The ion storage mechanism and ion concentration play crucial roles in determining the electrochemical energy storage performances of multi-ion-based batteries and/or capacitors. Here, we take δ-MnO2-A2SO4 (A = Li, Na, K) as an example system to explore the physical and chemical mechanisms related to electrochemical energy storage using experimental analysis and first-principles calculations. Among the studied systems, superior capacitance performance is found in δ-MnO2-Li2SO4 due to excellent mobility (migration barrier 0.168 eV) of lithium ions. Better cycling stability appears in δ-MnO2-K2SO4, which is attributed to larger adsorption energy (−0.655 eV) between potassium ions and δ-MnO2. Moreover, compared with a pure Li2SO4 electrolyte, our calculations suggest that incorporation of moderate Na2SO4 or K2SO4 into the Li2SO4 electrolyte could considerably elongate the cycling lifetime. Overdose of Na+ or K+ is, however, adverse to the capacitance performance as verified by our experiments. We argue that the dominance role of Na+ or K+ ions played in the hybrid electrolyte originates from the larger formation enthalpy and adsorption energy of Na+ or K+ when reacting with δ-MnO2 compared with those of Li+. Our findings suggest that understanding of the ion storage mechanism can provide useful clues for searching the proper ion concentration ratio, which takes advantages of individual ions in multi-ion-based δ-MnO2 electrochemical energy storage devices.
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18 October 2021
Research Article|
October 19 2021
Ion storage mechanism of δ-MnO2 as supercapacitor cathode in multi-ion aqueous electrolyte: Experimental and theoretical analysis
Jing Wan;
Jing Wan
1
Department of Applied Physics, Chongqing University
, Chongqing 400044, People's Republic of China
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Xiao Gu;
Xiao Gu
2
School of Physical Science and Technology, Ningbo University
, Ningbo 315000, People's Republic of China
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Peiyuan Ji;
Peiyuan Ji
1
Department of Applied Physics, Chongqing University
, Chongqing 400044, People's Republic of China
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Jien Li;
Jien Li
1
Department of Applied Physics, Chongqing University
, Chongqing 400044, People's Republic of China
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Junlin Lu;
Junlin Lu
1
Department of Applied Physics, Chongqing University
, Chongqing 400044, People's Republic of China
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Shuang Luo;
Shuang Luo
1
Department of Applied Physics, Chongqing University
, Chongqing 400044, People's Republic of China
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Bangxing Li;
Bangxing Li
1
Department of Applied Physics, Chongqing University
, Chongqing 400044, People's Republic of China
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Li Huang
;
Li Huang
3
Guangdong Provincial Key Laboratory of Energy Materials for Electric Power, Southern University of Science and Technology
, Shenzhen 518055, China
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Mingquan He
;
Mingquan He
a)
1
Department of Applied Physics, Chongqing University
, Chongqing 400044, People's Republic of China
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Chenguo Hu
Chenguo Hu
a)
1
Department of Applied Physics, Chongqing University
, Chongqing 400044, People's Republic of China
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Appl. Phys. Lett. 119, 163901 (2021)
Article history
Received:
June 09 2021
Accepted:
October 05 2021
Citation
Jing Wan, Xiao Gu, Peiyuan Ji, Jien Li, Junlin Lu, Shuang Luo, Bangxing Li, Li Huang, Mingquan He, Chenguo Hu; Ion storage mechanism of δ-MnO2 as supercapacitor cathode in multi-ion aqueous electrolyte: Experimental and theoretical analysis. Appl. Phys. Lett. 18 October 2021; 119 (16): 163901. https://doi.org/10.1063/5.0059392
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