TiN Nanoparticles on CNT-Graphene Hybrid Support as Noble-Metal-Free Counter Electrode for Quantum-Dot-Sensitized Solar Cells

The development of an efficient noble‐metal‐free counter electrode is crucial for possible applications of quantum‐dot‐sensitized solar cells (QDSSCs). Herein, we present TiN nanoparticles on a carbon nanotube (CNT)–graphene hybrid support as a noble‐metal‐free counter electrode for QDSSCs employing a polysulfide electrolyte. The resulting TiN/CNT–graphene possesses an extremely high surface roughness, a good metal–support interaction, and less aggregation relative to unsupported TiN; it also has superior solar power conversion efficiency (4.13 %) when applying a metal mask, which is much higher than that of the state‐of‐the‐art Au electrode (3.35 %). Based on electrochemical impedance spectroscopy measurements, the enhancement is ascribed to a synergistic effect between TiN nanoparticles and the CNT–graphene hybrid, the roles of which are to provide active sites for the reduction of polysulfide ions and electron pathways to TiN nanoparticles, respectively. The combination of graphene and CNTs leads to a favorable morphology that prevents stacking of graphene or bundling of CNTs, which maximizes the contact of the support with TiN nanoparticles and improves electron‐transfer capability relative to either carbon material alone. Titanium nitride electrocatalyst: TiN nanoparticles on a carbon nanotube–graphene hybrid support are fabricated and utilized as a new counter electrode material for quantum‐dot‐sensitized solar‐cell applications. The new material exhibits enhanced power‐conversion efficiency (relative to the state‐of‐the‐art Au electrode), which is ascribed to a reduced charge‐transfer resistance and a larger surface area relative to the Au electrode.