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通过调制激发红外光谱法检测NH-SCR脱硝过程中SSZ-13中关键的瞬态铜中间体。

Detection of key transient Cu intermediates in SSZ-13 during NH-SCR deNO by modulation excitation IR spectroscopy.

作者信息

Greenaway Alex G, Marberger Adrian, Thetford Adam, Lezcano-González Inés, Agote-Arán Miren, Nachtegaal Maarten, Ferri Davide, Kröcher Oliver, Catlow C Richard A, Beale Andrew M

机构信息

UK Catalysis Hub , Research Complex at Harwell , Rutherford Appleton Laboratory , Didcot OX11 0FA , UK . Email:

Department of Chemistry , 20 Gordon Street , London , WC1H 0AJ , UK.

出版信息

Chem Sci. 2019 Nov 18;11(2):447-455. doi: 10.1039/c9sc04905c. eCollection 2020 Jan 14.

Abstract

The small pore zeolite Cu-SSZ-13 is an efficient material for the standard selective catalytic reduction of nitrogen oxides (NO ) by ammonia (NH). In this work, Cu-SSZ-13 has been studied at 250 °C under high conversion using a modulation excitation approach and analysed with phase sensitive detection (PSD). While the complementary X-ray absorption near edge structure (XANES) spectroscopy measurements showed that the experiments were performed under cyclic Cu/Cu redox, Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) experiments provide spectroscopic evidence for previously postulated intermediates Cu-N([double bond, length as m-dash]O)-NH and Cu-NO in the NH-SCR deNO mechanism and for the role of [Cu(OH)]. These results therefore help in building towards a more comprehensive understanding of the reaction mechanism which to date has only been postulated .

摘要

小孔沸石Cu-SSZ-13是一种通过氨(NH₃)对氮氧化物(NOₓ)进行标准选择性催化还原的高效材料。在这项工作中,采用调制激发方法在250℃、高转化率条件下对Cu-SSZ-13进行了研究,并通过相敏检测(PSD)进行分析。虽然互补的X射线吸收近边结构(XANES)光谱测量表明实验是在循环Cu/Cu氧化还原条件下进行的,但漫反射红外傅里叶变换光谱(DRIFTS)实验为NH₃-SCR脱硝机理中先前假定的中间体Cu-N(=O)-NH和Cu-NO以及[Cu(OH)]的作用提供了光谱证据。因此,这些结果有助于更全面地理解迄今为止仅为假定的反应机理。

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