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Nanowrinkled Carbon Aerogels Embedded with FeN_(x) Sites as Effective Oxygen Electrodes for Rechargeable Zinc-Air Battery

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Research 2019年第1期2019卷 1-13页

作者： Ting He Bingzhang Lu Yang Chen Yong Wang Yaqiang Zhang John L.Davenport Alan P.Chen Chih-Wen Pao Min Liu Zhifang Sun alexander Stram alexander mordaunt Jairo Velasco Jr Yuan Ping Yi Zhang Shaowei Chen State Key Laboratory for Powder Metallurgy College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083China Department of Chemistry and Biochemistry University of California1156 High StreetSanta CruzCalifornia 95064USA Department of Chemical and Materials Engineering University of AlbertaEdmontonAlbertaCanada T6G 1H9 Department of Physics University of California1156 High StreetSanta CruzCalifornia 95064USA X-Ray Absorption Group National Synchrotron Radiation Research CenterHsinchu 30076Taiwan Institute of Super-Microstructure and Ultrafast Process in Advanced Materials School of Physics and ElectronicsCentral South UniversityChangsha 410083China Key Laboratory of Materials Processing and Mold(Zhengzhou University) Ministry of EducationZhengzhou 450002China

Rational design of single-metal atom sites in carbon substrates by a flexible strategy is highly desired for the preparation of high-performance catalysts for metal-air *** this study,biomass hydrogel reactors are utilized as structural templates to prepare carbon aerogels embedded with single iron atoms by controlled *** tortuous and interlaced hydrogel chains lead to the formation of abundant nanowrinkles in the porous carbon aerogels,and single iron atoms are dispersed and stabilized within the defective carbon skeletons.X-ray absorption spectroscopy measurements indicate that the iron centers are mostly involved in the coordination structure of FeN_(4),with a minor fraction(ca.1/5)in the form of FeN_(3)***-principles calculations show that the FeN_(x) sites in the Stone-Wales configurations induced by the nanowrinkles of the hierarchically porous carbon aerogels show a much lower free energy than the normal *** resulting iron and nitrogen-codoped carbon aerogels exhibit excellent and reversible oxygen electrocatalytic activity,and can be used as bifunctional cathode catalysts in rechargeable Zn-air batteries,with a performance even better than that based on commercial Pt/C and RuO_(2) *** from this study highlight the significance of structural distortions of the metal sites in carbon matrices in the design and engineering of highly active single-atom catalysts.

关键词： Oxygen charge skeleton

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