Oxygen Functional Group Modification of Cellulose-Derived Hard Carbon for Enhanced Sodium Ion Storage

Oxygen Functional Group Modification of Cellulose-Derived Hard Carbon for Enhanced Sodium Ion Storage
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纤维素衍生硬碳的氧官能团改性以增强钠离子存储

DOI:
10.1021/acssuschemeng.9b04676
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发表时间:
2019-10
影响因子:
8.4
通讯作者:
Zhao Guangbo
Zhao Guangbo
中科院分区:
化学1区
文献类型:
--
作者:
Wang Hua;Sun Fei;Qu Zhibin;Wang Kunfang;Wang Lijie;Pi Xinxin;Gao Jihui;Zhao Guangbo

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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-H₂ 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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