Lv Yating, Wang Hai, Wu Huixin, Luo Qingsong, Wang Liang, Xiao Feng-Shou
Key Lab of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China.
Precis Chem. 2023 May 26;1(5):309-315. doi: 10.1021/prechem.3c00031. eCollection 2023 Jul 24.
Selective hydrogenation over earth-abundant metal catalysts is challenging but particularly valuable for practical applications in heterogeneous catalysis. Herein, we demonstrate that the catalytic selectivity of the commercial Raney nickel catalyst can be greatly tuned by modulation of the nickel surface by silica. Using quinoline hydrogenation as a model, we show that the silica-modified Raney nickel catalysts exhibit good activity, excellent selectivity, and long stability, whereas the undesired overhydrogenation reactions are effectively hindered. In contrast, the pristine Raney nickel catalyst shows inferior selectivity for the targeted product. Mechanistic studies confirm a positive role of silica to facilitate the desorption of 1,2,3,4-tetrahydroquinoline from the catalyst surface, thus enhancing the product selectivity.
在储量丰富的金属催化剂上进行选择性加氢具有挑战性，但对于多相催化的实际应用而言却格外有价值。在此，我们证明了通过二氧化硅对镍表面进行调控，可以极大地调整商业阮内镍催化剂的催化选择性。以喹啉加氢作为模型，我们表明二氧化硅改性的阮内镍催化剂具有良好的活性、出色的选择性和长稳定性，而不期望的过度加氢反应则受到有效抑制。相比之下，原始的阮内镍催化剂对目标产物的选择性较差。机理研究证实了二氧化硅在促进1,2,3,4-四氢喹啉从催化剂表面解吸方面的积极作用，从而提高了产物选择性。
