| 摘要： |
The applications of the most promising Fe—N–C
catalysts are prohibited by their limited intrinsic activities.
Manipulating the Fe energy level through anchoring electron-
withdrawing ligands is found effective in boosting the catalytic
performance. However, such regulation remains elusive as the
ligands are only uncontrollably introduced oweing to their
energetically unstable nature. Herein, we report a rational
manipulation strategy for introducing axial bonded O to the Fe
sites, attained through hexa-coordinating Fe with oxygen
functional groups in the precursor. Moreover, the O modifier
is stabilized by forming the Fe @ O @ Fe bridge bond, with the
approximation of two FeN 4 sites. The energy level modulation
thus created confers the sites with an intrinsic activity that is
over 10 times higher than that of the normal FeN 4 site. Our
finding opens a novel strategy to manage coordination
environments at an atomic level for high activity ORR
catalysts. |
