Journal
ADVANCED MATERIALS
Volume 34, Issue 17, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202110653
Keywords
Fenton-like reactions; heterogeneous catalysts; nitrogen species; single Fe atoms
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Funding
- National Natural Science Foundation of China [21871159, 22171157]
- Natural Science Foundation of Jiangsu Province [BK20211522]
- Science and Technology Key Project of Guangdong Province of China [2020B010188002]
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Recognizing and controlling the structure-activity relationships of single-atom catalysts is crucial for manipulating their catalytic properties. The study on Fe single-atom catalysts supported on nitrogen-doped carbon reveals high catalytic reactivity, stability, and wide pH suitability in Fenton-like reactions, with the roles of different N species further explored both experimentally and theoretically. Density functional theory calculations highlight how the location of d-band center of Fe sites affects the generation of Fe-oxo intermediates, leading to excellent catalytic properties.
Recognizing and controlling the structure-activity relationships of single-atom catalysts (SACs) is vital for manipulating their catalytic properties for various practical applications. Herein, Fe SACs supported on nitrogen-doped carbon (SA-Fe/CN) are reported, which show high catalytic reactivity (97% degradation of bisphenol A in only 5 min), high stability (80% of reactivity maintained after five runs), and wide pH suitability (working pH range 3-11) toward Fenton-like reactions. The roles of different N species in these reactions are further explored, both experimentally and theoretically. It is discovered that graphitic N is an adsorptive site for the target molecule, pyrrolic N coordinates with Fe(III) and plays a dominant role in the reaction, and pyridinic N, coordinated with Fe(II), is only a minor contributor to the reactivity of SA-Fe/CN. Density functional theory (DFT) calculations reveal that a lower d-band center location of pyrrolic-type Fe sites leads to the easy generation of Fe-oxo intermediates, and thus, excellent catalytic properties.
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