期刊
ENERGY & ENVIRONMENTAL MATERIALS
卷 6, 期 2, 页码 -出版社
WILEY
DOI: 10.1002/eem2.12346
关键词
oxygen reduction reaction; singe atom catalyst; stability; surface molecular engineering
This study developed a surface molecular engineering strategy using beta-cyclodextrins (CDs) as a localized molecular encapsulation to improve the stability of single-atom iron catalysts (Fe-SACs). The modified catalyst exhibited enhanced activity and long-term stability for the oxygen reduction reaction (ORR). The modification of beta-CDs regulated the atomic Fe coordination chemistry and acted as a protective barrier against poisoning molecules, leading to improved ORR activity and stability for Fe-SACs.
Fe single-atom catalysts (Fe-SACs) have been extensively studied as a highly efficient electrocatalyst toward the oxygen reduction reaction (ORR). Nonetheless, they suffer from stability issue induced by dissolution of Fe metal center and the OH- blocking. Herein, a surface molecular engineering strategy is developed by using beta-cyclodextrins (CDs) as a localized molecular encapsulation. The CD-modified Fe-SAC (Fe-SNC-beta-CD) shows obviously improved activity toward the ORR with 0.90 V, 4.10 and 4.09 mA cm(-2) for E-1/2, J(0) and J(k0.9), respectively. Meanwhile, the Fe-SNC-beta-CD shows the excellent long-term stability against aggressive stress and the poisoning. It is confirmed through electrochemical investigation that modification of beta-CD can, on one hand, regulate the atomic Fe coordination chemistry through the interaction between the CD and FeNx moiety, while on the other mitigate the strong adsorption of OH- and function as protective barrier against the poisoning molecules leading to enhanced ORR activity and stability for the Fe-SACs. The molecular encapsulation strategy demonstrates the uniqueness of post-pyrolysis surface molecular engineering for the design of single-atom catalyst.
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