期刊
CHEMICAL ENGINEERING JOURNAL
卷 429, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.132214
关键词
Ordered macropore; Nanoporous carbon; Fe-N-x; Sulfur doping; Oxygen reduction reaction
资金
- Shanghai Pujiang Program [19PJ1402500]
- National Natural Science Foundation of China [22005099]
The optimized catalyst Fe-N-x/HPC-1000, with atomically dispersed Fe-N-x sites, shows excellent oxygen reduction reaction performance. Secondary sulfur-doping enhances the properties of the catalyst, making it more favorable for the ORR.
The electrocatalytic performance of carbon-based materials determined by the active sites' density, accessibility, and utilization rate. In this work, ordered macroporous Fe-containing zeolitic-imidazole frameworks (Fe-ZIF) single-crystalline was carefully synthesized by confined growing Fe-ZIF in the interior space of closely-packed polystyrene sphere template. Then ordered macro-microporous carbon with atomically dispersed Fe-N-x sites (Fe-N-x/HPC) were successfully fabricated by direct carbonizing the ordered macroporous Fe-ZIF. The optimized catalyst Fe-N-x/HPC-1000 shows a high specific surface area of 1293 m(2).g(-1), a nitrogen and iron doping of 3.4 and 0.12 at.%, respectively. Thanks to the open and hierarchically porous structure, high specific surface area, and rich Fe-N-x moieties, Fe-N-x/HPC-1000 demonstrates outstanding oxygen reduction reaction (ORR) performance with an onset potential of 0.97 V, a half-wave potential of 0.881 V, and excellent durability. Secondary sulfur-doping was carried out to modify the properties of Fe-N-x/HPC-1000, which is favorable for ORR. These findings provide new insight into producing atomically dispersed Fe-N-x- and sulfur-modified MOF-derived ordered macroporous carbon electrocatalyst.
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