Feng Zhaolu, Liu Ziting, Bai Xuefeng
College of Materials Science and Chemical Engineering, Harbin Engineering University, Harbin 150001, China.
Institute of Petrochemical, Heilongjiang Academy of Sciences, Harbin 150040, China.
Inorg Chem. 2023 Sep 4;62(35):14355-14367. doi: 10.1021/acs.inorgchem.3c02013. Epub 2023 Aug 24.
Using Ni as a template and reductant, Ni core-Pd shell nanoparticles (Ni@Pd NPs) supported on KIT-6 (Ni@Pd/K6) were prepared by a galvanic replacement reaction under ultrasonic radiation. The characterization results show that the Ni@Pd core-shell NPs with an average diameter of 1.9 ± 0.3 nm are uniformly dispersed on KIT-6. The d-band center position of Pd in Ni@Pd core-shell NPs can be affected by both ligand and strain effects. The relationship between the d-band center of Pd and the selectivity of intermediates is a nearly straight curve. The dehydrogenation efficiency of dodecahydro--ethylcarbazole on Ni@Pd(6:1)/K6 is 100% only for 3 h at 180 °C and 95.5% for 6 h at 160 °C, which is better than the reported catalysts. The outstanding catalytic dehydrogenation performance of Ni@Pd(6:1)/K6 can be attributed to the synergistic effect of the ligand and strain effect, the high dispersion of core-shell NPs, and the weak H binding ability of the catalyst.
以镍为模板和还原剂，通过超声辐射下的电置换反应制备了负载在KIT-6上的镍核-钯壳纳米颗粒（Ni@Pd NPs）（Ni@Pd/K6）。表征结果表明，平均直径为1.9±0.3 nm的Ni@Pd核壳纳米颗粒均匀分散在KIT-6上。Ni@Pd核壳纳米颗粒中钯的d带中心位置会受到配体和应变效应的影响。钯的d带中心与中间体选择性之间的关系近似为直线。十二氢-乙基咔唑在Ni@Pd(6:1)/K6上的脱氢效率在180℃下仅3小时为100%，在160℃下6小时为95.5%，优于已报道的催化剂。Ni@Pd(6:1)/K6出色的催化脱氢性能可归因于配体和应变效应的协同作用、核壳纳米颗粒的高分散性以及催化剂较弱的氢结合能力。
