Dense binary Fe–Cu sites promoting CO 2 utilization enable highly reversible hybrid Na–CO 2 batteries

• Published in: Journal of materials chemistry. A, Materials for energy and sustainability Materials for energy and sustainability, 2021-10, Vol.9 (38), p.22114-22128
• Main Authors: Xu, Changfan, Zhan, Jing, Wang, Huanwei, Kang, Yao, Liang, Feng
• Format: Article
• Language: English
• ISSN: 2050-7488; 2050-7496
• DOI: 10.1039/D1TA06611K

High-performance and low-cost catalysts are particularly desirable for the exploitation of practical low-overpotential Na–CO 2 batteries with protracted cyclability. Herein, a well-defined morphology of nitrogen-rich graphitic carbon frameworks with dense bimetallic active sites (Fe–Cu–N–C) was facilely prepared by introducing Fe 3+ and Cu 2+ to regulate in situ grown carbon nanotubes as an advanced catalyst toward hybrid Na–CO 2 batteries. Through metal content tuning and carbon architecture altering, Fe–Cu–N–C proved to be dramatically more effective than Cu–N–C and Fe–N–C. As the cathodic catalyst of a hybrid Na–CO 2 battery, Fe–Cu–N–C can facilitate the fast evolution and degradation of flocculent discharge products and achieve an excellent long-term cyclability with up to 1550 cycles (over 600 h), which makes it one of the greatest catalysts for hybrid Na–CO 2 /air batteries that have been reported to date. The observed outstanding battery performance is attributable to the cross-linked conductive framework affording a “highway” for accelerated electron transport and Na + /CO 2 diffusion. Besides, the synergistic effects among defect-rich interfaces, Fe/Fe 3 C nanocrystals, and Fe–N x and Cu–N x sites derived from nitrogen atom doping enhance the catalytic activity. In addition, the possible growth and decomposition mechanisms of NaHCO 3 products with different morphologies on Fe–N–C, Cu–N–C, and Fe–Cu–N–C electrodes were presented and discussed.