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- Title
High-density frustrated Lewis pairs based on Lamellar Nb<sub>2</sub>O<sub>5</sub> for photocatalytic non-oxidative methane coupling.
- Authors
Chen, Ziyu; Ye, Yutao; Feng, Xiaoyi; Wang, Yan; Han, Xiaowei; Zhu, Yu; Wu, Shiqun; Wang, Senyao; Yang, Wenda; Wang, Lingzhi; Zhang, Jinlong
- 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 Nb2O5 through a thermal-reduction promoted phase-transition process. Benefitting from the planar atomic arrangement of lamellar Nb2O5, the frustrated Lewis pairs sites are highly exposed and accessible to reactants, which results in a superior methane conversion rate of 1456 μmol g−1 h−1 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. To achieve efficient photocatalytic non-oxidative methane coupling, a strong polarization environment with abundant activation sites for C-H scissoring is needed. This can be created through the fabrication of high-density frustrated Lewis pairs on lamellar Nb2O5 using a thermal-reduction promoted phase-transition process.
- Subjects
LEWIS pairs (Chemistry); LEWIS bases; BASE pairs; LEWIS acids; OXIDATIVE coupling; PRECIOUS metals; METHANE as fuel; METHANE
- Publication
Nature Communications, 2023, Vol 14, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-023-37663-x