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MgO- and Pt-Promoted TiO2 as an Efficient Photocatalyst for the Preferential Reduction of Carbon Dioxide in the Presence of Water

作者:Shunji Xie, Yu Wang, Yu Wang, Qinghong Zhang, Weiping Deng, Ye Wang, Ye Wang · 发表于:ACS Catalysis · 年份:2014 · DOI:10.1021/cs500648p · 被引用次数:449 · 研究领域:Advanced Photocatalysis Techniques、Catalytic Processes in Materials Science、CO2 Reduction Techniques and Catalysts

The photocatalytic reduction of carbon dioxide with water to fuels and chemicals is a longstanding challenge. This article focuses on the effects of cocatalysts and reaction modes on photocatalytic behaviors of TiO 2 with an emphasis on the selectivity of photogenerated electrons for CO 2 reduction in the presence of H 2 O, which has been overlooked in most of the published papers. Our results clarified that the reaction using H 2 O vapor exhibited significantly higher selectivity for CO 2 reduction than that by immersing the photocatalyst into liquid H 2 O. We examined the effect of noble metal cocatalysts and found that the rate of CH 4 formation increased in the sequence of Ag < Rh < Au < Pd < Pt, corresponding well to the increase in the efficiency of electron–hole separation. This indicates that Pt is the most effective cocatalyst to extract photogenerated electrons for CO 2 reduction. The selectivity of CH 4 in CO 2 reduction was also enhanced by Pt. The size and loading amount of Pt affected the activity; a smaller mean size of Pt particles and an appropriate loading amount favored the formation of reduction products. The reduction of H 2 O to H 2 was accelerated more than the reduction of CO 2 in the presence of Pt, leading to a lower selectivity for CO 2 reduction and limited increases in CH 4 formation rate. We demonstrated that the addition of MgO into the Pt–TiO 2 catalyst could further enhance the formation of CH 4 . The formation of H 2 was suppressed simultaneo...