Self-Assembled Graphene/MWCNTs Bilayers as Platinum-Free Counter Electrodes in Dye-Sensitized Solar Cells

in: ChemPhysChem (2019)
Wahyuono, Ruri Agung; Jia, Guobin; Plentz, Jonathan; Dellith, Jan; Herrmann-Westendorf, Felix; Seyring, Martin; Presselt, Martin; Andrä, Gudrun; Rettenmayr, Markus; Dietzek, Benjamin
We describe the preparation and properties of bilayers of graphene- and multi-walled carbon nanotubes (MWCNTs) as an alternative to conventionally used platinum-based counter electrode for dye-sensitized solar cells (DSSC). The counter electrodes were prepared by a simple and easy-to-implement double self-assembly process. The preparation allows for controlling the surface roughness of electrode in a layer-by-layer deposition. Annealing under N2 atmosphere improves the electrode's conductivity and the catalytic activity of graphene and MWCNTs to reduce the I3¯ species within the electrolyte of the DSSC. The performance of different counter-electrodes is compared for ZnO photoanode-based DSSCs. Bilayer electrodes show higher power conversion efficiencies than monolayer graphene electrodes or monolayer MWCNTs electrodes. The bilayer graphene (bottom)/MWCNTs (top) counter electrode-based DSSC exhibits a maximum power conversion efficiency of 4.1% exceeding the efficiency of a reference DSSC with a thin film platinum counter electrode (efficiency of 3.4%). In addition, the double self-assembled counter electrodes are mechanically stable, which enables their recycling for DSSCs fabrication without significant loss of the solar cell performance.

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