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The solar H2 generation directly from natural seawater is a sustainable way of green energy. However, it is limited by a low H2 generation rate even compared to fresh water. In this report, TiO2 is chosen as a model photocatalyst to disclose the critical factor to deteriorate the H2 generation rate from seawater. The simulated seawater (SSW), which is composed of eight ions (Na+, K+, Ca2+, Mg2+, Cl−, Br−, SO42−, and CO32−), is investigated the effect of each ion on the H2 production. The results indicate that all ions have a negative effect at the same concentration as in the seawater except Br−. The CO32− has the most serious deterioration, and the H2 production rate lowers near 40% even at [CO32−] of 1.5 mmol·L−1. The H2 production rate can be recovered to 85% if the CO32− is excluded from the SSW. To understand the reason, the zeta potential of the TiO2 treated with different ions aqueous solution reveals that the zeta potential decreases when it is treated with CO32− and SO42− due to they can adsorb on the surface of TiO2 nanoparticles. Fourier transform infrared (FTIR) and thermogravimetric analysis-mass spectroscopy (TGA-MS) further confirm that the adsorbed ion is mainly from CO32−. Since the pH of seawater is about 8.9 between pKa1 (6.37) and pKa2 (10.3) of H2CO3, the CO32− should exist in the form of HCO3− in the seawater. We proposed a simple method to remove the adsorbed HCO3− from the TiO2 surface by adjusting the pH below the pKa1. The results indicate that if a trace amount of HCl (adjusting pH ~ 6.0) is added to the SSW, the H2 production rate can be recovered to 85% of that in pure water.
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