Postsynthesis of Ti-UZM-35 titanosilicate as efficient catalyst for phenol hydroxylation reaction

The MSE-type aluminosilicate UZM-35 was efficiently prepared via adding a rational amount of MCM-68 as seed and using commercially available dimethyldipropylammonium hydroxide (DMDPAOH) as the structure-directing agent. The operation window of Si/Al ratio was widened significantly and the synthetic...

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Veröffentlicht in:Microporous and mesoporous materials 2020-10, Vol.305, p.110321, Article 110321
Hauptverfasser: Yin, Jianyong, Lu, Xinqing, Yan, Jiayin, Su, Fangzheng, Streiff, Stephane, Xu, Hao, Wu, Peng
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Sprache:eng
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Zusammenfassung:The MSE-type aluminosilicate UZM-35 was efficiently prepared via adding a rational amount of MCM-68 as seed and using commercially available dimethyldipropylammonium hydroxide (DMDPAOH) as the structure-directing agent. The operation window of Si/Al ratio was widened significantly and the synthetic system was less sensitive to the Na+/K+ ratio, compared to the synthetic systems of MCM-68 and traditional UZM-35 without seed. The crystallization time was also shortened to 4 days, compared to MCM-68 (14 days) and traditional UZM-35 (7 days). Moreover, the framework of UZM-35 kept intact after the dealumination process including high temperature calcination and acid treatment. Tetrahedrally coordinated Ti4+ ions were introduced into the framework of highly dealuminated UZM-35 via solid-gas reaction with TiCl4 vapor and the obtained Ti-UZM-35 exhibited comparable catalytic activity to Ti-MCM-68 in the phenol hydroxylation reaction. The H2O2 feeding style was adjusted in present work to improve the H2O2 utilization efficiency up to 70%. In addition, the Ti-UZM-35 catalyst was stable in the regeneration-reuse cycles. The aluminosilicate UZM-35 was efficiently prepared via adding a rational amount of MCM-68 as seed and using commercially available dimethyldipropylammonium hydroxide (DMDPAOH) as the structure-directing agent. Afterwards, the Ti-UZM-35 titanosilicate was post-synthesized by dealumination and subsequent incorporation of Ti4+ into the UZM-35 framework. The obtained Ti-UZM-35 exhibited outstanding activity in the phenol hydroxylation reaction. [Display omitted] •The aluminosilicate UZM-35 was prepared using commercially available SDA and MCM-68 as the seed.•The operation window of Si/Al ratio was widened and the synthetic system was less sensitive to the Na+/K+ ratio.•The crystallization time was shortened to 4 days.•Ti ions were tetrahedrally incorporated into the UZM-35 framework via atom-planting method.•Ti-UZM-35 zeolite demonstrated comparable catalytic performance to Ti-MCM-68 in phenol hydroxylation reaction.
ISSN:1387-1811
1873-3093
DOI:10.1016/j.micromeso.2020.110321