AI Article Synopsis

  • Near-infrared light-driven photocatalytic CO reduction (NIR-COPR) is a promising method for producing chemicals and fuels, but effective photocatalysts for this process are hard to develop.
  • A novel photocatalyst made of an anionic Ru complex within NiAl-layered double hydroxide nanosheets (NiAl-Ru-LDH) achieves efficient CO reduction with good selectivity and stability under 1200 nm light.
  • The catalyst works well due to the Ru complex lowering the band gap and facilitating electron transfer, while hydroxyl defects in the LDH enhance CO molecule adsorption and reduce energy barriers for the reaction.

Article Abstract

Near-infrared light-driven photocatalytic CO reduction (NIR-COPR) holds tremendous promise for the production of valuable commodity chemicals and fuels. However, designing photocatalysts capable of reducing CO with low energy NIR photons remains challenging. Herein, a novel NIR-driven photocatalyst comprising an anionic Ru complex intercalated between NiAl-layered double hydroxide nanosheets (NiAl-Ru-LDH) is shown to deliver efficient CO photoreduction (0.887 μmol h) with CO selectivity of 84.81 % under 1200 nm illumination and excellent stability over 50 testing cycles. This remarkable performance results from the intercalated Ru complex lowering the LDH band gap (0.98 eV) via a compression-related charge redistribution phenomenon. Furthermore, transient absorption spectroscopy data verified light-induced electron transfer from the Ru complex towards the LDH sheets, increasing the availability of electrons to drive COPR. The presence of hydroxyl defects in the LDH sheets promotes the adsorption of CO molecules and lowers the energy barriers for NIR-COPR to CO. To our knowledge, this is one of the first reports of NIR-COPR at wavelengths up to 1200 nm in LDH-based photocatalyst systems.

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http://dx.doi.org/10.1002/anie.202407638DOI Listing

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