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Dye-sensitized solar cells (DSSCs) have gained a broad interest as an emerging photovoltaic technology with the potential to achieve high power conversion efficiency. Efficient DSSCs demand maximum photon absorption and minimum electron–hole recombination; achieved by designing various photoanode and cathode architectures. Graphene and 3D graphene-based materials (3D GBMs) have been recently explored to be incorporated in DSSCs for photocurrent enhancements via efficient charge carrier transport. The highly porous structure and interconnected pore networks/channels in 3D GBMs provide excellent electrical conductivity, large specific surface area, and high electrocatalytic activity leveraging rapid electron transport in 3D space. 3D GBMs are synthesized through bottom-up strategies including: (i) self-assembly approaches, and/or (ii) template-directed approaches. In this chapter, we describe the potential of 3D GBMs in improving the overall performance of DSSCs. In addition, the use of toxic-free carotenoids/proteins sensitizers has been highlighted for enhanced photoanode visible-light absorption.

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