VMOF derived VOx/Al2O3 millimeter spherical catalyst for propane dehydrogenation with enhanced activity and stability

IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL Applied Catalysis A: General Pub Date : 2025-05-05 Epub Date: 2025-03-17 DOI:10.1016/j.apcata.2025.120225
Yuheng Zhou , Jixiang Chen , Kang Wang , Xitao Wang
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Abstract

VMOF derived VOx/Al2O3 millimeter spherical catalysts were prepared using MIL-100(V) as precursor by gum arabic-assisted sol-gel and N2-air dual calcination method, and the effects of preparation method and V loading of catalyst on the properties of VOx/Al2O3 and propane dehydrogenation performance were investigated systematically. The as-prepared spherical catalyst exhibited a watermelon-seed-like structure with VMOF derived VOx as seeds, and isolated VOx species with good dispersion could be achieved even at a higher vanadium loading owing to the isolation effects of organic ligands of MOF and alumina support. The hierarchical porous structure with mesopores of alumina and micro-scale rod-like pores left by the decomposition of MIL-100(V) through N2-air dual calcination could be created. Besides, weaker interaction between VOx derived from MOF and alumina is beneficial for increasing the amount of reducible isolated species and decreasing strong acid site amount. 7.4VOx/Al2O3 presented the highest catalytic performance with propane conversion of 30.8 %/28.2 % (initial/final) and propylene selectivity of 91.6 %/94.7 % (initial/final) within 5.25 h reaction due to the good dispersion of VOx species, hierarchical porous structure and moderate amount of surface acid sites. The high stability and excellent reaction-regeneration cycle performance of 7.4VOx/Al2O3 offered a great potential for the industrial application of vanadium-based catalysts in the propane dehydrogenation reaction.
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VMOF衍生的VOx/Al2O3毫米球形丙烷脱氢催化剂的活性和稳定性增强
以MIL-100(V)为前驱体,采用阿拉伯胶辅助溶胶-凝胶法和n2 -空气双煅烧法制备了VMOF衍生的VOx/Al2O3毫米球形催化剂,系统研究了制备方法和催化剂负载V对VOx/Al2O3性能和丙烷脱氢性能的影响。制备的球形催化剂以VMOF衍生的VOx为种子,呈西瓜种子状结构,由于MOF和氧化铝支撑的有机配体的隔离作用,即使在较高的钒负载下,也能分离出分散性良好的VOx物种。通过n_2 -空气双煅烧,MIL-100(V)分解后形成氧化铝介孔和微尺度棒状孔的分级多孔结构。此外,MOF生成的VOx与氧化铝的相互作用较弱,有利于增加可还原分离种的数量,减少强酸位点的数量。7.4VOx/Al2O3表现出最高的催化性能,在5.25 h的反应时间内丙烷转化率为30.8 %/28.2 %(初/终),丙烯选择性为91.6 %/94.7 %(初/终)。7.4VOx/Al2O3的高稳定性和优异的反应再生循环性能为钒基催化剂在丙烷脱氢反应中的工业应用提供了巨大的潜力。
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来源期刊
Applied Catalysis A: General
Applied Catalysis A: General 化学-环境科学
CiteScore
9.00
自引率
5.50%
发文量
415
审稿时长
24 days
期刊介绍: Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.
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