Resolving the Dilemma of Fe–N–C Catalysts by the Selective Synthesis of Tetrapyrrolic Active Sites via an Imprinting Strategy

• DOI: 10.1021/jacs.1c04884
• Publication Date: 2021-10-24T12:00:45Z
• Authors: Davide Menga; Jian Liang Low; Yan-Sheng Li; Iztok Arčon; Burak Koyutürk; Friedrich Wagner; Francisco Ruiz-Ze...; Miran Gaberšček; Beate Paulus; Tim-Patrick Felli...
• Keywords: EXAFS; selective synthesis; info:eu-repo/classification/udc/54; Fe-N-C catalysts; tetrapyrrolic active sites; single atom; DFT; 01 natural sciences; 7. Clean energy; XANES; 0104 chemical sciences

Combining the abundance and inexpensiveness of their constituent elements with atomic dispersion, atomically dispersed Fe-N-C catalysts represent most promising alternative to precious-metal-based materials in proton exchange membrane (PEM) fuel cells. Due high temperatures involved synthesis sensitivity Fe ions toward carbothermal reduction, current synthetic methods are intrinsically limited type amount desired, catalytically active Fe-N4 sites, site densities have been out reach (dilemma catalysts). We herein identify a paradigm change arising from developments other M-N-C single-atom catalysts. Supported by DFT calculations we propose fundamental principles for materials. further exploit proposed novel strategy surpass dilemma The selective formation tetrapyrrolic Zn-N4 sites tailor-made Zn-N-C material is utilized as an active-site imprint preparation corresponding catalyst. By successive low- high-temperature ion reactions, obtain phase-pure catalyst, loading (>3 wt %). Moreover, catalyst entirely composed sites. density more than six times previously reported single-site cell