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Developing a convenient ternary layered double hydroxide (LDH) semiconductor for highly active photocatalytic reduction is necessary for solving the energy crisis and environmental pollution. In this work, a highly active ternary CoAlLa-LDH was formed through inducing La³⁺ to enhance coordinatively unsaturated metals centers for development of reductive sites that resulted in improvement of photogenerated charge carrier separation. It was demonstrated that the ratio of cations between the Co/Al/La-LDHs greatly determined the LDH structure for photocatalytic activity toward CO₂ reduction. The increase of La content resulted in destruction of LDH structure with lower photoactivity for CO₂ reduction. The rate of CO and CH₄ evolution in Co₂Al₁-LDH was about 15.3 and 9.2 μmol g_cat^–1 h^–1, much higher than Co₃Al₁-LDH and Co₄Al₁-LDH, which indicates that the Co₂Al₁-LDH among CoAl-LDHs is a promising …