Zhou Yiming, Shi Libin, Qi Suitao, Tan Xiao, Yi Chunhai, Yang Bolun
Shaanxi Key Laboratory of Energy Chemical Process Intensification, School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an 710049, Shaanxi, P. R. China.
SINOPEC Research Institute of Petroleum Processing Co., Ltd., Beijing 100083, P. R. China.
J Phys Chem A. 2023 Feb 9;127(5):1179-1189. doi: 10.1021/acs.jpca.2c07249. Epub 2023 Jan 30.
Polycyclic aromatic hydrocarbons (PAHs) have been paid more attention as liquid organic hydrogen carriers (LOHCs) because of their high hydrogen storage, easy transportation, low price, and other advantages. Dehydrogenation is the key point of the PAH hydrogen storage. However, the dehydrogenation reaction rate of perhydro-PAHs is slow, and their pathway is still not clear. To clarify the PAH dehydrogenation pathway, three kinds of perhydro-PAHs containing six-membered rings (methylcyclohexane, perhydro-diphenylmethane, and perhydro-dibenzyltoluene) are selected, and their dehydrogenation processes over the Pt/AlO catalyst are carried out by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFT). It was found that the dehydrogenation in the six-membered ring started in the para position of the -CH group, and then, the six-membered ring was transformed into a benzene ring gradually. Between the six-membered rings, dehydrogenation started from the side ring, which has fewer groups.
多环芳烃（PAHs）因其高储氢量、易于运输、价格低廉等优点，作为液态有机氢载体（LOHCs）受到了更多关注。脱氢是PAH储氢的关键环节。然而，全氢-PAHs的脱氢反应速率较慢，其反应途径仍不明确。为阐明PAH脱氢途径，选取了三种含六元环的全氢-PAHs（甲基环己烷、全氢二苯甲烷和全氢二苄基甲苯），并通过原位漫反射红外傅里叶变换光谱（DRIFT）对其在Pt/AlO催化剂上的脱氢过程进行了研究。结果发现，六元环中的脱氢反应始于-CH基团的对位，然后，六元环逐渐转化为苯环。在六元环之间，脱氢反应从基团较少的侧环开始。
