Highly Selective Conversion of CH_4 to High Value-Added C_1 Oxygenates over Pd Loaded ZnTi-LDH

Lei Fu; Ruixue Zhang; Jianlong YangJiale ShiHai-Ying JiangJunwang Tang

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Highly Selective Conversion of CH_4 to High Value-Added C_1 Oxygenates over Pd Loaded ZnTi-LDH

机译：Highly Selective Conversion of CH_4 to High Value-Added C_1 Oxygenates over Pd Loaded ZnTi-LDH

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The selective oxidation of methane to high value-added liquid oxygenatedcompounds under mild conditions is of great significance to promote theefficient utilization of the carbon source, but it also faces the dilemma of lowactivity and over-oxidation. Here, ZnTi-layered double hydroxides (LDH)-A200photocatalysts with Pd loading are prepared to achieve efficient oxidation ofmethane, with O_2 as an oxidant under ambient condition. The highestgeneration rate of C_1 liquid products (methanol and formaldehyde) reaches4924.47 μmol g~(-1) h~(-1) with a selectivity close to 100% over0.5Pd-ZnTi-LDH-A200, which is 20 times higher than that of bareZnTi-LDH-A200. The photochemical results show that the modifiedphotocatalysts present much higher generation and separation efficiency ofelectron-hole pairs. In situ X-ray photoelectron spectroscopy indicates that Pdnanoparticles are the hole acceptor, which is beneficial to charge separation inthe photocatalysis. Furthermore, electron spinresonance spectroscopy andtemperature-programmed-desorption analysis prove that Pd loading ishelpful to the adsorption of methane and oxygen on the surface ofZnTi-LDH-A200, promoting the production of reactive oxygen species andactivation of methane. All these factors work together to promote the efficientconversion of CH_4 to high value-added C_1 oxygenates.

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来源
《Advanced energy materials》 |2023年第29期|2301118.1-2301118.10|共10页
作者
Lei Fu; Ruixue Zhang; Jianlong YangJiale ShiHai-Ying JiangJunwang Tang;
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作者单位

Key Lab of Synthetic and Natural Functional Molecule Chemistry of Ministry of Education, the Energy and Catalysis Hub, College of Chemistry and Materials Science Northwest University Xi’an 710127, P. R. China;

Department of Chemical Engineering UniversityCollege London WC1E7JE London,UK;

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正文语种英语
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C_1 products; methane conversion; Pd co-catalysts; photocatalysis; ZnTi-LDH;

Highly Selective Conversion of CH_4 to High Value-Added C_1 Oxygenates over Pd Loaded ZnTi-LDH

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