Two-Step Electrochemical Synthesis of Polypyrrole/Reduced Graphene Oxide Composites as Efficient Pt-Free Counter Electrode for Plastic Dye-Sensitized Solar Cells

Polypyrrole/reduced graphene oxide (PPy/RGO) composites on the rigid and plastic conducting substrates were fabricated via a facile two-step electrochemical process at low temperature. The polypyrrole/graphene oxide (PPy/GO) composites were first prepared on the substrate with electrochemical polymerization method, and the PPy/RGO composites were subsequently obtained by electrochemically reducing the PPy/GO. The resultant PPy/GO and PPy/RGO composites were porous, in contrast to the dense and flat pristine PPy films. The cyclic voltammetry measurement revealed that resultant composites exhibited a superior catalytic performance for triiodide reduction in the order of PPy/RGO > PPy/GO > PPy. The catalytic activity of PPy/RGO was comparable to that of Pt counter electrode (CE). Under the optimal conditions, an energy conversion efficiency of 6.45% was obtained for a rigid PPy/RGO-based dye-sensitized solar cell, which is 90% of that for a thermally deposited Pt-based device (7.14%). A plastic counter electrode was fabricated by depositing PPy/RGO composites on the plastic ITO/PEN substrate, and then an all-plastic device was assembled and exhibited an energy conversion efficiency of 4.25%, comparable to that of the counterpart using a sputtered-Pt CE (4.83%) on a plastic substrate. These results demonstrated that electrochemical synthesis is a facile low-temperature method to fabricate high-performance RGO/polyrner composite-based CEs for plastic DSCs.