In掺杂的MoVTeNbOx催化剂用于丙烷选择性氧化制丙烯酸

摘要/Abstract

摘要： 采用共沉淀法合成了MoVTeNbO_x催化剂，并在催化剂中掺杂少量In组分，制备了一种可用于丙烷选择性氧化制丙烯酸的In掺杂MoVTeNbO_x催化剂（Mo_1.00V_0.30Te_0.23Nb_0.12InyO_x），与不掺杂In的MoVTeNbO_x催化剂相比，新制备催化剂上的丙烯酸产率和选择性显著提高。使用X射线衍射、H₂程序升温还原、扫描透射电子显微镜、X射线光电子能谱等方法对In掺杂催化剂进行表征，试验结果表明，适量的In掺杂能够有效提升催化剂表面Mo⁶⁺，V⁵⁺，Te⁴⁺的含量，进而影响催化剂的活性以及丙烯酸的选择性。y的最佳范围是0.025~0.04，在该范围内的In掺杂有助于调节催化剂表面酸性位点的数量，使催化剂的氧化性提高。在反应温度为400 ℃、空速为1000mL/(g·h)、原料气组成n(C₃H₈): n(O₂): n(H₂O)为1：2：12、催化剂In和Mo摩尔比为0.025的条件下，丙烷转化率可达67.99%，丙烯酸选择性为58.30%，丙烯酸收率为39.64%。

关键词: 丙烷选择性氧化, 丙烯酸, MoVTeNbO_x催化剂, In掺杂

Abstract: Indium-doped MoVTeNbO_x catalyst (Mo_1.00V_0.30Te_0.23Nb_0.12InyO_x) for the selective oxidation of propane to acrylic acid was prepared by the coprecipitation method. Compared with the MoVTeNbO_x catalyst without In-doping, the yield of acrylic acid on the above-mentioned catalyst was significantly increased. Indium-doped catalysts were characterized by X-ray diffraction, H₂ temperature-programmed reduction, scanning transmission electron microscopy and X-ray photoelectron spectroscopy. The results showed that proper amount of Indium-doping could effectively increase the content of Mo⁶⁺, V⁵⁺ and Te⁴⁺ on the surface of the catalyst, thereby influencing the activity of the catalyst and the selectivity of acrylic acid. The optimal range of y was 0.025 to 0.04. Indium-doping in this range helped to adjust the number of acid sites on the surface of the catalyst and improve the oxidation of the catalyst. Under the conditions of the reaction temperature of 400 ℃, the space velocity of 1 000 mL/(g·h), the n(C₃H₈): n(O₂): n(H₂O) equaling to 1:2:12 and the molar ratio In/Mo of 0.025, the conversion of propane was 67.99%, the selectivity of acrylic acid was 58.30%, and the yield of acrylic acid was 39.64%.

Key words: selective oxidation, acrylic acid, MoVTeNbO_x catalyst, indium-doped

燕晓宇孙宇涵徐晓晴李春义曹佳惠张雨欣. In掺杂的MoVTeNbOx催化剂用于丙烷选择性氧化制丙烯酸[J]. 石油炼制与化工, 2024, 55(11): 17-24.

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