J. Mater. Sci. Technol. ›› 2021, Vol. 67: 116-126.DOI: 10.1016/j.jmst.2020.06.028
• Research article • Previous Articles Next Articles
Bhavana Joshia,b, Edmund Samuela, Yong-il Kima, Govindasami Periyasamic, Mostafizur Rahamanc, Sam S. Yoona,*()
Received:
2020-03-31
Revised:
2020-06-05
Accepted:
2020-06-06
Published:
2021-03-20
Online:
2021-04-15
Contact:
Sam S. Yoon
About author:
* E-mail address: skyoon@korea.ac.kr (S.S. Yoon).1These authors contributed equally to this work.
Bhavana Joshi, Edmund Samuel, Yong-il Kim, Govindasami Periyasami, Mostafizur Rahaman, Sam S. Yoon. Bimetallic zeolitic imidazolate framework-derived substrate-free anode with superior cyclability for high-capacity lithium-ion batteries[J]. J. Mater. Sci. Technol., 2021, 67: 116-126.
ZIF derived Sample | ZnAc (mM) | CoNt (mM) | As-synthesized sample details |
---|---|---|---|
ZnO/C | 12.5 | 0 | ZIF8 |
ZnCoO/C (2:1) | 8.4 | 4.1 | ZIF8/ZIF67 (2:1) |
ZnCoO/C (1:1) | 6.25 | 6.25 | ZIF8/ZIF67 (1:1) |
ZnCoO/C (1:2) | 4.1 | 8.4 | ZIF8/ZIF67 (1:2) |
CoO/C | 0 | 12.5 | ZIF67 |
Table 1 ZIF-derived samples prepared with varying proportions of ZIF-8/ZIF-67.
ZIF derived Sample | ZnAc (mM) | CoNt (mM) | As-synthesized sample details |
---|---|---|---|
ZnO/C | 12.5 | 0 | ZIF8 |
ZnCoO/C (2:1) | 8.4 | 4.1 | ZIF8/ZIF67 (2:1) |
ZnCoO/C (1:1) | 6.25 | 6.25 | ZIF8/ZIF67 (1:1) |
ZnCoO/C (1:2) | 4.1 | 8.4 | ZIF8/ZIF67 (1:2) |
CoO/C | 0 | 12.5 | ZIF67 |
Fig. 1. Schematic of the experimental process for the fabrication of ZIF-8, ZIF-67, and ZIF-8/ZIF-67 loaded on PAN/2MI fibers, in the counterclockwise direction, respectively.
Parameters | Details |
---|---|
Battery tester | WBCS3000 battery cycler system (WonATech, Seoul, South Korea) |
Cell | CR 2032 Coin cell |
Working electrode | ZIF derived composite fibers |
Counter electrode | Li metal foil |
Electrolyte | 1-M LiPF6 dissolved in ethylene carbonate, dimethyl carbonate, and ethyl methyl carbonate (1:1:1) |
Separator | Celgard 2400 polymer |
Voltage range | 0.01-3 V at 25 °C |
Current rate | 100, 200, 500, 1000, 1200 mA·g-1 |
Table 2 Charge-discharge test conditions of coin cells.
Parameters | Details |
---|---|
Battery tester | WBCS3000 battery cycler system (WonATech, Seoul, South Korea) |
Cell | CR 2032 Coin cell |
Working electrode | ZIF derived composite fibers |
Counter electrode | Li metal foil |
Electrolyte | 1-M LiPF6 dissolved in ethylene carbonate, dimethyl carbonate, and ethyl methyl carbonate (1:1:1) |
Separator | Celgard 2400 polymer |
Voltage range | 0.01-3 V at 25 °C |
Current rate | 100, 200, 500, 1000, 1200 mA·g-1 |
Fig. 4. TEM image of the ZnCoO/C (2:1) sample at (a) low (100 nm) and (b) high magnification (50 nm) (inset shows 20 nm); (c) elemental maps of C, Co, and Zn.
Fig. 6. (a, c, and e) Discharge-charge profiles and (b, d, and f) variations in differential capacity for (a, b) ZnO/C, (c, d) ZnCoO/C (2:1), and (e, f) CoO/C after 1st, 2nd, and 300th cycles at a current density of 100 mA·g-1.
Fig. 7. Electrochemical analyses of samples: (a) rate capability; long-term cycling at (b) low current density (100 mA·g-1) and (c) high current density (1000 mA·g-1). Here, N represents the number of cycles and CE is the coulombic efficiency. Relative capacity retention at (d) low current density (100 mA·g-1) and (e) high current density (1000 mA·g-1). Here, the shaded and solid bars indicate the capacity retention at N = 1 and N = 2, respectively.
