Journal
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
Volume 7, Issue 22, Pages 18554-18565Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.9b04676
Keywords
cellulose; hard carbon; oxygen functional group; mechanochemistry; sodium-ion battery
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Funding
- National Natural Science Foundation of China [51806050]
- Fundamental Research Funds for the Central Universities of Harbin Institute of Technology
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Oxygen-containing groups in carbon materials have been demonstrated to be effective in the anodic sodium-ion storage process; however, the effect of specific oxygen-containing groups on the sodium-ion storage in the carbon framework remains to be explored. Based on a mechanochemical process (exemplified by ball milling in the presence of dry ice), a selectively modified cellulose-derived hard carbon (BHC-CO2) with a high oxygen content of 19.33 at. % and carboxyl-dominant groups was prepared in this work. The fabricated BHC-CO2 anode exhibits excellent electrochemical performance with a high reversible capacity of 293.5 mA h g(-1) at a current density of 0.05 A g(-1), two times as high as that of the oxygen-deficient BHC-CO2-H-2 anode, demonstrating the significant role of oxygen-containing groups in enhancing the Na+ storage. Moreover, the BHC-CO2 anode has an excellent high-rate cycling stability with a specific capacity of 80.0 mA h g(-1) even after 2000 cycles at 1 A g(-1). Qualitative analyses of capacitive effect combined with density functional theory calculations further reveal that carboxyl groups introduced by the mechanochemical process facilitate Na+ adsorption on the carbon surface, enhancing the capacitive Na+ storage process and thus greatly improving the capacity. This work demonstrates the role of carboxyl on Na+ storage by carbonaceous materials and provides theoretical guidance for the oxygen functional group modification of carbon materials to enhance the sodium-ion storage.
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