Phenylamine-Functionalized rGO/TiO2 Photocatalysts: Spatially Separated Adsorption Sites and Tunable Photocatalytic Selectivity

The preferential adsorption of targeted contaminants on a photocatalyst surface is highly required to realize its photocatalytic selective decomposition in a complex system. To realize the tunable preferential adsorption, altering the surface charge or polarity property of photocatalysts has widely been reported. However, it is quite difficult for a modified photocatalyst to realize the simultaneously preferential adsorption for both cationic and anionic dyes. In this study, to realize the selective adsorption for both cationic and anionic dyes on a photocatalyst surface, the negative reduced graphene oxide (rGO) nanosheets and positive phenylamine (PhNH2) molecules are successfully loaded on the TiO2 surface (PhNH2/rGO-TiO2) with spatially separated adsorption sites, where the negative rGO and positive PhNH2 molecules work as the preferential adsorption sites for cationic and anionic dyes, respectively. It was interesting to find that although all the TiO2 samples (including the naked TiO2, PhNH2/TiO2, rGO-TiO2, and PhNH2/rGO-TiO2) clearly showed a better adsorption performance for cationic dyes than anionic dyes, only the PhNH2/rGO-TiO2 with spatially separated adsorption-active sites exhibited an opposite photocatalytic selectivity, namely, the naked TiO2, PhNH2/TiO2, and rGO-TiO2 showed a preferential decomposition for cationic dyes, while the resultant PhNH2/rGO-TiO2 exhibited an excellently selective decomposition for anionic dyes. In addition, the resultant PhNH2/rGO-TiO2 photocatalyst not only realizes the tunable photocatalytic selectivity but also can completely and sequentially decompose the opposite cationic and anionic dyes.