WVOx Supported on Industrial Al2O3, SiO2, AC, TiO2–Al2O3 for Catalytic Dehydration of Gas-Glycerol to Acrolein

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters Pub Date : 2024-09-13 DOI:10.1007/s10562-024-04822-8

Xiansong Xia, Liangqi Li, Lin Chen, Qi Yao, Miao Liu, Hai Lan

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引用次数: 0

Abstract

WVO_x bi-metal oxides supported on the cost-effective industrial mesoprous Al₂O₃, SiO₂, active carbon (AC), and TiO₂–Al₂O₃ with different specific surface areas (WVO/Al₂O₃, WVO/SiO₂, WVO/AC, and WVO/TiO₂–Al₂O₃) were designed and prepared through co-impregnation method for large-scale bio-glycerol dehydration to acrolein. The XRD, BET, SEM–EDS, XPS, and NH₃-TPD characterization results revealed the WO₃–VO_x (V⁴⁺/V⁵⁺) species existed with better dispersion, lower molar ratio of V⁴⁺/V⁵⁺, and enhanced strength of surface acid sites on the developed mesoporous TiO₂–Al₂O₃ in comparison with that on the mesoporous Al₂O₃, SiO₂, and AC, demonstrating strong interaction of WO₃–VO_x species with the TiO₂–Al₂O₃ support and accounting for the acrolein selectivity over catalysts following the order of WVO/TiO₂–Al₂O₃ (75.8%) > WVO/AC (71.2%) > WVO/SiO₂ (55.3%) > WVO/Al₂O₃ (42.8%). Over the WVO/TiO₂–Al₂O₃, gas-glycerol conversion reached above 97.0% with acrolein selectivity of about 75.0% under the gas hourly space velocity (GHSV) of 120–360 h⁻¹, and maintained an improved catalytic stability.

Graphical Abstract

The acrolein selectivity over the prepared catalysts followed the order of WVO/TiO₂–Al₂O₃ > WVO/AC > WVO/SiO₂ > WVO/Al₂O₃, Among them, the WVO/TiO₂–Al₂O₃ catalyst demonstrated a low V⁴⁺/V⁵⁺ ratio, surface acid sites, and exceptional catalytic performance with a gas-glycerol conversion rate of 97.2% and an acrolein selectivity of 75.8%. Even after continuous reaction for 16 h, both gas-glycerol conversion and acrolein selectivity remained above 75% and 90%, respectively. This study presents a remarkable advancement in the development of industrial catalysts with outstanding performance in terms of efficiency, stability, and cost-effectiveness. Moreover, this catalyst shows great promise for its utilization in acrolein synthesis via glycerol dehydration.

Abstract Image

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以工业 Al2O3、SiO2、AC、TiO2-Al2O3 为支撑的 WVOx 催化气体-甘油脱水生成丙烯醛

设计并通过共浸渍法制备了支撑在具有成本效益的工业介质 Al2O3、SiO2、活性炭 (AC) 和 TiO2-Al2O3 上的 WVOx 双金属氧化物，它们具有不同的比表面积（WVO/Al2O3、WVO/SiO2、WVO/AC 和 WVO/TiO2-Al2O3），用于大规模生物甘油脱水制丙烯醛。XRD、BET、SEM-EDS、XPS 和 NH3-TPD 表征结果表明，与介孔 Al2O3 相比，WO3-VOx（V4+/V5+）物种在所制备的介孔 TiO2-Al2O3 上具有更好的分散性、更低的 V4+/V5+ 摩尔比和更强的表面酸位点强度、SiO2 和 AC 上相比，开发的介孔 TiO2-Al2O3 上的表面酸性位点强度增强，这表明 WO3-VOx 物种与 TiO2-Al2O3 载体有很强的相互作用，这也是丙烯醛选择性高于 WVO/TiO2-Al2O3 （75.8%）；WVO/AC（71.2%）；WVO/SiO2（55.3%）；WVO/Al2O3（42.8%）。在气体时空速度（GHSV）为 120-360 h-1 的条件下，WVO/TiO2-Al2O3 的气体-甘油转化率达到 97.0% 以上，丙烯醛选择性约为 75.0%，并保持了较好的催化稳定性。其中，WVO/TiO2-Al2O3 催化剂的 V4+/V5+ 比值低，表面酸性位点多，催化性能优异，气体-甘油转化率达 97.2%，丙烯醛选择性达 75.8%。即使在连续反应 16 小时后，气体-甘油转化率和丙烯醛选择性仍分别保持在 75% 和 90% 以上。这项研究为开发在效率、稳定性和成本效益方面性能卓越的工业催化剂带来了重大进展。此外，该催化剂在通过甘油脱水合成丙烯醛方面的应用前景广阔。

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来源期刊

Catalysis Letters 化学-物理化学

CiteScore

5.70

自引率

3.60%

发文量

327

审稿时长

1 months

期刊介绍： Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.