Defect and pyridinic nitrogen engineering of carbon-based metal-free nanomaterial toward oxygen reduction

• Published in: Nano energy 2018-10, Vol.52, p.307-314
• Main Authors: Zhang, Jian, Sun, Yuanmiao, Zhu, Jiawei, Kou, Zongkui, Hu, Pei, Liu, Lei, Li, Shuzhou, Mu, Shichun, Huang, Yunhui
• Format: Article
• Language: English
• Subjects: Electrocatalysts; Graphene; Graphene-like nanocarbon; Oxygen reduction; Zn–air batteries
• ISSN: 2211-2855
• DOI: 10.1016/j.nanoen.2018.08.003

Defect and N-activated electronic engineering are of paramount importance for developing highly active carbon-based electrocatalysts toward oxygen reduction reaction (ORR) because the binding affinity of the carbon matrix can be efficiently tuned and thus promote the electrocatalytic activity. Herein, we present a facile and general strategy for fabricating pyridinic-N dominated and defect-enriched graphene-like nanocarbon material (ND-GLC) involving in-situ alkaline activation of cellulose and ammonia injection. The ND-GLC material has a superior and enhanced ORR activity and stability compared to commercial Pt/C catalyst in both rotating disk electrode measurements and Zn-air battery applications. Experimental and theoretical studies describe that the high electrocatalytic activity of ND-GLC mainly originates from the synergetic effect of edges/defects and pyridinic-N dopants. Importantly, our concept is demonstrated to be universal for other carbon-based nanomaterials (i.e., graphite nanoplates, carbon nanotubes, carbon nanospheres, graphene nanosheets). [Display omitted] •Pyridinic-N and defect-enriched graphene-like carbon (ND-GLC) was fabricated.•The ND-GLC catalyst shows an excellent ORR performance compared to Pt/C catalyst.•DFT reveals that the defects and pyridinic-N can synergistically boost ORR activity.•A general strategy for the development of high efficient carbon-based electrocatalysis.