4.6 Article

Nonoxidative coupling of ethane with gold loaded photocatalysts

期刊

CATALYSIS SCIENCE & TECHNOLOGY
卷 12, 期 5, 页码 1551-1561

出版社

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1cy02193a

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资金

  1. Nanotechnology Platform project of the MEXT, Japan [JPMXP09A21KT0030]
  2. ISHIZUE 2020 of the Kyoto University Research Development Program
  3. Japan Society for the Promotion of Science (JSPS) [21H01975, 20K21108, 19K15359]
  4. Program for Elements Strategy Initiative for Catalysts & Batteries (ESICB) by the MEXT of Japan [JPMXP0112101003]
  5. JICA
  6. Grants-in-Aid for Scientific Research [21H01975, 20K21108, 19K15359] Funding Source: KAKEN

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This study investigated the direct conversion of ethane to n-butane and hydrogen using gold loaded gallium oxide and titanium dioxide photocatalysts. The Ga2O3 photocatalyst produced n-butane, ethene, and hydrogen with a nearly stoichiometric ratio of products. The addition of gold to the Ga2O3 sample significantly increased the production rate of n-butane, while the addition of gold cocatalyst improved the photocatalytic performance of the TiO2 sample.
Direct and continuous conversion of ethane to yield n-butane and hydrogen at near room temperature (ca. 320 K) was examined with gold loaded gallium oxide and titanium dioxide photocatalysts without the aid of any oxidant in a flow reactor. A Ga2O3 photocatalyst produced n-butane and ethene as well as hydrogen with an almost stoichiometric ratio of products from ethane. Loading Au on the Ga2O3 sample gave a 12 times higher production rate of n-butane such as 0.65 mu mol h(-1) with a high selectivity of 89%. Although a bare TiO2 sample showed very low yield due to poor reduction resistance, the addition of an Au cocatalyst drastically improved the photocatalytic performance of the TiO2 sample, i.e., the Au(0.2)/TiO2 sample produced n-butane and ethene continuously at least for 5 h, where the production rate of n-butane, the n-butane selectivity, and the apparent quantum efficiency (AQE) for n-butane formation were 0.92 mu mol h(-1), 92%, and 0.02%, respectively. The reaction mechanism of n-butane formation as the main reaction was proposed to be the photocatalytic nonoxidative coupling of ethane (NOCE), which is similar to the photocatalytic nonoxidative coupling of methane (NOCM).

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