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Asymmetric Electron Redistribution in Niobic-Oxygen Vacancy Associates to Tune Non-Covalent Interaction in CO 2 Photoreduction.

Jun DiChao ChenYao WuHao ChenJun XiongRan LongShuzhou LiLi SongWei JiangZheng Liu
Published in: Advanced materials (Deerfield Beach, Fla.) (2024)
The role of vacancy associates in photocatalytic CO 2 reduction is an open question. Herein, the Nb-O vacancy associates (V Nb-O ) are engineered into niobic acid (NA) atomic layers to tailor the CO 2 photoreduction performance. The intrinsic charge compensation from O to Nb around Nb-O vacancy associates could manipulate the active electronic states, leading to the asymmetric electron redistribution. This local symmetry breaking sites will show a charge density gradient, forming a localized polarization field to polarize non-polar CO 2 molecules and tune the non-covalent interaction of reaction intermediates. This unique configuration contributed to the 9.3 times increased activity for photocatalytic CO 2 reduction. Meantime, this V Nb-O NA also show excellent photocatalytic activity for NO 3 - -NH 4 + synthesis, with NH 4 + formation rate up to 3442 µmol g -1 h -1 . This work supplies fresh insights into the vacancy associates design for electron redistribution and non-covalent interaction tuning in photocatalysis. This article is protected by copyright. All rights reserved.
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