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Tuning Pd–Au Bimetallic Catalysts for Heterogeneous Parahydrogen-Induced Polarization C

Wang, Weiyu, Hu, Han, Xu, Jun, Wang, Qiang, Qi, Guodong, Wang, Chao, Zhao, Xingling, Zhou, Xue, Deng, Feng
Journal of physical chemistry 2018 v.122 no.2 pp. 1248-1257
alloys, catalysts, catalytic activity, gold, hydrogen, hydrogenation, ligands, nanoparticles, nuclear magnetic resonance spectroscopy, palladium, physical chemistry, polyvinyl alcohol, propylene, stabilizers, washing
The heterogeneous hydrogenation of propene over supported Pd–Au bimetallic nanoparticles was investigated using NMR and the parahydrogen-induced polarization (PHIP) technique. The composition and structure of Pd–Au/TiO₂ catalysts were correlated to both catalytic activity and pairwise hydrogen addition. Sol-immobilization, impregnation, and deposition–precipitation methods were used for preparation of the Pd–Au bimetallic catalysts. A strong signal enhancement was observed on the bimetallic catalyst prepared through the sol-immobilization method, up to 24-fold higher than that with the other two methods. The polyvinyl alcohol (PVA) stabilizer bound to the metal surface was responsible for the enhanced PHIP effect. The removal of the PVA ligands by water washing and calcination treatments shows a significant effect on the hydrogen pairwise addition. Increasing the Au content in the bimetallic alloy led to a promotion of the pairwise selectivity due to the ensemble effect. The pairwise selectivity could be tuned by the morphologies of Pd–Au structures; the Au-shell/Pd-core morphology produced a higher pairwise selectivity than that of the Pd-shell/Au-core structure, while the random PdAu alloy showed the best PHIP effect.