Iron-doping and facet engineering of NiSe octahedron for synergistically enhanced triiodide reduction activity in photovoltaics.

The synergy between iron doping and (1 1 1) facet engineering in Fe-NiSe octahedron reinforces catalytic activity for IRR to yield impressive photovoltaic performance of DSSCs. [Display omitted] • The possibility of Fe-NiSe (1 1 1) as CE catalysts was investigated by DFT calculation. • The well-defined Fe-doped NiSe octahedron with (1 1 1) plane was synthesized. • Synergy between doping and facet engineering reinforces electrochemical behavior. • PCE can be further enhanced by introducing Fe heteroatom into NiSe (1 1 1). Reasonable design of cost-effective counter electrode (CE) catalysts for triiodide (I 3 −) reduction reaction (IRR) by simultaneously combining heteroatom doping and facet engineering is highly desired in iodine-based dye-sensitized solar cells (DSSCs), but really challenging. Herein, the density function theory (DFT) calculations were first conducted to demonstrate that the Fe-doped NiSe (1 1 1) showed an appropriate adsorption energy for I 3 −, increased number of metal active sites, reinforced charge-transfer ability, and strong interaction between 3 d states of metal sites and 5 p state of I 1 atoms in I 3 −, compared to NiSe (1 1 1). Based on this finding, the well-defined Fe-NiSe octahedron with exposed (1 1 1) plane (marked as Fe-NiSe (1 1 1)) and NiSe octahedron with the same exposed plane (named as NiSe (1 1 1)) are controllably synthesized. When the as-prepared Fe-NiSe (1 1 1) and NiSe (1 1 1) worked as CE catalysts, Fe-NiSe (1 1 1) exhibits improved electrochemical performance with higher power conversion efficiency (PCE) than NiSe (1 1 1), providing new opportunity to replace precious Pt for DSSCs. [ABSTRACT FROM AUTHOR]