Active repair of a dinuclear photocatalyst for visible-light-driven hydrogen production

in: Nature Chemistry (2022)
Pfeffer, Michael; Müller, Carolin; Kastl, Evelyn T. E.; Mengele, Alexander; Bagemihl, Benedikt; Fauth, Sven; Habermehl, Johannes; Petermann, Lydia; Wächtler, Maria; Schulz, Martin; Chartrand, Daniel; Laverdière, François; Seeber, Phillip; Kupfer, Stephan; Gräfe, Stefanie; Hanan, Gary S.; Vos, Johannes G.; Dietzek-Ivanšić, Benjamin; Rau, Sven
The molecular apparatus behind biological photosynthesis retains its long-term functionality through enzymatic repair. However, bioinspired molecular devices designed for artificial photosynthesis, consisting of a photocentre, a bridging ligand and a catalytic centre, can become unstable and break down when their individual modules are structurally compromised, halting their overall functionality and operation. Here we report the active repair of such an artificial photosynthetic molecular device, leading to complete recovery of catalytic activity. We have identified the hydrogenation of the bridging ligand, which inhibits the light-driven electron transfer between the photocentre and catalytic centre, as the deactivation mechanism. As a means of repair, we used the light-driven generation of singlet oxygen, catalysed by the photocentre, to enable the oxidative dehydrogenation of the bridging unit, which leads to the restoration of photocatalytic hydrogen formation.

Third party cookies & scripts

This site uses cookies. For optimal performance, smooth social media and promotional use, it is recommended that you agree to third party cookies and scripts. This may involve sharing information about your use of the third-party social media, advertising and analytics website.
For more information, see privacy policy and imprint.
Which cookies & scripts and the associated processing of your personal data do you agree with?

You can change your preferences anytime by visiting privacy policy.