Anode material | Metal source | Ligand | Capacity [mA⋅h·g-1] (N) | Current Rate [mA·g-1] | Current collector/ binder | Refs. |
---|---|---|---|---|---|---|
Zinc cobalt oxide plates | Co(NO3)2·6H2O | 2MI | 1027 (100) | 100 | Cu foil/PVDF | [ |
ZnO@C | Zn(NO3)2·6H2O Co(NO3)2·6H2O | 2MI | 526 (500) | 250 | Cu foil/PVDF | [ |
721 (500) | 250 | |||||
Co3O4/C | ||||||
ZnCo2O4 | Zn(NO3)2·6H2O CoCl2.6H2O | Terephthalic acid | 890 (100) | 100 | Cu foil/ sodium carboxymethyl | [ |
Cellulose | ||||||
Co-Zn/N doped carbon polyhedral nanocages | Zn(NO3)2·6H2O | 2MI | 702 (400) | 200 | Cu foil/PVDF | [ |
CoCl2·6H2O | ||||||
CoNiFeP | Co(NO3)2·6H2O | 2MI | 512 (300) | 500 | Cu foil/ carboxymethyl | [ |
Cellulose | ||||||
NiCoP | Co(NO3)2·6H2O | 2MI | 104 (100) | 1000 | Cu foil/PVDF | [ |
Ni(NO3)2·6H2O | ||||||
Co8FeS8/N-C Dodecahedral nanocages | Co(NO3)2·6H2O | 2MI | 396 (400) | 500 | - | [ |
Iron(III) acetylacetonate | ||||||
Zn0.76Co0.24S@C@CNF | Co(NO3)2·6H2O | 2MI | 1113 (250) | 100 | Cu foil/PVDF | [ |
Zn(NO3)2·6H2O | ||||||
ZnCoS@Co9S8/NC | Co(NO3)2·6H2O | 2MI | 1813 (500) | 500 | Cu foil/PVDF | [ |
Zn(NO3)2·6H2O | ||||||
NiCo2S4 | Co(NO3)2·6H2O | 2MI | 770 (100) | 100 | Cu foil/PVDF | [ |
Ni(NO3)2·6H2O | ||||||
Co1-xS/ZnS@C | Co(NO3)2·6H2O | 2MI | 586 (100) | 300 | Cu foil/PVDF | [ |
Zn(NO3)2·6H2O | ||||||
Bimetallic ZIF derived | Zn(NO3)2·6H2O Co(NO3)2·6H2O | 2MI | 711 (500) | 1000 | Freestanding, flexible binder free | Present |
1048 (300) | 100 |
Table 3 Comparison of electrochemical performance of previously reported bimetallic ZIF-derived composite materials with those reported in this study.
Anode material | Metal source | Ligand | Capacity [mA⋅h·g-1] (N) | Current Rate [mA·g-1] | Current collector/ binder | Refs. |
---|---|---|---|---|---|---|
Zinc cobalt oxide plates | Co(NO3)2·6H2O | 2MI | 1027 (100) | 100 | Cu foil/PVDF | [ |
ZnO@C | Zn(NO3)2·6H2O Co(NO3)2·6H2O | 2MI | 526 (500) | 250 | Cu foil/PVDF | [ |
721 (500) | 250 | |||||
Co3O4/C | ||||||
ZnCo2O4 | Zn(NO3)2·6H2O CoCl2.6H2O | Terephthalic acid | 890 (100) | 100 | Cu foil/ sodium carboxymethyl | [ |
Cellulose | ||||||
Co-Zn/N doped carbon polyhedral nanocages | Zn(NO3)2·6H2O | 2MI | 702 (400) | 200 | Cu foil/PVDF | [ |
CoCl2·6H2O | ||||||
CoNiFeP | Co(NO3)2·6H2O | 2MI | 512 (300) | 500 | Cu foil/ carboxymethyl | [ |
Cellulose | ||||||
NiCoP | Co(NO3)2·6H2O | 2MI | 104 (100) | 1000 | Cu foil/PVDF | [ |
Ni(NO3)2·6H2O | ||||||
Co8FeS8/N-C Dodecahedral nanocages | Co(NO3)2·6H2O | 2MI | 396 (400) | 500 | - | [ |
Iron(III) acetylacetonate | ||||||
Zn0.76Co0.24S@C@CNF | Co(NO3)2·6H2O | 2MI | 1113 (250) | 100 | Cu foil/PVDF | [ |
Zn(NO3)2·6H2O | ||||||
ZnCoS@Co9S8/NC | Co(NO3)2·6H2O | 2MI | 1813 (500) | 500 | Cu foil/PVDF | [ |
Zn(NO3)2·6H2O | ||||||
NiCo2S4 | Co(NO3)2·6H2O | 2MI | 770 (100) | 100 | Cu foil/PVDF | [ |
Ni(NO3)2·6H2O | ||||||
Co1-xS/ZnS@C | Co(NO3)2·6H2O | 2MI | 586 (100) | 300 | Cu foil/PVDF | [ |
Zn(NO3)2·6H2O | ||||||
Bimetallic ZIF derived | Zn(NO3)2·6H2O Co(NO3)2·6H2O | 2MI | 711 (500) | 1000 | Freestanding, flexible binder free | Present |
1048 (300) | 100 |
Fig. 8. (a) Nyquist plots obtained from EIS for ZIF-derived bimetallic nanocage-decorated CNF electrodes (all samples). The inset shows the Randles equivalent circuit. (b) Z′ vs. the inverse square root of angular frequency in the Warburg diffusion tail region, used to calculate the Warburg coefficient (σw).
Sample | Rs | Rct |
---|---|---|
ZnO/C | 7.3 | 124.5 |
ZnCoO/C (2:1) | 3.6 | 197.6 |
ZnCoO/C (1:1) | 3.6 | 248.0 |
ZnCoO/C (1:2) | 3.4 | 348.7 |
CoO/C | 3.2 | 381.6 |
Table 4 Resistance of various samples, as deduced from the Randles equivalent circuit.
Sample | Rs | Rct |
---|---|---|
ZnO/C | 7.3 | 124.5 |
ZnCoO/C (2:1) | 3.6 | 197.6 |
ZnCoO/C (1:1) | 3.6 | 248.0 |
ZnCoO/C (1:2) | 3.4 | 348.7 |
CoO/C | 3.2 | 381.6 |
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