Preparation of gold-containing binary metal clusters by co-deposition-precipitation method and for hydrogenation of chloronitrobenzene

Ya-Ting Tsu; Yu-Wen Chen; Ya-Ting Tsu; Yu-Wen Chen

doi:10.3934/matersci.2017.3.738

AIMS Materials Science

2017, Volume 4, Issue 3: 738-754. doi: 10.3934/matersci.2017.3.738

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Preparation of gold-containing binary metal clusters by co-deposition-precipitation method and for hydrogenation of chloronitrobenzene

Ya-Ting Tsu ¹,
Yu-Wen Chen ^{1,2
,
,}

1.
Department of Chemical and Materials Engineering, National Central University, Jhong-Li 32001, Taiwan
2.
Department of Chemistry, Tomsk State University, Tomsk, Siberia, Russia

Received: 25 April 2017 Accepted: 07 June 2017 Published: 13 June 2017

Nano-gold catalyst has been reported to have high activity and selectivity for liquid phase hydrogenation reaction. In this study, gold-containing bimetals were loaded on TiO₂. For bimetallic catalysts, gold and different metals were prepared by the deposition-precipitation method, and then used NaBH₄ to reduce metal cations. The catalysts were characterized by X-ray diffraction, transmission electron microscopy, high resolution transmission electron microscopy, and X-ray photoelectron spectroscopy. The catalytic properties of these catalysts were tested by hydrogenation of p-chloronitrobenzene (p-CNB) in a batch reactor at 1.1 MPa H₂ pressure, 373 K and 500 rpm. Cu, Ag, Ru, and Pd formed nano-alloy with Au. In addition, Cu–Au, Ag–Au, and Ru–Au alloy had Cu-, Ag-, and Ru-enriched surface, respectively. Instead, Pd–Au alloy had Pd-enriched surface. There are two kinds of alloy effects: (1) geometric effects, i.e., the surface-enriched metal would change the distance of Au–Au atoms that is required for facilitating the hydrogenation of chloronitrobenzene; and (2) electronic effects, which involve charge transfer between the metals. The activity decreased in the following order: PdAu/TiO₂ > Au/TiO₂ > NiAu/TiO₂ > AgAu/TiO₂ > RuAu/TiO₂ > CuAu/TiO₂. Comparing with other metals, adding Pd in Au showed a higher activity. Adding palladium could reduce gold-valence state, and increased active sites for reaction.
- nanoalloy gold catalyst,
- metal cluster,
- titanium oxide,
- hydrogenation,
- chloronitrobenzene
Citation: Ya-Ting Tsu, Yu-Wen Chen. Preparation of gold-containing binary metal clusters by co-deposition-precipitation method and for hydrogenation of chloronitrobenzene[J]. AIMS Materials Science, 2017, 4(3): 738-754. doi: 10.3934/matersci.2017.3.738

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Abstract

Nano-gold catalyst has been reported to have high activity and selectivity for liquid phase hydrogenation reaction. In this study, gold-containing bimetals were loaded on TiO₂. For bimetallic catalysts, gold and different metals were prepared by the deposition-precipitation method, and then used NaBH₄ to reduce metal cations. The catalysts were characterized by X-ray diffraction, transmission electron microscopy, high resolution transmission electron microscopy, and X-ray photoelectron spectroscopy. The catalytic properties of these catalysts were tested by hydrogenation of p-chloronitrobenzene (p-CNB) in a batch reactor at 1.1 MPa H₂ pressure, 373 K and 500 rpm. Cu, Ag, Ru, and Pd formed nano-alloy with Au. In addition, Cu–Au, Ag–Au, and Ru–Au alloy had Cu-, Ag-, and Ru-enriched surface, respectively. Instead, Pd–Au alloy had Pd-enriched surface. There are two kinds of alloy effects: (1) geometric effects, i.e., the surface-enriched metal would change the distance of Au–Au atoms that is required for facilitating the hydrogenation of chloronitrobenzene; and (2) electronic effects, which involve charge transfer between the metals. The activity decreased in the following order: PdAu/TiO₂ > Au/TiO₂ > NiAu/TiO₂ > AgAu/TiO₂ > RuAu/TiO₂ > CuAu/TiO₂. Comparing with other metals, adding Pd in Au showed a higher activity. Adding palladium could reduce gold-valence state, and increased active sites for reaction.

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