Nanowrinkled Carbon Aerogels Embedded with FeNx Sites as Effective Oxygen Electrodes for Rechargeable Zinc-Air Battery
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,
Yuan Ping,
Yi Zhang,
Shaowei Chen
Affiliations
Ting He
State Key Laboratory for Powder Metallurgy, College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China; Department of Chemistry and Biochemistry, University of California, 1156 High Street, Santa Cruz, California 95064, USA
Bingzhang Lu
Department of Chemistry and Biochemistry, University of California, 1156 High Street, Santa Cruz, California 95064, USA
Yang Chen
State Key Laboratory for Powder Metallurgy, College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China
Yong Wang
State Key Laboratory for Powder Metallurgy, College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China
Yaqiang Zhang
Department of Chemical and Materials Engineering, University of Alberta, Edmonton, Alberta, Canada
John L. Davenport
Department of Physics, University of California, 1156 High Street, Santa Cruz, California 95064, USA
Alan P. Chen
Department of Physics, University of California, 1156 High Street, Santa Cruz, California 95064, USA
Chih-Wen Pao
X-Ray Absorption Group, National Synchrotron Radiation Research Center, Hsinchu 30076, Taiwan
Min Liu
Institute of Super-Microstructure and Ultrafast Process in Advanced Materials, School of Physics and Electronics, Central South University, Changsha 410083, China
Zhifang Sun
State Key Laboratory for Powder Metallurgy, College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China
Alexander Stram
Department of Physics, University of California, 1156 High Street, Santa Cruz, California 95064, USA
Alexander Mordaunt
Department of Physics, University of California, 1156 High Street, Santa Cruz, California 95064, USA
Jairo Velasco
Department of Physics, University of California, 1156 High Street, Santa Cruz, California 95064, USA
Yuan Ping
Department of Chemistry and Biochemistry, University of California, 1156 High Street, Santa Cruz, California 95064, USA
Yi Zhang
State Key Laboratory for Powder Metallurgy, College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China; Key Laboratory of Materials Processing and Mold (Zhengzhou University), Ministry of Education, Zhengzhou 450002, China
Shaowei Chen
Department of Chemistry and Biochemistry, University of California, 1156 High Street, Santa Cruz, California 95064, USA
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 batteries. In this study, biomass hydrogel reactors are utilized as structural templates to prepare carbon aerogels embedded with single iron atoms by controlled pyrolysis. The 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 FeN4, with a minor fraction (ca. 1/5) in the form of FeN3C. First-principles calculations show that the FeNx 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 counterparts. The 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 RuO2 catalysts. Results 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.
