Zhang Yuchen, Zhang Jianhui, Liu Zongcheng, Wu Yiyi, Lv Yu, Xie Yadian, Wang Huanjiang
Key Laboratory of Low-Dimensional Materials and Big Data, School of Chemical Engineering, Guizhou Minzu University, Guiyang 550025, China.
Nanomaterials (Basel). 2022 Oct 28;12(21):3803. doi: 10.3390/nano12213803.
Motivated by the prominent catalytic performance and durability of nanoalloy catalysts, the Pd-based bimetallic nanoalloy catalysts were prepared using an aqueous reduction method. The Fe-Pd bimetallic nanoalloy catalyst (nano-Fe/Pd) demonstrated 98.4% yield and 99.7% selectivity for the unsaturated 1,4-dicarboxylic acid diesters. Moreover, the inductively coupled plasma (ICP) analysis shows that the Pd leaching of the catalyst can be effectively suppressed by alloying Fe atoms into the Pd crystal lattice for acetylene dicarbonylation. The detailed catalyst structure and morphology characterization demonstrate that introducing Fe into the Pd nanoparticles tunes the electronic-geometrical properties of the catalyst. Theoretical calculations indicate that the electrons of Fe transfer to Pd in the nano-Fe/Pd catalyst, enhancing activation of the C≡C bond in acetylene and weakening CO absorption capacity on catalyst surfaces. Alloying Fe into the Pd nanocatalyst effectively inhibits active metal leaching and improves catalyst activity and stability under high-pressure CO reactions.
受纳米合金催化剂卓越的催化性能和耐久性的驱动，采用水相还原法制备了钯基双金属纳米合金催化剂。铁-钯双金属纳米合金催化剂（纳米-Fe/Pd）对不饱和1,4-二羧酸二酯的产率为98.4%，选择性为99.7%。此外，电感耦合等离子体（ICP）分析表明，通过将铁原子合金化到钯晶格中用于乙炔二羰基化，可以有效抑制催化剂的钯浸出。详细的催化剂结构和形态表征表明，将铁引入钯纳米颗粒中可调节催化剂的电子几何性质。理论计算表明，在纳米-Fe/Pd催化剂中，铁的电子转移到钯上，增强了乙炔中C≡C键的活化，并减弱了催化剂表面对CO的吸附能力。将铁合金化到钯纳米催化剂中可有效抑制活性金属浸出，并提高高压CO反应下的催化剂活性和稳定性。
