Enhancing butadiene yield and catalyst stability via aqueous feed dilution in 1,3-butanediol dehydration

IF 2.9 3区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Reaction Chemistry & Engineering Pub Date : 2026-01-08 DOI:10.1039/D5RE00367A

Andrea C. Rodriguez, María E. Sad and Cristina L. Padró

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Abstract

The influence of using water as a diluent on the catalytic performance and deactivation in the gas-phase reaction of 1,3-butanediol (1,3BDOL) at 523 K was studied on four solid acid catalysts: HZSM5, SiO₂/Al₂O₃, Al₂O₃, and TPA (tungstophosphoric acid)/SiO₂. Reactions were carried out using both pure 1,3BDOL and 1,3BDOL 10 wt% in water as reactants. Both fresh and spent catalysts were characterized using various techniques, including N₂ physisorption, Fourier Transform Infrared (FTIR) spectroscopy, FTIR of adsorbed pyridine, MAS NMR, and Temperature Programmed Oxidation (TPO). The use of 1,3-butanediol diluted in water in the reaction increased butadiene selectivity over SiO₂/Al₂O₃, HZSM5, and TPA/SiO₂ while reducing coke formation, without altering the nature of the carbonaceous deposits, as confirmed by TPO and FTIR analyses. The reaction results showed that the presence of water is a key parameter in mitigating deactivation, enhancing the stability of catalytic activity during the conversion of 1,3BDOL on SiO₂/Al₂O₃, HZSM5, and TPA/SiO₂, as well as the selectivity towards butadiene.

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在1,3-丁二醇脱水过程中，通过水稀释提高丁二烯收率和催化剂稳定性

以HZSM5、SiO2/Al2O3、Al2O3和TPA（钨磷酸）/SiO2四种固体酸为催化剂，研究了水作为稀释剂对523 K下1,3-丁二醇（1,3bdol）气相反应的催化性能和失活的影响。用纯1,3bdol和水中浓度为10%的1,3bdol作为反应物进行反应。利用N2物理吸附、傅里叶红外光谱（FTIR）、吸附吡啶的傅里叶红外光谱（FTIR）、MAS NMR和程序升温氧化（TPO）等多种技术对新鲜和废催化剂进行了表征。通过TPO和FTIR分析证实，在反应中使用水中稀释的1,3-丁二醇比SiO2/Al2O3、HZSM5和TPA/SiO2增加了丁二烯的选择性，同时减少了焦炭的形成，而没有改变碳质沉积物的性质。结果表明，水的存在是缓解失活的关键参数，提高了1,3bdol在SiO2/Al2O3、HZSM5和TPA/SiO2上转化的催化活性稳定性，以及对丁二烯的选择性。

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来源期刊

Reaction Chemistry & Engineering Chemistry-Chemistry (miscellaneous)

CiteScore

6.60

自引率

7.70%

发文量

227

期刊介绍： Reaction Chemistry & Engineering is a new journal reporting cutting edge research into all aspects of making molecules for the benefit of fundamental research, applied processes and wider society. From fundamental, molecular-level chemistry to large scale chemical production, Reaction Chemistry & Engineering brings together communities of chemists and chemical engineers working to ensure the crucial role of reaction chemistry in today’s world.