Single-Atom Fe Catalysts for Fenton-Like Reactions: Roles of Different N Species

Yu Xiong; Hongchao Li; Chuangwei Liu; Lirong Zheng; Chen Liu; Jia-Ou Wang; Shoujie Liu; Yunhu Han; Lin Gu; Jieshu Qian; Dingsheng Wang

doi:10.1002/adma.202110653

Single-Atom Fe Catalysts for Fenton-Like Reactions: Roles of Different N Species

Adv Mater. 2022 Apr;34(17):e2110653. doi: 10.1002/adma.202110653. Epub 2022 Mar 26.

Authors

Yu Xiong^{1

2}, Hongchao Li³, Chuangwei Liu⁴, Lirong Zheng⁵, Chen Liu⁵, Jia-Ou Wang⁵, Shoujie Liu⁶, Yunhu Han⁷, Lin Gu⁸, Jieshu Qian³, Dingsheng Wang²

Affiliations

¹ Department of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, China.
² Department of Chemistry, Tsinghua University, Beijing, 100084, China.
³ School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing, 210094, China.
⁴ Key Lab for Anisotropy and Texture of Materials, School of Materials Science and Engineering, Northeastern University, Shenyang, 110819, China.
⁵ Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, China.
⁶ Chemistry and Chemical Engineering of Guangdong Laboratory, Shantou, 515063, China.
⁷ Institute of Flexible Electronics, Northwestern Polytechnical University, Xi'an, 710072, China.
⁸ Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, China.

PMID: 35263466
DOI: 10.1002/adma.202110653

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.

Keywords: Fenton-like reactions; heterogeneous catalysts; nitrogen species; single Fe atoms.

Abstract

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