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Doped ZnO nanostructures have shown great potential for solar energy applications. Considering the compatible ionic radius, Mg atoms can be doped into ZnO at different concentrations. The current work reports a combined experimental and density functional theory study on the influence of the Mg dopant concentration on ZnO performance simultaneously for photocatalytic dye removal and photoelectrochemical water splitting. Among all the samples, Mg(3)-ZnO (3 at. % Mg) exhibits superior sunlight-driven photocatalytic performance. The optimal Mg-ZnO shows an 8-fold increase in the photocatalytic activity compared to the pristine ZnO. Likewise, the most active photocatalyst shows high photoelectrochemical performance with a photocurrent response of 1.54 mA at the lowest onset potential, 11 times higher than the pristine ZnO. Tuning of the Mg content results in the generation of extra charge carriers and a reduced recombination rate, which are the crucial factors responsible for enhanced photocatalytic and photoelectrochemical performance.

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