Li Jianfeng, Suo Wenli, Huang Yuena, Chen Minglin, Ma Haowen, Liu Chuang, Zhang Huan, Liang Kun, Dong Zhengping
State Key Laboratory of Applied Organic Chemistry, Laboratory of Special Function Materials and Structure Design of the Ministry of Education, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, PR China.
Lanzhou Petrochemical Company, PetroChina Company Limited, Lanzhou 730060, PR China.
J Colloid Interface Sci. 2023 Dec 15;652(Pt A):1053-1062. doi: 10.1016/j.jcis.2023.08.076. Epub 2023 Aug 12.
The selective hydrogenation of alkynes to alkenes is widely applied in the chemical industry; nevertheless, achieving highly selective hydrogenation with high catalytic activity is considerably challenging. Herein, ultrafine PdCu bimetallic nanoparticles encapsulated by high-surface-area mesoporous α-AlO were prepared by high-temperature calcination-reduction using a porous organic framework (POF) as the template. As-obtained PdCu@α-AlO exhibited a high selectivity of 95% for the semi-hydrogenation of phenylacetylene as a probe reaction under mild reaction conditions. The separation of continuous Pd atoms and modification of the Pd electronic state by Cu atoms suppressed β-hydride formation and alkene adsorption, contributing to high selectivity for the catalytic hydrogenation of alkynes. The catalytic activity was maintained after 7 cycles due to the strong interaction between the PdCu bimetallic nanoparticles and α-AlO as well as the encapsulation effect of mesoporous α-AlO. Thus, the current work provides a facile strategy for fabricating high-surface-area mesoporous α-AlO-supported catalysts for industrial catalysis applications.
炔烃选择性加氢制烯烃在化学工业中有着广泛应用；然而，实现具有高催化活性的高选择性加氢极具挑战性。在此，以多孔有机框架（POF）为模板，通过高温煅烧还原法制备了由高比表面积介孔α-AlO包覆的超细钯铜双金属纳米颗粒。所得的PdCu@α-AlO在温和反应条件下，作为探针反应对苯乙炔半加氢表现出95%的高选择性。连续钯原子的分离以及铜原子对钯电子态的修饰抑制了β-氢化物的形成和烯烃吸附，有助于炔烃催化加氢的高选择性。由于钯铜双金属纳米颗粒与α-AlO之间的强相互作用以及介孔α-AlO的包覆作用，催化活性在7次循环后仍得以保持。因此，当前工作为制备用于工业催化应用的高比表面积介孔α-AlO负载型催化剂提供了一种简便策略。
