期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 62, 期 5, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202212335
关键词
Diode Rectification; Oxygen Reduction Reaction; Single-Atom Catalysis; Two-Dimensional Metal Chalcogenide; p-n Junction
This study successfully surpasses the activity limit of single-atom catalysts (SACs) by utilizing n-type semiconductor supports for p-type SACs and discovers that the activity of supported SACs can be continuously tuned through rectification strategy.
Fine-tuning single-atom catalysts (SACs) to surpass their activity limit remains challenging at their atomic scale. Herein, we exploit p-type semiconducting character of SACs having a metal center coordinated to nitrogen donors (MeNx) and rectify their local charge density by an n-type semiconductor support. With iron phthalocyanine (FePc) as a model SAC, introducing an n-type gallium monosulfide that features a low work function generates a space-charged region across the junction interface, and causes distortion of the FeN4 moiety and spin-state transition in the Fe-II center. This catalyst shows an over two-fold higher specific oxygen-reduction activity than that of pristine FePc. We further employ three other n-type metal chalcogenides of varying work function as supports, and discover a linear correlation between the activities of the supported FeN4 and the rectification degrees, which clearly indicates that SACs can be continuously tuned by this rectification strategy.
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