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The surface plasmon resonance of metal nanoparticles has been widely used to improve photochemical transformations by plasmon-induced charge transfer. However, it remains elusive for the molecular-like metal clusters with non-metallic or excitonic behavior to enable light harvesting including electron/hole pair production and separation. Here we report a paradigm for solar energy conversion on an atomically precise Au 4 Ru 2 cluster supported on TiO 2 with oxygen vacancies, in which the electron-hole pairs can be directly generated from the excited Au 4 Ru 2 cluster and the TiO 2 support, and the photogenerated electrons can transfer to the Ru atoms. Importantly, the Ru atoms in the Au 4 Ru 2 cluster are capable of injecting the electrons into adsorbed N 2 to activate N 2 molecules. The cooperative effect in the supported Au 4 Ru 2 catalyst efficiently boosts the photocatalytic activity for N 2 fixation in comparison with homogold (Au  n  ) clusters.

chemical science

Excitonic Au4Ru2(PPh3)2(SC2H4Ph)8 cluster for light-driven dinitrogen fixation