Impact Factor:30.849
DOI number:10.1002/adma.202110653
Affiliation of Author(s):中南大学
Journal:Advanced Materials
Abstract: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.
Indexed by:Journal paper
Document Code:202110653
Discipline:Natural Science
First-Level Discipline:Chemistry
Document Type:J
ISSN No.:0935-9648
Translation or Not:no
Included Journals:SCI
Links to published journals:https://onlinelibrary.wiley.com/doi/10.1002/adma.202110653