Immobilisation interaction between photoactive Cu(I)-complexes and polymeric matrices studied computationally and experimentally

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Within the frame of sustainable solar energy harvesting we use noble-metal free systems based on photoactive Cu(I) 4H-imidazolate complexes, which are efficiently photoreduced in the presence of a sacrificial donor. However, to achieve a fully sustainable system, i.e. without a sacrificial donor, we investigate the immobilisation of the photoactive Cu(I) 4H-imidazolate complexes in (functional) polymeric matrices for the prospective coupling of photooxidation and photoreduction. This project takes the first step towards an understanding of the immobilization interactions between anionic Cu(I) 4H-imidazolate complexes and cationic polymer matrices in a combined theoretical and experimental approach. Molecular dynamics simulations are used to study binding interactions and to elucidate the impact of the polymer matrix on the function-determining electronic properties of the Cu(I) complexes. These investigations are complemented by spectroscopically and electrochemically obtained data on the mutual interactions of the Cu(I) 4H-imidazolate complex and the polymer matrix. In particular, the stability of the polymer matrix under photoreductive conditions will be investigated. Only with the combination of theory and experiment an in-depth understanding of the host-guest interaction of Cu(I) complexes in polymeric matrices will be gained allowing for the purposeful development of both, the Cu(I) complex and the polymer matrix.