High-density frustrated Lewis pairs based on Lamellar Nb<sub>2</sub>O<sub>5</sub> for photocatalytic non-oxidative methane coupling.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 37037834.
- Also identified by DOI 10.1038/s41467-023-37663-x and PMC identifier 10086065.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
Photocatalytic methane conversion requires a strong polarization environment composed of abundant activation sites with the robust stretching ability for C-H scissoring. High-density frustrated Lewis pairs consisting of low-valence Lewis acid Nb and Lewis base Nb-OH are fabricated on lamellar Nb<sub>2</sub>O<sub>5</sub> through a thermal-reduction promoted phase-transition process. Benefitting from the planar atomic arrangement of lamellar Nb<sub>2</sub>O<sub>5</sub>, the frustrated Lewis pairs sites are highly exposed and accessible to reactants, which results in a superior methane conversion rate of 1456 μmol g<sup>-1</sup> h<sup>-1</sup> for photocatalytic non-oxidative methane coupling without the assistance of noble metals. The time-dependent DFT calculation demonstrates the photo-induced electron transfer from LA to LB sites enhances their intensities in a concerted way, promoting the C-H cleavage through the coupling of LA and LB. This work provides in-depth insight into designing and constructing a polarization micro-environment for photocatalytic C-H activation of methane without the assistance of noble metals.