In:
Angewandte Chemie, Wiley, Vol. 135, No. 5 ( 2023-01-26)
Abstract:
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 (MeN x ) 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 FeN 4 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 FeN 4 and the rectification degrees, which clearly indicates that SACs can be continuously tuned by this rectification strategy.
Type of Medium:
Online Resource
ISSN:
0044-8249
,
1521-3757
DOI:
10.1002/ange.202212335
Language:
English
Publisher:
Wiley
Publication Date:
2023
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