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The one-step oxidation of methanol to dimethoxymethane over sulfated vanadia-titania catalysts: influence of calcination temperature

机译:硫酸钒-二氧化钛催化剂将甲醇一步氧化为二甲氧基甲烷:煅烧温度的影响

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Sulfated vanadia-titania catalysts were prepared by the rapid combustion method and calcined at different temperatures. The influence of calcination temperature on the physicochemical properties of the catalysts was characterized by nitrogen adsorption (BET), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), inductively coupled plasma-optical emission spectroscopy (ICP-OES), X-ray photoelectron spectroscopy (XPS), temperature-programmed reduction (H-2-TPR-MS), thermogravimetry (TG) and temperature programmed desorption of ammonia (NH3-TPD) techniques. The catalytic activities were evaluated by the partial oxidation of methanol to dimethoxymethane (DMM). The results showed that vanadia and sulfate were highly dispersed as the catalysts were calcined at 723 and 773 K. The reducibility of the highly dispersed vanadia was stronger than the aggregated vanadia. And the larger number of acidic sites was related to the higher dispersion of sulfate. Moreover, the higher dispersion of vanadia contributed to higher methanol conversion, and the stronger reducibility combined with the larger number of acidic sites led to high DMM selectivity. As a result, the catalysts calcined at 723 and 773 K presented higher methanol conversion and DMM selectivity than those calcined at 673 K or above 823 K.
机译:采用快速燃烧法制备了硫酸钒-二氧化钛催化剂,并在不同温度下煅烧。煅烧温度对催化剂理化性质的影响通过氮吸附(BET),X射线衍射(XRD),傅里叶变换红外光谱(FTIR),电感耦合等离子体-光发射光谱(ICP-OES), X射线光电子能谱(XPS),程序升温还原(H-2-TPR-MS),热重分析(TG)和程序升温氨解吸(NH3-TPD)技术。通过甲醇部分氧化为二甲氧基甲烷(DMM)评估催化活性。结果表明,当催化剂在723和773 K下煅烧时,钒和硫酸盐高度分散。高度分散的钒的还原性强于聚集的钒。酸性位点的增多与硫酸盐的较高分散有关。此外,钒的较高分散度有助于较高的甲醇转化率,而较强的还原性和大量的酸性位点导致较高的DMM选择性。结果,在723 K和773 K下煅烧的催化剂比在673 K或823 K以上煅烧的催化剂具有更高的甲醇转化率和DMM选择性。

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