Nitrogen Modified Carbon Nano-Materials as Stable Catalysts for Phosgene Synthesis

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• 作者：Navneet K. Gupta ; Bo Peng ; Gary L. Haller ; Erika E. Ember ; Johannes A. Lercher
• 刊名：ACS Catalysis
• 出版年：2016
• 出版时间：September 2, 2016
• 年：2016
• 卷：6
• 期：9
• 页码：5843-5855
• 全文大小：798K
• 年卷期：0
• ISSN：2155-5435

文摘

The carbon-catalyzed reaction of Clb>2b> and CO constitutes the most important industrial route to phosgene. Although defects in carbon lead to surface chemical reactions, direct polarization of C-heteroatom bonds induces a more successful Clb>2b> catalytic activation, the rate-determining step in the overall catalytic cycle. The interplay between the electron-donating and -withdrawing ability of the incorporated nitrogen substituents on the formation and stabilization of active sites was examined by X-ray photoelectron and Raman spectroscopy. Mechanistic studies indicate that the polarized Clb>2b> induced by the direct interaction of Clb>2b> with a strongly electron-deficient carbon site in close proximity to a nitrogen substituent is essential for phosgene production. Nitrogen substitution into ordered carbon materials led to very active and stable carbon catalysts for COClb>2b> synthesis.