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用于合成MnO₂-TiO₂活性催化剂的反胶束策略,该催化剂用于低温和低锰含量下NH₃选择性催化还原NO

Reverse Micelle Strategy for the Synthesis of MnO -TiO Active Catalysts for NH-Selective Catalytic Reduction of NO at Both Low Temperature and Low Mn Content.

作者信息

Bonelli Barbara, Tammaro Olimpia, Martinovic Ferenc, Nasi Roberto, Dell'Agli Gianfranco, Rivolo Paola, Giorgis Fabrizio, Ditaranto Nicoletta, Deorsola Fabio Alessandro, Esposito Serena

机构信息

Dipartimento di Scienza Applicata e Tecnologia (DISAT) and INSTM Unit of Torino-Politecnico, Politecnico di Torino, Corso Duca degli Abruzzi, 24, 10129 Torino, Italy.

Dipartimento di Ingegneria Civile e Meccanica, Università degli Studi di Cassino e del Lazio Meridionale, Via G. Di Biasio 43, 03043 Cassino, Frosinone, Italy.

出版信息

ACS Omega. 2021 Sep 14;6(38):24562-24574. doi: 10.1021/acsomega.1c03153. eCollection 2021 Sep 28.

Abstract

MnO -TiO catalysts (0, 1, 5, and 10 wt % Mn nominal content) for NH-SCR (selective catalytic reduction) of NO have been synthesized by the reverse micelle-assisted sol-gel procedure, with the aim of improving the dispersion of the active phase, usually poor when obtained by other synthesis methods (e.g., impregnation) and thereby lowering its amount. For comparison, a sample at nominal 10 wt % Mn was obtained by impregnation of the (undoped) TiO sample. The catalysts were characterized by using an integrated multitechnique approach, encompassing X-ray diffraction followed by Rietveld refinement, micro-Raman spectroscopy, N isotherm measurement at -196 °C, energy-dispersive X-ray analysis, diffuse reflectance UV-vis spectroscopy, temperature-programmed reduction technique, and X-ray photoelectron spectroscopy. The obtained results prove that the reverse micelle sol-gel approach allowed for enhancing the catalytic activity, in that the catalysts were active in a broad temperature range at a substantially low Mn loading, as compared to the impregnated catalyst. Particularly, the 5 wt % Mn catalyst showed the best NH-SCR activity in terms of both NO conversion (ca. 90%) and the amount of produced NO (ca. 50 ppm) in the 200-250 °C temperature range.

摘要

通过反胶束辅助溶胶-凝胶法合成了用于NH₃选择性催化还原NO的MnOₓ-TiO₂催化剂(名义锰含量为0、1、5和10 wt%),目的是改善活性相的分散性,活性相通过其他合成方法(如浸渍法)获得时通常分散性较差,从而减少其用量。作为对比,通过浸渍(未掺杂的)TiO₂样品获得了名义锰含量为10 wt%的样品。采用综合多技术方法对催化剂进行了表征,包括X射线衍射及Rietveld精修、显微拉曼光谱、-196℃下的N₂等温线测量、能量色散X射线分析、漫反射紫外可见光谱、程序升温还原技术和X射线光电子能谱。所得结果证明,反胶束溶胶-凝胶法能够提高催化活性,因为与浸渍催化剂相比,这些催化剂在相当低的锰负载量下在较宽的温度范围内具有活性。特别是,5 wt% Mn催化剂在200-250℃温度范围内,在NO转化率(约90%)和生成的N₂O量(约50 ppm)方面均表现出最佳的NH₃-SCR活性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/dc4c/8482467/d0789ece3336/ao1c03153_0004.jpg

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