A versatile transition metal ion-binding motif derived from covalent organic framework for efficient CO2 electroreduction

Autor: Haijin Zhu, Gordon G. Wallace, Long Hao, Jing Ning, Amruthalakshmi Vijayakumar, Yong Zhao, Caiyun Wang
Rok vydání: 2021
Předmět:
Zdroj: Applied Catalysis B: Environmental. 291:119915
ISSN: 0926-3373
DOI: 10.1016/j.apcatb.2021.119915
Popis: We demonstrate a versatile transition metal ion-binding motif for constructing highly efficient metal atom-embedded carbon catalysts for electrochemical CO production. It is a mesoporous N-doped carbon (N-C) derived from a covalent organic framework via molten-salt assisted carbonization. Three different transition metals (Co, Fe or Ni) have been immobilized into the N-rich mesopores via ion coordination, forming catalysts with isolated and coordinately unsaturated metal-N moieties. These catalysts all exhibit excellent electrocatalytic activities for CO2-to-CO conversion with a high faradaic efficiency > 80 % and a high current density > 10 mA cm−2 at modest overpotentials around 500 mV. Using Ni- or Fe-N-C, a highly selective (> 95 %) CO generation was observed. By performing the structure-property analysis with three other N-C materials as control, such high performance is ascribed to the efficient metal-N catalytic sites generated by the cooperative immobilization of metal atoms with pyridinic-N and pyrrolic-N species in the mesoporous carbon matrix.
Databáze: OpenAIRE