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In this article, the roles of surface-active sites in dominating photoelectron selectivity for CO2 reduction products are well demonstrated over photocatalyst models of 100 SrTiO3 and 110 SrTiO3. On the easily exposed 100 facets terminated with Sr-O atoms, photoelectrons are of 8 mol % for CH4 and 92 mol % for CO generation. The Sr-O-Ti configuration in the 110 facets could enrich the surface charge density due to the lower interface resistance for higher photocatalytic efficiency (1.6-fold). The dual sites of Ti and adjacent Sr atoms are
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