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监测最终形态下的催化剂:整体式催化剂的光谱研究。

Monitoring catalysts at work in their final form: spectroscopic investigations on a monolithic catalyst.

机构信息

Instituto de Catálisis y Petroleoquímica, Consejo Superior de Investigaciones Científicas, Calle Marie Curie 2, Cantoblanco, 28049-Madrid, Spain.

出版信息

Phys Chem Chem Phys. 2012 Feb 21;14(7):2171-7. doi: 10.1039/c1cp22629k. Epub 2011 Oct 18.

DOI:10.1039/c1cp22629k
PMID:22009277
Abstract

A monolithic vanadia-titania based catalyst has been subjected to studies with in situ FTIR spectroscopy coupled with mass spectrometry, during the SCR (Selective Catalytic Reduction) reaction. A device based on a transmission reactor cell for monolithic samples was constructed, dedicated to the study of surface species during reaction. After analysing the steady state SCR activity under industrially relevant conditions, NH(3) chemisorption phenomena as a function of temperature and the subsequent SCR reaction of NO + O(2) with chemisorbed ammonia and ammonium ion species were also investigated. The observations reported here serve as a demonstration of the great potential for the application of operando spectroscopy on monolithic systems. This cross disciplinary approach aims to identify reaction pathways, active sites, intermediate- and spectator-species for catalytic reactions under truly industrial conditions in a shaped monolithic catalyst based on monitoring chemical profiles along its channels. In particular, by demonstrating the feasibility of the approach using the technically challenging operando transmission FTIR spectroscopy methodology, we foresee easy future adaption of this approach with other surface or bulk sensitive techniques, e.g. Raman and UV-vis spectroscopy.

摘要

一种整体式的钒钛基催化剂已经在 SCR(选择性催化还原)反应中通过原位傅里叶变换红外光谱(FTIR)结合质谱(MS)技术进行了研究。构建了一种基于传输反应器池的用于整体式样品的装置,用于研究反应过程中的表面物种。在分析了在工业相关条件下的稳态 SCR 活性之后,还研究了 NH(3)化学吸附现象作为温度的函数,以及随后的 NO + O(2)与化学吸附的氨和铵离子物种的 SCR 反应。这里报告的观察结果证明了在基于监测通道中化学分布的整体式系统上进行操作光谱学的应用具有很大的潜力。这种跨学科的方法旨在通过监测沿其通道的化学分布来确定在真正工业条件下的催化反应的反应途径、活性位点、中间和旁观物种。特别地,通过使用具有技术挑战性的操作传输 FTIR 光谱学方法证明了该方法的可行性,我们预见到未来很容易适应这种方法与其他表面或体相敏感技术,例如拉曼和紫外可见光谱学。

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