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Cu/ZrO2/S2O8(2-)/γ-Al2O3固体酸催化剂的制备及其对NO选择性还原的催化活性

[Preparation of Cu/ZrO2/S2O8(2-)/gamma-Al2O3 solid acid catalyst and its catalytic activity to selective reduction of NO].

作者信息

Guo Xi-kun, Wang Xiao-ming

机构信息

Department of Chemistry, Shantou University, Shantou 515063, China.

出版信息

Huan Jing Ke Xue. 2008 Jun;29(6):1737-42.

PMID:18763532
Abstract

Cu/ZrO2/S2O8(2-)/gamma-Al2O3 solid acid catalyst was prepared by loading of (NH4)2S2O8, ZrOCl2, and Cu(NO3)2 onto gamma-Al2O3 step by step, which was obtained from calcining of pseudoboehmite. The catalytic property of Cu/ZrO2/S2O8(2-)/gamma-Al2O3 on the selective reduction of NO by C3H6 in excess oxygen was investigated. The relationship between the structure and the catalytic property of Cu/ZrO2/S2O8(2-)/gamma-Al2O3 catalyst was also explored by means of SEM, XRD, Py-IR and TPR. The experimental results of catalytic activity of the title catalyst indicated that the maximum conversion rate of NO could reach 82.9% in the absence of water and was up to 80.2% even in the presence of 10% water vapor. The results of the structural characterization toward the catalyst showed that S2O8(2-) and ZrO2 could restrain the sinteration of gamma-Al2O3 particles and the formation of CuAl2O4 spinelle, and also facilitate the formation of new acidic sites (Brönsted acid) and the enhance of the acidity on the surface of the catalyst. In addition, ZrO2 could increase the reducibility of Cu on the catalyst. Consequently, the catalytic activity and hydrothermal stability of the catalyst were improved effectively.

摘要

通过将(NH₄)₂S₂O₈、ZrOCl₂和Cu(NO₃)₂逐步负载到由拟薄水铝石煅烧得到的γ -Al₂O₃上,制备了Cu/ZrO₂/S₂O₈²⁻/γ -Al₂O₃固体酸催化剂。研究了Cu/ZrO₂/S₂O₈²⁻/γ -Al₂O₃在过量氧气中对C₃H₆选择性还原NO的催化性能。还通过扫描电子显微镜(SEM)、X射线衍射(XRD)、吡啶吸附红外光谱(Py -IR)和程序升温还原(TPR)等手段探究了Cu/ZrO₂/S₂O₈²⁻/γ -Al₂O₃催化剂的结构与催化性能之间的关系。标题催化剂催化活性的实验结果表明,在无水条件下,NO的最大转化率可达82.9%,即使在存在10%水蒸气的情况下也高达80.2%。对该催化剂的结构表征结果表明,S₂O₈²⁻和ZrO₂可以抑制γ -Al₂O₃颗粒的烧结以及CuAl₂O₄尖晶石的形成,还促进了新酸性位点(布朗斯特酸)的形成以及催化剂表面酸度的增强。此外,ZrO₂可以提高催化剂上Cu的还原性。因此,有效地提高了催化剂的催化活性和水热稳定性。

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