Great Enhancement of Carbon Energy Storage through Narrow Pores and Hydrogen-Containing Functional Groups for Aqueous Zn-Ion Hybrid Supercapacitor

The proton transfer mechanism on the carbon cathode surface has been considered as an effective way to boost the electrochemical performance of Zn-ion hybrid supercapacitors (SCs) with both ionic liquid and organic electrolytes. However, cheaper, potentially safer, and more environmental friendly supercapacitor can be achieved by using aqueous electrolyte. Herein, we introduce the proton transfer mechanism into a Zn-ion hybrid supercapacitor with the ZnSO(4) aqueous electrolyte and functionalized activated carbon cathode materials (FACs). We reveal both experimentally and theoretically an enhanced performance by controlling the micropores structure and hydrogen-containing functional groups (–OH and –NH functions) of the activated carbon materials. The Zn-ion SCs with FACs exhibit a high capacitance of 435 F g(−1) and good stability with 89% capacity retention over 10,000 cycles. Moreover, the proton transfer effect can be further enhanced by introducing extra hydrogen ions in the electrolyte with low pH value. The highest capacitance of 544 F g(−1) is obtained at pH = 3. The proton transfer process tends to take place preferentially on the hydroxyl-groups based on the density functional theory (DFT) calculation. The results would help to develop carbon materials for cheaper and safer Zn-ion hybrid SCs with higher energy.