Isolated Fe Single Atomic Sites Anchored on Highly Steady Hollow Graphene Nanospheres as an Efficient Electrocatalyst for the Oxygen Reduction Reaction

Qiu, XY (Qiu, Xiaoyu)[ 1 ] ; Yan, XH (Yan, Xiaohong)[ 1 ] ; Pang, H (Pang, Huan)[ 2 ] ; Wang, JC (Wang, Jingchun)[ 1 ] ; Sun, DM (Sun, Dongmei)[ 1 ] ; Wei, SH (Wei, Shaohua)[ 1 ] ; Xu, L (Xu, Lin)[ 1 ]*（徐林）; Tang, YW (Tang, Yawen)[ 1 ]*（唐亚文）

[ 1 ] Nanjing Normal Univ, Jiangsu Key Lab New Power Batteries, Jiangsu Collaborat Innovat Ctr Biomed Funct Mat, Sch Chem & Mat Sci, Nanjing 210023, Jiangsu, Peoples R China

[ 2 ] Yangzhou Univ, Sch Chem & Chem Engn, Yangzhou 225009, Jiangsu, Peoples R China

ADVANCED SCIENCE，201901,6(2)

The rational design of economical and high-performance nanocatalysts to substitute Pt for the oxygen reduction reaction (ORR) is extremely desirable for the advancement of sustainable energy-conversion devices. Isolated single atom (ISA) catalysts have sparked tremendous interests in electrocatalysis due to their maximized atom utilization efficiency. Nevertheless, the fabrication of ISA catalysts remains a grand challenge. Here, a template-assisted approach is demonstrated to synthesize isolated Fe single atomic sites anchoring on graphene hollow nanospheres (denoted as Fe ISAs/GHSs) by using Fe phthalocyanine (FePc) as Fe precursor. The rigid planar macrocycle structure of FePc molecules and the steric-hindrance effect of graphene nanospheres are responsible for the dispersion of Fe-N-x species at an atomic level. The combination of atomically dispersed Fe active sites and highly steady hollow substrate affords the Fe ISAs/GHSs outstanding ORR performance with enhanced activity, long-term stability, and better tolerance to methanol, SO2, and NOx in alkaline medium, outperforming the state-of-the-art commercial Pt/C catalyst. This work highlights the great promises of cost-effective Fe-based ISA catalysts in electrocatalysis and provides a versatile strategy for the synthesis of other single metal atom catalysts with superior performance for diverse applications.

文章链接：

https://onlinelibrary.wiley.com/doi/full/10.1002/advs.201801103

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