Publication date: 15th December 2014
Photoelectrochemical hydrogen production from water splitting using solar energy is a promising approach for solving the increasingly serious energy crisis and environmental problems. Recently, (oxy)nitrides photoanodes such as Ta3N5 and LaTiO2N have attracted considerable interest, since they meet several criteria for efficient photoelectrochemical hydrogen production, such as high theoretical solar-to-hydrogen efficiency (over 15%) and suitable band edge positions for unassisted water splitting. Here, we show the particular requirements for efficient charge transport among (oxy)nitride particles in the resulting film, and report the correspondingly enhanced photoelectrochemical performances for water spltting over LaTiO2N photoanodesby establishing highly crystalline porous LaTiO2N particles and superior inter-particle connectivity with reduced density of grain boundaries among the film particles. The addition of hole scavengers (for example Na2SO3) in the electrolyte allows us to assess the charge separation efficiencies of the LaTiO2N photoanodes and validates the advantages of the presently designed film characteristics. A plateau photocurrent of 6.5 mA/cm2 on Co3O4 modified LaTiO2N photoanodes has been demonstrated 1 M NaOH (pH = 13.6) electrolytes under simulated sunlight (AM 1.5 G, 100 mW/cm2) illumination. More broadly, our work shows the intrinsic requirements and significance of constituting (oxy)nitride particles for efficient charge transport and therefore desirable photoelectrochemical performances on the (oxy)nitride photoelectrodes.
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