Liu Ying, Liu Lili, Wang Leyuan, Zang Miaoliang, Li Lei, Zhang Yunkai
School of Chemistry & Chemical Engineering and Environmental Engineering, Weifang University, Weifang 261061, China.
Molecules. 2024 May 9;29(10):2217. doi: 10.3390/molecules29102217.
A series of MOF-derived ZrO-supported Pd-Ni bimetallic catalysts (PdNi/UiO-67-CTAB(n)-A500) were prepared by co-impregnation and pyrolysis at 500 °C under air atmosphere using UiO-67-CTAB(n) (CTAB: cetyltrimethylammonium bromide; n: the concentration of CTAB; = 0, 3, 8, 13, 18) as a sacrificial template. The catalytic activity of PdNi/UiO-66-CTAB(n)-A500 in 1,3-butadiene hydrogenation was found to be dependent on the crystal morphology of the UiO-67 template. The highest activity was observed over the PdNi/UiO-67-CTAB(3)-A500 catalyst which was synthesized using UiO-67-CTAB(3) with uniform octahedral morphology as the template for the 1,3-butadiene selective hydrogenation. The 1,3-butadiene conversion and total butene selectivity were 98.4% and 44.8% at 40 °C within 1 h for the PdNi/UiO-67-CTAB(3)-A500 catalyst, respectively. The catalyst of PdNi/UiO-67-CTAB(3)-A500 can be regenerated in flowing N at 200 °C. Carbon deposited on the surface of the catalyst was the main reason for its deactivation. This work is valuable for the high-efficiency bimetallic catalyst's development on the selective hydrogenation of 1,3-butadiene.
通过共浸渍法并在空气气氛中于500℃下热解,以UiO-67-CTAB(n)(CTAB:十六烷基三甲基溴化铵;n:CTAB的浓度;n = 0、3、8、13、18)作为牺牲模板,制备了一系列金属有机框架(MOF)衍生的ZrO负载的Pd-Ni双金属催化剂(PdNi/UiO-67-CTAB(n)-A500)。发现PdNi/UiO-66-CTAB(n)-A500在1,3-丁二烯加氢反应中的催化活性取决于UiO-67模板的晶体形态。在以具有均匀八面体形态的UiO-67-CTAB(3)为模板合成的PdNi/UiO-67-CTAB(3)-A500催化剂上,观察到了最高活性。对于PdNi/UiO-67-CTAB(3)-A500催化剂,在40℃下1小时内,1,3-丁二烯转化率和总丁烯选择性分别为98.4%和44.8%。PdNi/UiO-67-CTAB(3)-A500催化剂可在200℃的流动N₂中再生。沉积在催化剂表面的碳是其失活的主要原因。这项工作对于开发用于1,3-丁二烯选择性加氢的高效双金属催化剂具有重要价值。