Model Catalytic Studies on the Thermal Dehydrogenation of the Benzaldehyde/Cyclohexylmethanol LOHC System on Pt(111)

被引：0

作者：

Schwaab, Valentin ^{[1
,2
]}

Hemauer, Felix ^{[1
,2
]}

Steffen, Julien ^{[3
,4
]}

Waleska-Wellnhofer, Natalie J. ^{[1
]}

Marie Freiberger, Eva ^{[1
]}

Steinmetz, Marius ^{[1
]}

Goerling, Andreas ^{[3
,4
]}

Wasserscheid, Peter ^{[5
,6
]}

Steinrueck, Hans-Peter ^{[1
]}

Papp, Christian ^{[2
]}

机构：

[1] Friedrich Alexander Univ Erlangen Nurnberg FAU, Lehrstuhl Phys Chem 2, Egerlandstr 3, D-91058 Erlangen, Germany

[2] Freie Univ Berlin FU Berlin, Angew Phys Chem, Arnimallee 22, D-14195 Berlin, Germany

[3] Friedrich Alexander Univ Erlangen Nurnberg FAU, Lehrstuhl Theoret Chem, Egerlandstr 3, D-91058 Erlangen, Germany

[4] Erlangen Natl High Performance Comp Ctr NHRFAU, Martensstr 1, D-91058 Erlangen, Germany

[5] Forschungszentrum Julich, Helmholtz Inst Erlangen Nurnberg Renewable Energy, Cauerstr 1, D-91058 Erlangen, Germany

[6] Friedrich Alexander Univ Erlangen Nurnberg FAU, Lehrstuhl Chem Reaktionstechn, Egerlandstr 3, D-91058 Erlangen, Germany

来源：

CHEMISTRY-A EUROPEAN JOURNAL | 2024年 / 30卷 / 72期

关键词：

Liquid Organic Hydrogen Carriers (LOHCs); Alcohols; Surface Reactions; Cyclohexylmethanol; Benzaldehyde; ORGANIC HYDROGEN CARRIERS; PHOTOELECTRON-SPECTROSCOPY; MOLECULAR-BEAM; CO; ADSORPTION; EFFICIENT; STORAGE; INDOLE/INDOLINE/OCTAHYDROINDOLE; DICYCLOHEXYLMETHANE; DIPHENYLMETHANE;

D O I：

10.1002/chem.202402793

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

We investigated the dehydrogenation reaction and the thermal robustness of the liquid organic hydrogen carrier (LOHC) couple benzaldehyde/cyclohexylmethanol on a Pt(111) model catalyst in situ in synchrotron radiation photoelectron spectroscopy- and complementary temperature-programmed desorption experiments. The system stores hydrogen in a cyclohexyl group and a primary alcohol functionality and achieves an attractive hydrogen storage capacity of 7.0 mass %. We observed a stepwise dehydrogenation mechanism, characterized by a low temperature dehydrogenation of the alcohol group at 235 K. However, stability limitations challenge the system's application as reversible hydrogen storage solution, as the resultant aldehyde was found to decompose during the dehydrogenation of its cyclohexyl group (between 250 and 350 K). A comparison of cyclohexylmethanol with the structurally related secondary alcohol (1-cyclohexylethanol; 6.3 mass % hydrogen) revealed a parallel stepwise dehydrogenation pattern for both compounds, but a technically relevant superior thermal robustness of the latter, demonstrating the influence of the alcohol-group's substitution degree on the dehydrogenation characteristics of alcohol-functionalized LOHCs. Density functional theory calculations are in agreement with the experimentally observed stability trend.

引用

页数：10

共 72 条

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