Adsorption, Thermal Conversion, and Catalytic Hydrogenation of Acrolein on Cu Surfaces
Adsorption, Thermal Conversion, and Catalytic Hydrogenation of Acrolein on Cu Surfaces
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DOI：
10.1016/j.jcat.2022.09.013
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发表时间：
2022-09
影响因子：
7.3
通讯作者：
Mindika Tilan Nayakasinghe;R. Ponce Perez;Bo Chen;N. Takeuchi;F. Zaera
中科院分区：
文献类型：
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作者：
Mindika Tilan Nayakasinghe;R. Ponce Perez;Bo Chen;N. Takeuchi;F. Zaera
丙烯醛在铜模型表面上的吸附、热化学和催化加氢的特征在于结合表面科学技术，即反射吸收红外光谱（RAIRS）和程序升温脱附（TPD）、量子力学（DFT）计算和使用所谓的“高压电池”的催化动力学测量。丙烯醛在Cu表面的吸附主要涉及羰基氧原子和C双键。热活化导致在低于160 K时早期解离和脱氢以产生乙炔和一氧化碳，并且随后产生乙烯酮（220 K）和丙烯（260 K）。在真空下氢化与H2是不可能的，但在predosing的表面与原子H的所有可能的氢化产物，即，丙醛，1-丙醇，和烯丙醇，在TPD实验中检测到，在162，190，和210 K，分别。最后，在大气压下的催化氢化反应是缓慢的，并且仅产生丙醛，转换频率低于0.2 s-1。
The adsorption, thermal chemistry, and catalytic hydrogenation of acrolein on copper model surfaces was characterized by a combination of surface-science techniques, namely, reflection–absorption infrared spectroscopy (RAIRS) and temperature program desorption (TPD), quantum mechanics (DFT) calculations, and catalytic kinetic measurements using a so-called “high-pressure cell”. Adsorption of acrolein on the Cu surface was found to involve both the carbonyl oxygen atom and the Cdouble bondC bond. Thermal activation leads to early dissociation and dehydrogenation to produce acetylene and carbon monoxide below 160 K, and later to the production of ketene (220 K) and propene (260 K). Under vacuum hydrogenation with H2is not possible, but upon predosing of the surface with atomic H all the possible hydrogenation products, namely, propanal, 1-propanol, and allyl alcohol, were detected in TPD experiments, at 162, 190, and 210 K, respectively. Finally, catalytic hydrogenation under atmospheric pressures is slow and only produces propanal, at turnover frequencies below 0.2 s−1.