Pd/Al₂O₃ catalysts were synthesized via one-pot evaporation-induced self-assembly and hydrothermal methodology, and the conventional impregnation method. XRD, N₂ adsorption-desorption and TEM showed that the one-pot synthesized catalyst, especially evaporation-induced self-assembly one (EISA-Pd/Al₂O₃) possesses the large specific surface area, ordered mesopores with the narrow pore size distribution and well-dispersed Pd particles encapsulated inside the mesopores of Al₂O₃. Catalytic hydrogenation of 2-ethyl-anthraquinone (EAQ) to form anthrahydroquinone at 0.3MPa and 70°C showed that EISA-Pd/Al₂O₃ exhibits superior performance, with the improvement of 50% in the selectivity and 82% in the activity compared with the impregnated catalyst. The high selectivity is due to the increased electron density of Pd particles and lower amount of acid sites measured by NH₃-TPD, which had an inhibitory effect on the formation of the by-product and degradation products. The high activity could be ascribed to the higher proportion of linear carbonyls which has a positive correlation with low-coordinated Pd atoms, characterized by in situ FTIR. DFT calculations revealed that the high activity of the defective Pd surface with low-coordinated Pd atoms is due to the larger adsorption energy and longer length of carbonyl bond of EAQ adsorbed on it than on the perfect Pd surface.

中文翻译：

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在有序介孔Al2O3上一锅法合成Pd纳米粒子，用于2-乙基蒽醌的催化加氢

通过一锅蒸发诱导的自组装和水热方法，以及常规的浸渍方法，合成了Pd / Al ₂ O ₃催化剂。XRD，N ₂吸附-解吸和TEM分析表明，一锅法合成的催化剂，尤其是蒸发诱导的自组装催化剂（EISA-Pd / Al ₂ O ₃）具有较大的比表面积，有序的中孔，窄孔径。分布在Al ₂ O ₃的中孔内的Pd颗粒分布均匀且分布良好。在0.3MPa和70°C下催化2-乙基蒽醌（EAQ）加氢形成蒽氢醌表明EISA-Pd / Al ₂ O ₃具有优异的性能，与浸渍的催化剂相比，选择性提高了50％，活性提高了82％。高选择性是由于Pd颗粒的电子密度增加和NH ₃ -TPD测得的酸位较低，这对副产物和降解产物的形成具有抑制作用。高活性可以归因于线性羰基化合物的较高比例，其与低配位的Pd原子呈正相关，其特征在于原位FTIR。DFT计算表明，具有低配位Pd原子的缺陷Pd表面的高活性是由于其吸附的能量大于EAQ上的EAQ的羰基键长，而不是完美的Pd表面。