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A series of Ti/Li/Al ternary layered double hydroxides (TiLiAl-LDHs) with different Ti:Li:Al molar ratios were prepared by a coprecipitation method for photocatalytic CO 2  reduction. It was demonstrated that the contents of anions between the layers of Ti/Li/Al-LDHs greatly determined the photocatalytic activity for CO 2  reduction. With Ti:Li:Al molar ratios optimized to be 1:3:2, the largest contents of    \documentclass[12pt]{minimal} 				\usepackage{amsmath} 				\usepackage{wasysym}  				\usepackage{amsfonts}  				\usepackage{amssymb}  				\usepackage{amsbsy} 				\usepackage{mathrsfs} 				\usepackage{upgreek} 				\setlength{\oddsidemargin}{-69pt} 				\begin{document}$${{\bf{CO}}}_{{\bf{3}}}^{{\bf{2}}}$$\end{document}CO    3    2−  anion and hydroxyl group were obtained for the Ti 1 Li 3 Al 2 -LDHs sample, which exhibited the highest photocatalytic activity for CO 2  reduction, with CH 4  production rate achieving 1.33 mmol h −1  g −1 . Moreover, the theoretical calculations show that Ti 1 Li 3 Al 2 -LDHs is a p-type semiconductor with the narrowest band gap among all the obtained TiLiAl-LDHs. After calcined at high temperatures such as 700 °C, and the obtained TiLiAl-700 sample showed much increased photocatalytic activity for CO 2  reduction, with CH 4  production rate reaching about 1.59 mmol h −1  g −1 . This calcination induced photocatalytic enhancement should be related to the cystal structure transformation from hydrotalcite to mixed oxides containing high reactive oxygen species for more efficient CO 2  reduction.

Synthesis and Optimization of Ti/Li/Al Ternary Layered Double Hydroxides for Efficient Photocatalytic Reduction of CO2 to CH4