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Ga(Nb,Ta)SiBEA zeolites prepared by two-step postsynthesis method: acid–base characteristics and catalytic performance in the dehydrogenation of propane to propylene with CO2
Journal of Porous Materials ( IF 2.6 ) Pub Date : 2021-06-04 , DOI: 10.1007/s10934-021-01099-9
S. M. Orlyk , M. R. Kantserova , V. I. Chedryk , P. I. Kyriienko , D. Y. Balakin , Y. Millot , S. Dzwigaj

Ga(Ta,Nb)SiBEA zeolites with Ta(V), Nb(V) and Ga(III)-single sites were prepared by two-step post-synthesis preparation procedure as evidenced by X-ray Diffraction, Fourier Transform Infrared Spectroscopy (FT–IR), 71Ga Magic Angle Spinning Nuclear Magnetic Resonance Spectroscopy and X-ray Photoelectron Spectroscopy. The acid–base properties of the zeolite catalysts were studied by Temperature-Programmed Desorption of NH3 and CO2 with mass-spectrometry control and FT–IR spectroscopy of adsorbed pyridine. The catalytic performance of the Ga(Ta,Nb)SiBEA was tested in the process of oxidative dehydrogenation of propane to propylene with CO2. For Ga4.0SiBEA zeolite catalyst the propane conversion of 57.5% and propene selectivity of 64–73% at 873 K was achieved. For Ga1.0-, Ga2.0Ta2.0- and Ga2.0Nb2.0SiBEA catalysts a higher propylene selectivity of 70–77% was reached. The key role of weak and medium strength Lewis acid sites related to the presence of well dispersed framework Ga(III) was determined for the target process.



中文翻译:

两步后合成法制备的Ga(Nb,Ta)SiBEA沸石:CO2丙烷脱氢制丙烯的酸碱特性及催化性能

具有 Ta(V)、Nb(V) 和 Ga(III) 单位点的 Ga(Ta,Nb)SiBEA 沸石是通过两步合成后制备程序制备的,如 X 射线衍射、傅里叶变换红外光谱证明( FT-IR)、71 Ga 魔角自旋核磁共振光谱和 X 射线光电子光谱。沸石催化剂的酸碱性质通过NH 3和CO 2的程序升温脱附与质谱控制和吸附吡啶的FT-IR光谱进行研究。测试了Ga(Ta,Nb)SiBEA在丙烷与CO 2氧化脱氢制丙烯过程中的催化性能。对于 Ga 4.0SiBEA 沸石催化剂在 873 K 下实现了 57.5% 的丙烷转化率和 64-73% 的丙烯选择性。对于 Ga 1.0 -、Ga 2.0 Ta 2.0 - 和 Ga 2.0 Nb 2.0 SiBEA 催化剂,达到了 70-77% 的更高丙烯选择性。为目标工艺确定了与存在良好分散的骨架 Ga(III) 相关的弱和中强度路易斯酸位点的关键作用。

更新日期:2021-06-04
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