three commercial Pt–Rh gauzes (fresh, activated, and spent) in the temporal analysis of products reactor with submillisecond-time resolution using isotopic traces. These gauzes differed in the extent of reaction-induced restructuring as well as impurity content. The ability of the gauzes to form HCN in the dual interactions of CH4 with NH3 or NO was compared considering the morphological differences of the gauzes. It was found that the progressive structural changes increased the gauze activity for methane conversion and facilitate the stabilization of methane fragments on the catalyst surface, but did not influence significantly the surface residence time of N-containing species. The well-known increase in HCN selectivity within first hours on-stream in the Andrussow process was suggested to be likely due to restructuring-induced stabilization of surface methane fragments. The decrease in the HCN selectivity after a stable phase of operation is mainly related to consecutive oxidation of HCN over iron oxide accumulated on the catalyst surface under industrial conditions of the Andrussow process.

Graphical abstractThe ability of three Pt–Rh gauzes for HCN formation via coupling of CH4 with NH3 or with NO and for oxidative and non-oxidative HCN conversion was compared considering their morphological differences.Figure optionsDownload full-size imageDownload high-quality image (62 K)Download as PowerPoint slide

Keywords
Hydrogen cyanide; Mechanism; Pt–Rh gauze; TAP-2
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Mechanistic aspects of the Andrussow process over Pt–Rh gauzes. Pathways of formation and consumption of HCN
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Publisher
Database: Elsevier - ScienceDirect
Journal: Applied Catalysis A: General - Volume 381, Issues 1–2, 15 June 2010, Pages 74–82
Authors
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Subjects
Physical Sciences and Engineering Chemical Engineering Catalysis
Get Full-Text Now
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Price was $35.95
You save - $31
Price after discount Only $4.95
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