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Synthesis and activation for catalysis of Fe-SAPO-34 prepared using iron polyamine complexes as structure directing agents
Catalysis Science & Technology ( IF 5 ) Pub Date : 2017-08-29 00:00:00 , DOI: 10.1039/c7cy01269a
Alessandro Turrina 1, 2, 3, 4, 5 , A. Iulian Dugulan 6, 7, 8, 9 , Jillian E. Collier 4, 5, 10 , Richard I. Walton 4, 11, 12, 13 , John L. Casci 4, 5, 14 , Paul A. Wright 1, 2, 3, 4
Affiliation  

The use of transition metal cations complexed by polyamines as structure directing agents (SDAs) for silicoaluminophosphate (SAPO) zeotypes provides a route, via removal of the organic by calcination, to microporous solids with well-distributed, catalytically-active extra-framework cations and avoids the need for post-synthesis aqueous cation exchange. Iron(II) complexed with tetraethylenepentamine (TEPA) is found to be an effective SDA for SAPO-34, giving as-prepared solids where Fe2+–TEPA complexes reside within the cha cages, as indicated by Mössbauer, optical and X-ray absorption near edge spectroscopies. By contrast, when non-coordinating tetraethylammonium ions are used as the SDAs in Fe-SAPO-34 preparations, iron is included as octahedral Fe3+ within the framework. The complex-containing Fe-SAPO-34(TEPA) materials give a characteristic visible absorption band at 550 nm (and purple colouration) when dried in air that is attributed to oxygen chemisorption. Some other Fe2+ polyamine complexes (diethylenetriamine, triethylenetetramine and pentaethylenehexamine) show similar behaviour. After calcination in flowing oxygen at 550 °C, ‘one-pot’ Fe(TEPA) materials possess Fe3+ cations and a characteristic UV-visible spectrum: they also show appreciable activity in the selective catalytic reduction of NO with NH3.

中文翻译:

铁多胺配合物为结构导向剂制备的Fe-SAPO-34的合成及催化活化

通过多胺络合的过渡金属阳离子作为硅铝磷酸盐(SAPO)分子型的结构指导剂(SDA)的使用,提供了一条途径,通过煅烧去除有机物,从而形成分布均匀,具有催化活性的骨架外阳离子和避免了合成后水性阳离子交换的需要。铁(II)络合与四亚乙基五胺(TEPA)被发现是SAPO-34的有效SDA,得到所制备的固体,其中的Fe 2+ -TEPA络合物驻留在内如Mössbauer所述,笼罩在边缘光谱仪附近具有光学吸收和X射线吸收。相比之下,当非配位四乙基铵离子用作Fe-SAPO-34制剂中的SDA时,铁以八面体Fe 3+的形式包含在框架中。当在空气中干燥时,由于氧气的化学吸附作用,含有配合物的Fe-SAPO-34(TEPA)材料在550 nm处具有特征性的可见吸收带(呈紫色)。其他一些Fe 2+多胺络合物(二亚乙基三胺,三亚乙基四胺和五亚乙基六胺)表现出相似的行为。在550°C的流动氧气中煅烧后,“一锅式” Fe(TEPA)材料具有Fe 3+阳离子和特征性的UV-可见光谱:它们在NH 3选择性催化还原NO的过程中也显示出明显的活性。
更新日期:2017-09-08
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