Abstract
The catalytic performance for the oxidative coupling of methane (OCM) over chloride-containing Li/SnO2 was investigated experimentally and the mechanism of OCM was further suggested. Cl− ions exerted remarkable influence on the catalytic performance of Li/SnO2, with that at 750 °C displaying the highest catalytic activity (18.5% C2 yield) for OCM. The prepared catalysts were characterized with N2 physisorption, X-ray diffraction, O2-temperature programmed desorption, X-ray photoelectron spectroscopy and H2 temperature programmed reduction measurement to elucidate the effect of Cl− ions on its properties and catalytic performance. The results showed that the enhanced OCM catalytic activity of the chloride-containing Li/SnO2 catalysts compared with pure Li/SnO2 catalyst may originate from the higher concentration of anion vacancies, more rapid oxygen mobility and improved redox ability of tin. In addition, characterization by CO2-temperature programmed desorption, infrared spectroscopy and O2 frequency pulse reactions results illustrated that adding Cl− ions improved performance of Li/SnO2, which not only reduced strong basic sites to prevent the formation of poisoning carbonate, but also facilitated the formed chloromethane to convert quickly to ethylene.
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