Defect-rich N/S-Co-doped Porous Hollow Carbon Nanospheres Derived from Fullerenes as Efficient Electrocatalysts for Oxygen Reduction Reaction and Zn-air Batteries
Zhimin He, Peng Wei, Ting Xu, Jiantao Han, Xuejiao Gao* and Xing Lu*
Materials Chemistry Frontiers，2021.
https://doi.org/10.1039/D1QM00854D
Abstract
The rational design of the electronic properties and geometric structure of the carbon matrix is aneffective strategy to develop high-performance carbon-based electrocatalysts toward the oxygenreduction reaction (ORR). Herein, hollow carbon nanospheres are synthesized using fullerene (C60) andethylenediamine, which then form nitrogen and sulfur co-doped porous hollow carbon nanospheres(N,S-PHCNSs) via direct pyrolysis in the presence of sulfur. The decomposition of fullerenes providescarbon matrix defects, and the use of sulfur effectively modifies the contents and the configurations ofthe N species in the N,S-PHCNSs along with successful sulfur doping. The optimal N,S-PHCNSs exhibitan excellent ORR performance that is comparable to commercial Pt/C, which is further confirmed byZn–air batteries. Theoretical calculations suggest that graphitic-N and thiophene-S co-doped pentagondefects can greatly elevate the ORR activity. This work not only presents a facile and effective strategyto regulate the electronic properties of the carbon matrix but also provides useful guidance for therational design of advanced carbon-based electrocatalysts.
