Photoelectrochemical-driven nitrogen reduction to ammonia by a Vo-SnO2/TiO2 composite electrode.

ABSTRACT

N2 molecules with the NN triple bond structure are difficult to cleave under mild conditions to achieve the nitrogen fixation reaction. Photoelectrochemical (PEC) catalysis technology combining the advantages of photocatalysis and electrocatalysis provides the possibility of the nitrogen reduction reaction under ambient conditions. Herein, an SnO2/TiO2 photoelectrode was first fabricated through depositing SnO2 quantum dots on TiO2 nanorod arrays via a simple hydrothermal method. The oxygen vacancy (Vo) content was then induced in SnO2 through annealing SnO2/TiO2 at high temperature under an inert atmosphere. The heterogeneous structure of Vo-SnO2 quantum dots and TiO2 nanorods boosted the separation of photocarriers. The photoelectrons generated by photoexcitation were transferred from the conduction band of TiO2 to the conduction band of Vo-SnO2 and trapped by Vo. Vo activates N2 molecules adsorbed on the catalyst surface, and reacts with H+ in the electrolyte to generate NH3. The nitrogen fixation yield of PEC catalysis and its faradaic efficiency can reach 19.41 µg cm-2 h-1, and 59.6% at -0.2 V bias potential, respectively. The heterogeneous structure of Vo-SnO2/TiO2, introduction of Vo and synergistic effect between light and electricity greatly promotes the PEC nitrogen reduction to NH3.