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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. [ABSTRACT FROM AUTHOR]

Cover Feature: Surface Studies on the Energy Release of the MOST System 2-Carbethoxy-3-Phenyl-Norbornadiene/Quadricyclane (PENBD/PEQC) on Pt(111) and Ni(111) (Chem. Eur. J. 25/2023) Keywords: catalysis; energy storage; MOST system; photoelectron spectroscopy; surface reactions EN catalysis energy storage MOST system photoelectron spectroscopy surface reactions 1 1 1 05/04/23 20230502 NES 230502 B The energy storage cycle b of the molecular solar thermal (MOST) system has been investigated. Catalysis, energy storage, MOST system, photoelectron spectroscopy, surface reactions. [Extracted from the article]

2D materials, covalent functionalization, hexagonal boron nitride nanomesh, high-resolution photoemission spectroscopy, spatially defined chemical modification Keywords: 2D materials; covalent functionalization; hexagonal boron nitride nanomesh; high-resolution photoemission spectroscopy; spatially defined chemical modification EN 2D materials covalent functionalization hexagonal boron nitride nanomesh high-resolution photoemission spectroscopy spatially defined chemical modification 13095 13095 1 09/17/21 20210915 NES 210915 B By using an atomic hydrogen source b and a supersonic molecular beam of oxygen, the hexagonal boron nitride nanomesh on Rh(111) was covalently functionalized with molecular oxygen and atomic hydrogen. Cover Feature: Selective Oxygen and Hydrogen Functionalization of the h-BN/Rh(111) Nanomesh (Chem. Eur. J. 52/2021). [Extracted from the article]