TY - JOUR
T1 - A versatile transition metal ion-binding motif derived from covalent organic framework for efficient CO2 electroreduction
AU - Zhao, Yong
AU - Hao, Long
AU - Ning, Jing
AU - Zhu, Haijin
AU - Vijayakumar, Amruthalakshmi
AU - Wang, Caiyun
AU - Wallace, Gordon G.
N1 - Publisher Copyright:
© 2021 Elsevier B.V.
PY - 2021/8/15
Y1 - 2021/8/15
N2 - 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.
AB - 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.
KW - COreduction
KW - Covalent organic framework
KW - Electrocatalysis
KW - Metal ion coordination
KW - Metal-binding motif
UR - http://www.scopus.com/inward/record.url?scp=85103560854&partnerID=8YFLogxK
U2 - 10.1016/j.apcatb.2021.119915
DO - 10.1016/j.apcatb.2021.119915
M3 - 文章
AN - SCOPUS:85103560854
SN - 0926-3373
VL - 291
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
M1 - 119915
ER -