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Experimental and Theoretical Investigation into Visible–light–promoted Selective Hydrogenation of Crotonaldehyde to Crotonyl Alcohol using Au–Co,Ni Alloy Nanoparticles Supported Layered Double Hydroxides

Abstract

In this paper, Au–Co/Ni bimetal supported layered double hydroxides (Au–Co,Ni/LDHs) was synthesized and aimed to the hydrogenation reaction of crotonaldehyde (CDE) to crotonyl alcohol (COL) both with high conversion and selectivity supplied with light irradiation. The hydrogenation experimental results indicated that both the conversion of CDE hydrogenation and the selectivity of COL have been greatly improved under visible light irradiation catalyzed by Au–Co,Ni/LDHs, with the best performance of turnover frequency of 189 h–1, 100% conversion and 99.1% selectivity (using Au–Ni/LDHs). Such high property is attributed to a synergistic effect of localized surface plasmon resonance (LSPR) of Au nanoparticles, and the additional Co or Ni species would further enhance this effect. The DFT calculation of CDE hydrogenation at Au–Co,Ni/LDHs showed that the hydrogenation happens at C2=O1 first to produce COL by following mechanism A2. Au–Ni/LDHs with lower activation energy had higher catalytic activity than that of Au–Co/LDHs. Further calculation showed that the COL hydration reaction can be hindered on Au–Co,Ni/LDHs compared to the unmodified Au/LDHs, which indicates the introduce of second metal Ni or Co besides Au could further increase the COL productivity. The DFT calculations well explained and supported the experimental results.

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Publication details

The article was received on 06 Jun 2018, accepted on 13 Jul 2018 and first published on 13 Jul 2018


Article type: Paper
DOI: 10.1039/C8TA05383A
Citation: J. Mater. Chem. A, 2018, Accepted Manuscript
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    Experimental and Theoretical Investigation into Visible–light–promoted Selective Hydrogenation of Crotonaldehyde to Crotonyl Alcohol using Au–Co,Ni Alloy Nanoparticles Supported Layered Double Hydroxides

    G. Zhang, X. Zhang, Y. Meng, X. Zhou, G. Pan, Z. Ni and S. Xia, J. Mater. Chem. A, 2018, Accepted Manuscript , DOI: 10.1039/C8TA05383A

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