Electroactive and Sustainable Cu-MOF/PEDOT Composite Electrocatalysts for Multiple Redox Mediators and for High-Performance Dye-Sensitized Solar Cells

An electrically conductive Cu-MOF, {[Cu₂(6-mercaptonicotinic acid)(6-mercaptonicotinate)]·NH₄}_n, was successfully electrodeposited on the conductive substrates via using poly(3,4-ethylenedioxythiophene) (PEDOT) as the binder. Multiple functionalities of the Cu-MOF microparticle within the Cu-MOF/PEDOT composite electrode were systematically vindicated as (1) releasing the cohesive strength among the PEDOT matrix, thus enhancing the film adhesion to substrate, (2) providing excellent intrinsic heterogeneous rate constant via lowering the reaction active energy, (3) supplying numerous active sites at the center or edges on its (-Cu-S-)_n honeycomb-like planes, (4) facilitating the electron transfer through its two-dimensional (-Cu-S-)_n plains, and (5) benefiting the penetration of the redox mediators through its porous frameworks. In multiple redox mediators (i.e., I^-/I₃^-, cobalt(II/III)-complex, and copper(I/II)-complex), the composite Cu-MOF/PEDOT electrode exhibited superior electrocatalyst activity and kept almost 100% of its initial redox peak currents after continuous cyclic voltammetric scanning for 300 cycles. As a high-performance electrocatalyst for the counter electrode in dye-sensitized solar cells (DSSCs), the composite Cu-MOF/PEDOT electrode rendered its cell a decent solar-to-electricity conversion efficiency of up to 9.45% at 1 sun and 22.80% at room light illumination. Compared to the traditional platinum electrode (7.67%), the low-cost Cu-MOF/PEDOT composite electrode has great possibility to be used for various electrochemical devices and the Internet-of-things applications.