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The effect of Si environments on NH3 selective catalytic reduction performance and moisture stability of Cu-SAPO-34 catalysts
Journal of Catalysis ( IF 6.5 ) Pub Date : 2020-09-11 , DOI: 10.1016/j.jcat.2020.09.002
Yi Cao , Dong Fan , Dali Zhu , Lijing Sun , Lei Cao , Peng Tian , Zhongmin Liu

SAPO-34s with varying Si content templated by bulky tetraethylammonium hydroxide (TEAOH) were prepared to investigate the effect of Si environments on the selective catalytic reduction (SCR) of NOx and the moisture stability of Cu-SAPO-34 catalysts. These Cu-SAPO-34s have similar Cu loadings, isolated Cu2+ content, and Brønsted acid sites (BAS). Both the ratio of Si islands and the acid strength of Cu-SAPO-34s increase with increasing Si content. In situ diffused reflection infrared Fourier transform spectroscopy (DRIFTS) studies reveal that the NH3 adsorbed on mild BAS (associated with Si(4Al) species) is more active for NOx conversion than NH3 adsorbed on strong ones (associated with Si islands). This agrees well with the high turnover frequency (TOF) and the low activation energy on Cu-SAPO-34 with low Si content and abundant Si(4Al) species (sample Si-7.7). Upon hydration treatment, the textural properties, strong acid sites, and reducibility of isolated Cu2+ ions show a decrease. This deterioration intensifies with the increasing Si islands in the catalysts due to the easier occurrence of Si migration and the formation of larger Si islands. Sample Si-7.7 exhibits the best moisture stability and thus well-preserved denitration performance. These results imply that a practical Cu-SAPO-34 catalyst with superior activity and moisture stability may be achieved by controlling the Si environments of SAPO-34 templated by bulky amines.



中文翻译:

Si环境对Cu-SAPO-34催化剂NH 3选择性催化还原性能和水分稳定性的影响

制备具有改变由笨重氢氧化四乙铵(TEAOH)模板Si含量SAPO-34,调查硅环境对选择性催化还原(SCR)的NO的影响X和Cu-SAPO-34的催化剂中的水分的稳定性。这些Cu-SAPO-34具有相似的Cu含量,分离的Cu 2+含量和布朗斯台德酸位(BAS)。随着Si含量的增加,Si岛的比例和Cu-SAPO-34s的酸强度均增加。原位漫反射傅里叶变换红外光谱(DRIFTS)的研究表明,该NH 3吸附于温和BAS(有Si(4AL相关联的)物种)更活跃NO X转化率比NH 3吸附在坚固的硅片上(与硅岛相关)。这与具有低Si含量和大量Si(4Al)物种的Cu-SAPO-34的高周转频率(TOF)和低活化能非常吻合(样品Si-7.7)。水合处理后,孤立的Cu 2+离子的质构性质,强酸位和还原性降低。由于容易发生Si迁移和形成较大的Si岛,这种劣化随着催化剂中Si岛的增加而加剧。Si-7.7样品表现出最佳的水分稳定性,因此保留了良好的脱硝性能。这些结果表明,可以通过控制由笨重的胺模板化的SAPO-34的Si环境来获得具有优异的活性和水分稳定性的实用的Cu-SAPO-34催化剂。

更新日期:2020-09-29
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