Surface-as-ligand, Surface-as-complex, stepwise assembly of photoactive dyes on a semiconductor surface

Nathalie Marinakis^a

^aUniversity of Basel, Spitalstrasse, 51, Basel, Switzerland

International Conference on Hybrid and Organic Photovoltaics
Proceedings of International Conference on Hybrid and Organic Photovoltaics 2015 (HOPV15)

Roma, Italy, 2015 May 11th - 13th

Organizer: Filippo De Angelis

Poster, Nathalie Marinakis, 346
Publication date: 5th February 2015

We present recent research that has been done in our group detailing the stepwise assembly of photoactive dyes on a semiconductor surface. The dyes being used are for the construction of n- or p- type solar cells consist of an anchoring ligand (Lanchor ), with carboxylic acid or phosphonic acid functionalization that will bind to the surface of the semiconductor. The dyes are heteroleptic copper(I) complexes with Lanchorcombined with a acillary ligand L_ancillary, and the combination of ligands ensures good electron transfer and injection into the semiconductor. Until now, the most common way of constructing a DSSC is to synthesize the dye as a complete entity and to attached it to the semiconductor surface (TiO2 or NiO) in one dye bath soaking. This technique, apart being time consuming for synthesis, generates uncertainties about the protonation states of the anchoring ligand fuctionalities. We have developed a breakthrough idea which consists of functionalizing the surface of the semiconductor by attaching, in a stepwise procedure, the units of the dye. The semiconductor is treated with the anchoring ligand which has functionalities (e.g. CO₂H or PO(OH)₂) that can bind to the oxide surface and a second domain is open for binding with a metal center. This 'new' surface can now be called a surface-as-ligand. In the second step the surface is immersed to a solution of [Cu(Lancilliary )2 ]⁺and a ligand exchange between Lancilliary and Lanchor forms a new surface consisting of [Cu(Lancilliary )(Lanchor )]⁺ that can be named surface-as-complex. The time scale of this method is a few hours to days, but a disadvantage of it is the loss of half of Lancilliary in the process. An alternative route that improves the 'atom efficiency' is to first fuctionalize the semiconductor with the Lanchor , followed by treatment of the surface with [Cu(MeCN)4 ][PF6 ] to form a surface-bound [Lanchor CuX2 ]⁺ species, and finally with Lancillary to give [Cu(Lancilliary )(Lanchor )]⁺. In this way the drawback concerning the loss of the half of the Lancilliary can be omitted.

Schonhofer E.; Bozic-Webwer B.; Martin C. J.; Constable E. C.;Housecroft E. C.; Zampese J. A.; `Surface-as-ligand, surface-as-complex`strategies for copper(I) dye-sesitized solar cells Dyes and Pigments 115 (2015) 154-165

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