Unexpected visible light driven photocatalytic activity without cocatalysts and sacrificial reagents from a (GaN)1- x (ZnO) x solid solution synthesized at high pressure over the entire composition range

在高压下合成的 (GaN)1-x (ZnO)x 固溶体在整个成分范围内表现出意想不到的可见光驱动光催化活性,无需助催化剂和牺牲剂

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作者:H A Naveen Dharmagunawardhane, Alwin James, Qiyuan Wu, William R Woerner, Robert M Palomino, Alexandra Sinclair, Alexander Orlov, John B Parise

Abstract

Optical and photocatalytic properties were determined for the solid solution series (GaN)1-x (ZnO) x synthesized at high pressure over the entire compositional range (x = 0.07 to 0.9). We report for the first time photocatalytic H2 evolution activity from water for (GaN)1-x (ZnO) x without cocatalysts, pH modifiers and sacrificial reagents. Syntheses were carried out by reacting GaN and ZnO in appropriate amounts at temperatures ranging from 1150 to 1200 °C, and at a pressure of 1 GPa. ZnGa2O4 was observed as a second phase, with the amount decreasing from 12.8 wt% at x = 0.07 to ∼0.5 wt% at x = 0.9. The smallest band gap of 2.65 eV and the largest average photocatalytic H2 evolution rate of 2.31 μmol h-1 were observed at x = 0.51. Samples with x = 0.07, 0.24 and 0.76 have band gaps of 2.89 eV, 2.78 eV and 2.83 eV, and average hydrogen evolution rates of 1.8 μmol h-1, 0.55 μmol h-1 and 0.48 μmol h-1, respectively. The sample with x = 0.9 has a band gap of 2.82 eV, but did not evolve hydrogen. An extended photocatalytic test showed considerable reduction of activity over 20 hours.

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