HCl Treatment of Mixed-Phase MoVTeNbOx Catalysts for Enhanced Performance in Selective Oxidation of Propane

Zeyue Wei, Hanzhi Zhang, Yunxing Bai, Xuanyu Zhang and Weixin Huang*, 
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引用次数: 0

Abstract

Hydrothermally synthesized mixed-phase MoVTeNbOx catalysts are active for catalyzing the selective oxidation of propane to acrylic acid but suffer from the presence of the amorphous phase and low specific surface areas. Herein we report that HCl treatment preferentially dissolves the amorphous phase in hydrothermally synthesized mixed-phase MoVTeNbOx catalysts and increases the catalytic performance. An optimal HCl treatment significantly increases the C3H8 conversion from 38.9% to 58.2% without changing the acrylic acid selectivity in the selective oxidation of propane to acrylic acid at 380 °C. The original and HCl treated catalysts exhibit similar apparent activation energies, while HCl treatment increases the specific surface area, surface acid sites, surface V5+ density, and C3H8 and C3H6 irreversible adsorption amounts but decreases the C3H8 and C3H6 irreversible adsorption heats. The C3H8 conversion rate is proportional to the surface V5+ density and C3H8 irreversible adsorption amount, and the TOF is measured as 3.31 ± 0.08 × 10–5 s–1 at 340 °C. Thus, HCl treatment enhances the catalytic performance of mixed-phase MoVTeNbOx catalysts mainly by increasing the active site density rather than by increasing the active site activity. Our results provide an effective approach to prepare highly active mixed-phase MoVTeNbOx catalysts for the selective oxidation of propane to acrylic acid.

混合相MoVTeNbOx催化剂的HCl处理提高丙烷选择性氧化性能
水热合成的混合相MoVTeNbOx催化剂具有催化丙烷选择性氧化制丙烯酸的活性,但存在非晶相和低比表面积的问题。本文报道了HCl处理优先溶解水热合成的混合相MoVTeNbOx催化剂中的非晶相,并提高了催化性能。在380℃丙烷选择性氧化制丙烯酸过程中,在不改变丙烯酸选择性的情况下,最佳的HCl处理显著提高了C3H8转化率,从38.9%提高到58.2%。原始催化剂和HCl处理的催化剂表现出相似的表观活化能,HCl处理增加了比表面积、表面酸位、表面V5+密度和C3H8和C3H6的不可逆吸附量,但降低了C3H8和C3H6的不可逆吸附热。C3H8转化率与表面V5+密度和C3H8不可逆吸附量成正比,340℃时的TOF为3.31±0.08 × 10-5 s-1。因此,HCl处理提高混合相MoVTeNbOx催化剂的催化性能主要是通过提高活性位点密度,而不是通过提高活性位点活性。本研究结果为制备丙烷选择性氧化制丙烯酸的高活性混合相MoVTeNbOx催化剂提供了一条有效途径。
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来源期刊
Precision Chemistry
Precision Chemistry 精密化学技术-
CiteScore
0.80
自引率
0.00%
发文量
0
期刊介绍: Chemical research focused on precision enables more controllable predictable and accurate outcomes which in turn drive innovation in measurement science sustainable materials information materials personalized medicines energy environmental science and countless other fields requiring chemical insights.Precision Chemistry provides a unique and highly focused publishing venue for fundamental applied and interdisciplinary research aiming to achieve precision calculation design synthesis manipulation measurement and manufacturing. It is committed to bringing together researchers from across the chemical sciences and the related scientific areas to showcase original research and critical reviews of exceptional quality significance and interest to the broad chemistry and scientific community.
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