In this study,we selected 10 Co-based double-atom catalysts(DACs)catalysts,namely CoMN_(6)-gra(OH)(M?Sc,Ti,V,Cr,Mn,Fe,Co,Ni,Cu,Zn),and investigated their oxygen reduction reactions(ORR)catalytic performances with/with...In this study,we selected 10 Co-based double-atom catalysts(DACs)catalysts,namely CoMN_(6)-gra(OH)(M?Sc,Ti,V,Cr,Mn,Fe,Co,Ni,Cu,Zn),and investigated their oxygen reduction reactions(ORR)catalytic performances with/without considering the magnetic coupling by means of density functional theory(DFT)calculations.It was found that CoNiN_(6)-gra(OH),CoCuN_(6)-gra(OH),and CoZnN_(6)-gra(OH)exhibit good catalytic activity of ORR(with low overpotentials of 0.33,0.34 and 0.23 V,respectively)when the magnetic coupling is considered.In particular,magnetic changes in CoMN_(6)-gra(OH)candidates play a vital role in their ORR catalytic activity.Interestingly,the d-band center can be utilized to well rationalize the ORR catalytic activity.This work highlights the importance of considering the magnetic coupling to well predict the activity of ORR catalysts,and discloses that the manipulation of the magnetic coupling between transition metal atoms is an emerging and powerful approach for the development of high-performance electrocatalysts for ORR and other related reactions.展开更多
基金financially supported in China by the National Natural Science Foundation of China(Grant Nos.11704203,11964024)the“Grassland Talents”project of Inner Mongolia Autonomous Region,China(Grant No.12000–12102613)+1 种基金the Young Science and Technology Talents Cultivation Project of Inner Mongolia University,China(21221505)the computational support from PARATEAR,and in USA by the National Science Foundation-Centers of Research Excellence in Science and Technology(NSF-CREST Center)for Innovation,Research and Education in Environmental Nanotechnology(CIRE2N)(Grant No.HRD-1736093).
文摘In this study,we selected 10 Co-based double-atom catalysts(DACs)catalysts,namely CoMN_(6)-gra(OH)(M?Sc,Ti,V,Cr,Mn,Fe,Co,Ni,Cu,Zn),and investigated their oxygen reduction reactions(ORR)catalytic performances with/without considering the magnetic coupling by means of density functional theory(DFT)calculations.It was found that CoNiN_(6)-gra(OH),CoCuN_(6)-gra(OH),and CoZnN_(6)-gra(OH)exhibit good catalytic activity of ORR(with low overpotentials of 0.33,0.34 and 0.23 V,respectively)when the magnetic coupling is considered.In particular,magnetic changes in CoMN_(6)-gra(OH)candidates play a vital role in their ORR catalytic activity.Interestingly,the d-band center can be utilized to well rationalize the ORR catalytic activity.This work highlights the importance of considering the magnetic coupling to well predict the activity of ORR catalysts,and discloses that the manipulation of the magnetic coupling between transition metal atoms is an emerging and powerful approach for the development of high-performance electrocatalysts for ORR and other related reactions.
基金supported by the National Natural Science Foundation of China (11828401, 11964024 and 12364038)the “Grassland Talents” Project of the Inner Mongolia Autonomous Region (12000-12102613)the Young Science and Technology Talents Cultivation Project of Inner Mongolia University (21200-5223708)。
