High-density frustrated Lewis pairs based on Lamellar Nb2O5 for photocatalytic non-oxidative methane coupling

Ziyu Chen, Yutao Ye, Xiaoyi Feng, Yan Wang, Xiaowei Han, Yu Zhu, Shiqun Wu, Senyao Wang, Wenda Yang, Lingzhi Wang () and Jinlong Zhang ()
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Ziyu Chen: East China University of Science & Technology
Yutao Ye: East China University of Science & Technology
Xiaoyi Feng: East China University of Science & Technology
Yan Wang: East China University of Science & Technology
Xiaowei Han: East China University of Science & Technology
Yu Zhu: East China University of Science & Technology
Shiqun Wu: East China University of Science & Technology
Senyao Wang: East China University of Science & Technology
Wenda Yang: East China University of Science & Technology
Lingzhi Wang: East China University of Science & Technology
Jinlong Zhang: East China University of Science & Technology

Nature Communications, 2023, vol. 14, issue 1, 1-12

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-37663-x

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