TY  - JOUR
AU  - Liu, Fan
AU  - Yan, Ning
AU  - Zhu, Guangqi
AU  - Liu, Zigeng
AU  - Ma, Shenqian
AU  - Xiang, Guolei
AU  - Wang, Songrui
AU  - Liu, Xingjiang
AU  - Wang, Wei
TI  - Fe–N–C single-atom catalysts with an axial structure prepared by a new design and synthesis method for ORR
JO  - New journal of chemistry
VL  - 45
IS  - 29
SN  - 0398-9836
CY  - London
PB  - RSC
M1  - FZJ-2021-05744
SP  - 13004 - 13014
PY  - 2021
AB  - Fe–N–C single-atom catalysts usually exhibit poor ORR activity due to their unsatisfactory O2 adsorption and activation. Here, a new design idea and tailored self-assembly synthesis method are reported to improve their ORR performance. DFT calculations indicate that the ORR electrocatalytic activity of Fe–N–C single-atom catalysts with an axial structure is superior to that of Fe–N–C single-atom catalysts with a Fe–N4 active site. In order to experimentally demonstrate the difference, Fe–N–C single-atom catalysts with a Fe–N5 active site were successfully synthesized on the surface of monolayer graphene. XANES, SEM, HRTEM, XRD, Raman and XPS analyses indicate that the synthesized Fe–N–C catalyst possessed nanofibre morphology and a curved layer-like crystal structure. For comparison, FePc powder was used as the FePc(Fe–N4) catalyst as its molecular structure involves a Fe–N4 active site embedded in carbon six-membered rings. The current density of the synthesized Fe–N5/C@G catalyst at a potential of 0.88 V vs. RHE is 1.65 mA cm−2, which is much higher than that of the FePc(Fe–N4) catalyst (1.04 mA cm−2) and even higher than that of commercial Pt/C catalyst (1.54 mA cm−2). The results are very well consistent with the DFT calculations, verifying the dependability and accuracy of DFT calculations. This work reports a new synthetic idea to obtain better performance and proposes a formation mechanism to explain the process of the synthesis method.
LB  - PUB:(DE-HGF)16
UR  - <Go to ISI:>//WOS:000669874900001
DO  - DOI:10.1039/D1NJ01380G
UR  - https://juser.fz-juelich.de/record/904174
ER  -