Nanowrinkled Carbon Aerogels Embedded with FeNx Sites as Effective Oxygen Electrodes for Rechargeable Zinc-Air Battery
Abstract
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 FeN 4 , with a minor fraction (ca. 1/5) in the form of FeN 3 C. First-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 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 RuO 2 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.
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Jan 01, 2019
- Source ID
- 10.34133/2019/6813585
Entities
People
- Alan P. Chen
- Alexander Mordaunt
- Alexander Stram
- Bingzhang Lu
- Chen Yang
- Chih-Wen Pao
- Jairo Velasco
- John L Davenport
- Min Liu
- Shaowei Chen
- Ting He
- Yaqiang Zhang
- Yi Zhang
- Yong Wang
- Yuan Ping
- Zhifang Sun
Organizations
- Army Research Office
- Central South University
- China Scholarship Council
- National Natural Science Foundation of China
- National Science Foundation
- National Synchrotron Radiation Research Center
- University of Alberta
- University of California
- Zhengzhou University