Journal
INORGANIC CHEMISTRY
Volume 59, Issue 18, Pages 13201-13210Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.0c01518
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Funding
- National Natural Science Foundation of China [21920102005, 21835002, 21621001, 21173100]
- National Key Research and Development Program of China [2016YFB0701100]
- 111 Project [B17020]
- U.S. DOE [DEAC02-06CH11357]
- Canadian Light Source
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Developing an effective strategy to synthesize perfect titanosilicate TS-1 zeolite crystals with desirable morphologies, enriched isolated framework Ti species, and thus enhanced catalytic oxidation properties is a pervasive challenge in zeolite crystal engineering. We here used an amino acid l-carnitine as a crystal growth modifier and ethanol as a cosolvent to regulate the morphologies and the Ti coordination states of TS-1 zeolites. During the hydrothermal crystallization process, the introduced l-carnitine can not only tailor the anisotropic growth rates of zeolite crystals but also induce the formation of uniformly distributed framework Ti species through building a suitable chemical interaction with the Ti precursor species. Condition optimizations could afford the generation of perfect hexagonal plate TS-1 crystals and elongated platelet TS-1 crystals enriched in tetrahedral framework Ti sites (TiO4) or mononuclear octahedrally coordinated Ti species (TiO6). Both samples showed significant improvement in catalytic activity for the H2O2-mediated epoxidation of alkenes. In particular, the elongated platelet TS-1 enriched in TiO6 species afforded the highest activity in 1-hexene epoxidation, with a turnover frequency (TOF) of up to 131 h(1), which is approximately twice as high as that of the conventional TS-1 zeolite (TOF: 65 h(1)) and even higher than those of the literature-reported TiO-containting TS-1 catalysts derived from the hydrothermal post-treatment of TS-1 zeolites. This work demonstrates that the morphologies and the titanium coordination states of TS-1 zeolites can be effectively tuned by directly introducing suitable crystal growth modifiers, thus providing new opportunities for developing highly efficient titanosilicate zeolite catalysts for important catalytic applications.
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