Outperformance of CaO-incorporated alumina-supported Pd catalysts in methanol decomposition

IF 3.5 3区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Research on Chemical Intermediates Pub Date : 2025-06-27 DOI:10.1007/s11164-025-05652-y

Busra Eryildirim, Nuray Oktar, Doruk Dogu

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引用次数: 0

Abstract

This study aimed to investigate the impact of CaO incorporation to alumina-supported Pd catalysts on the methanol decomposition reaction. For this purpose, mayenite, alumina and/or calcium oxide-supported Pd catalysts were synthesized. The synthesized catalysts were characterized by XRD, FTIR, Laser Raman spectroscopy, N₂ adsorption–desorption, pyridine adsorbed DRIFTS, CO₂-TPD, XPS, SEM–EDS, and ICP-OES techniques. Catalytic activity tests were carried out over a 6 h reaction period in the range of 100–400 °C. The results of the characterization and activity tests showed that the addition of CaO had significant effects on the physicochemical properties of the catalyst as well as on the catalytic activity. By adding CaO to the alumina support material, the acidity was reduced, thus reducing the selectivity for dimethyl ether (DME) formation, which is significantly high for the 1Pd@Al₂O₃ catalyst, and increasing the H₂ and CO selectivity. The mayenite-supported catalyst (1Pd@SGM), which contains alumina and calcium oxide in its unique crystal structure, showed an excellent catalytic performance close to complete methanol conversion with DME selectivity below 1% at 400 °C. In the stability test carried out at 350 °C for 6 h with 1Pd@Al₂O₃, 1Pd@SGM, and 1Pd@48CaO@Al₂O₃ catalysts used in the temperature scan, it was concluded that all catalysts were stable and 1Pd@SGM catalyst showed higher catalytic activity than the others.

Graphical abstract

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cao掺杂铝负载Pd催化剂在甲醇分解中的优异性能

本研究旨在探讨CaO掺入铝负载Pd催化剂对甲醇分解反应的影响。为此，合成了麻绿岩、氧化铝和/或氧化钙负载的钯催化剂。采用XRD、FTIR、激光拉曼光谱、N2吸附-脱附、吡啶吸附DRIFTS、CO2-TPD、XPS、SEM-EDS和ICP-OES等技术对合成的催化剂进行了表征。催化活性测试在100-400°C范围内进行了6小时的反应周期。表征和活性测试结果表明，CaO的加入对催化剂的理化性质和催化活性有显著的影响。通过在氧化铝载体材料中加入CaO，降低了酸性，从而降低了二甲醚（DME）生成的选择性，对于1Pd@Al2O3催化剂来说，二甲醚（DME）生成的选择性明显较高，并提高了H2和CO的选择性。该催化剂（1Pd@SGM）以其独特的晶体结构含有氧化铝和氧化钙，在400℃下表现出接近完全甲醇转化的优异催化性能，二甲醚选择性低于1%。采用1Pd@Al2O3、1Pd@SGM和1Pd@48CaO@Al2O3催化剂进行温度扫描，在350℃下进行了6 h的稳定性测试，结果表明，所有催化剂都是稳定的，1Pd@SGM催化剂的催化活性高于其他催化剂。图形抽象

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来源期刊

Research on Chemical Intermediates 化学-化学综合

CiteScore

5.70

自引率

18.20%

发文量

229

审稿时长

2.6 months

期刊介绍： Research on Chemical Intermediates publishes current research articles and concise dynamic reviews on the properties, structures and reactivities of intermediate species in all the various domains of chemistry. The journal also contains articles in related disciplines such as spectroscopy, molecular biology and biochemistry, atmospheric and environmental sciences, catalysis, photochemistry and photophysics. In addition, special issues dedicated to specific topics in the field are regularly published.