Ethanol upgrading via alkali-exchanged KL-zeolite: Unravelling catalytic behavior, reaction mechanism and thermodynamic effects

IF 1.7 4区化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Journal of Chemical Sciences Pub Date : 2024-08-10 DOI:10.1007/s12039-024-02290-6

Digvijay Badghaiya, Jigisha K Parikh, Parimal A Parikh

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Abstract

Catalysts based on KL-zeolite exchanged with alkali metal ions (Rb⁺ and Cs⁺) were studied for conversion of ethanol to oligomerization through the Guerbet reaction pathway. The catalysts were characterized by techniques such as ICP-AES, FESEM-EDX, N₂-adsorption-desorption, and CO₂-TPD to assess their physio-chemical properties. Effects of operating parameters, namely reaction temperature, pressure, and feed flow rate on catalytic activity for the conversion of ethanol to n-butanol were examined. Furthermore, influence of alkali metal loading on KL-zeolite was explored. Substantial ethanol conversion (42.6%) and n-butanol yield (13.9%) were achieved at 450°C and 30 kg/cm² after a 6 h reaction employing Cs-KL zeolite catalyst. Observations indicated that the butanol selectivity is highest among the reported literature. Additionally, this catalyst has exhibited low deactivation rate attributable to coke formation. Spent catalysts were studied for XRD and DTG/TGA analysis. Present investigation establishes that KL-zeolite, particularly when modified with alkali metal ions, proves to be an efficient catalyst for the Guerbet conversion of ethanol, highlighting its potential for ethanol upgrading.

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通过碱交换 KL 沸石进行乙醇升级：揭示催化行为、反应机理和热力学效应

研究了以碱金属离子（Rb+ 和 Cs+）交换的 KL 沸石为基础的催化剂，用于通过格尔伯特反应途径将乙醇转化为低聚物。采用 ICP-AES、FESEM-EDX、N2-吸附-解吸和 CO2-TPD 等技术对催化剂进行了表征，以评估其物理化学性质。研究了反应温度、压力和进料流速等操作参数对乙醇转化为正丁醇催化活性的影响。此外，还探讨了碱金属负载对 KL 沸石的影响。使用 Cs-KL 沸石催化剂在 450°C 和 30 kg/cm2 下反应 6 小时后，乙醇转化率（42.6%）和正丁醇产率（13.9%）均大幅提高。观察结果表明，该催化剂的丁醇选择性是文献报道中最高的。此外，由于焦炭的形成，这种催化剂的失活率较低。对废催化剂进行了 XRD 和 DTG/TGA 分析。目前的研究表明，KL-沸石，尤其是用碱金属离子改性后的KL-沸石，被证明是一种用于乙醇格尔伯特转化的高效催化剂，凸显了其在乙醇升级方面的潜力。

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来源期刊

Journal of Chemical Sciences CHEMISTRY, MULTIDISCIPLINARY-

CiteScore

3.10

自引率

5.90%

发文量

107

审稿时长

1 months

期刊介绍： Journal of Chemical Sciences is a monthly journal published by the Indian Academy of Sciences. It formed part of the original Proceedings of the Indian Academy of Sciences – Part A, started by the Nobel Laureate Prof C V Raman in 1934, that was split in 1978 into three separate journals. It was renamed as Journal of Chemical Sciences in 2004. The journal publishes original research articles and rapid communications, covering all areas of chemical sciences. A significant feature of the journal is its special issues, brought out from time to time, devoted to conference symposia/proceedings in frontier areas of the subject, held not only in India but also in other countries.