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Progress in Chemistry 2022, Vol. 34 Issue (2): 460-473 DOI: 10.7536/PC201113 Previous Articles   Next Articles

• Review •

Application of Bimetallic MOFs and Their Derivatives in Electrochemical Energy Storage

Yumeng Wang1, Rong Yang1,2(), Qijiu Deng2, Chaojiang Fan1,2, Suzhen Zhang1, Yinglin Yan1   

  1. 1 International Research Center for Composite and Intelligent Manufacturing Technology, Xi’an University of Technology,Xi'an 710048, China
    2 School of Materials Science and Engineering, Xi’an University of Technology,Xi’an 710048, China
  • Received: Revised: Online: Published:
  • Contact: Rong Yang
  • Supported by:
    International Science and Technology Cooperation Program of China(2015DFR50350); National Natural Science Foundation of China(51702256); China Postdoctoral Science Foundation(2019M653706); Innovation Capability Support Program of Shaanxi(2019TD-019); Postdoctoral Science Foundation of Shaanxi Province of China(2018BSHEDZZ120)
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Bimetallic organic frameworks and their derivatives have the characteristics of rich pore structure, large specific surface area, adjustable structure, abundant active sites, as well as the synergistic effect between bi-component and porous structure, so they are paid close attention to by researchers and widely used in electrochemical energy storage, catalysis, separation, sensors, medicine, gas storage and other fields. Just as monometallic organic frameworks, the poor conductivity and collapsible structure of bimetallic organic frameworks greatly limit their applications in electrochemical energy storage. It is through heat treatment of bimetallic organic frameworks that porous carbon@bimetallic oxide/sulfide/phosphide/selenide derivatives with uniform distribution, which not only keep rich pore structure, but also have improved conductivity and structural stability, being conducive to the application in the field of electrochemical energy storage are obtained. Therefore, in the view of the main metal ions in the bimetallic organic frameworks, this research reviewes the latest progress of the organic frameworks and their derivatives in electrochemical energy storage devices such as supercapacitors, lithium ion batteries, sodium ion batteries, and metal-air batteries, respectively. On this basis, the advantages of bimetallic MOFs in the application of electrochemical energy storage are summarized, and suggestions on its preparation, mechanism and post-treatment are put forward.

Contents

1 Introduction

2 Application of bimetallic MOFs in the field of electrochemical energy storage

2.1 Co-based bimetallic MOFs

2.2 Ni-based bimetallic MOFs

2.3 Zn-based bimetallic MOFs

2.4 Other bimetallic MOFs

3 Conclusion and outlook

Key words: bimetallic organic framework, derivatives, electrochemical energy storage
Fig. 1 The theoretical energy densities of different metal-air batteries
Table 1 Preparation of bimetallic MOFs and their derivatives
Metals Organic ligands Preparation method Post treatment Reagent Heat treatment
conditions
(Atmosphere,
Temperature/ ℃,
Time/h, Heating
rate/ ℃·min-1)		 Product Objective Application ref
CoZn 2-MeIm Stirring Carboni-
zation		 — Ar/H2, 700, 3, 5 Co Precursors for self-catalyzed CNTs growth Li-S batteries 26
ZnCo 2-MIM Immerse — Ar, 800, 2, 1 Co Enhance catalytic properties Zn-air/Al-Air batteries 27
CoFe benzimidazole Solvothermal — N2, 700, 4, — Co/Fe Enhance ORR activity Zn-air batteries 28
FeNi trimesic acid Stirring — Ar, 800, 6, 2 FeNi3Cx Enhance OER activity Zn-air batteries 29
CoCu 2-MeIm Solvothermal Oxidation — Air, 350, 2, 1 CuCo2O4 Formation of yolk shell structure Supercapacitors 30
CoMn urea Solvothermal — Air, 600, 5, 1 MnCo2O4 Manganese can bring high capacity Supercapacitors 31
CoNi H3BTC Hydrotherma — Air/Ar, 400, 2, 1 NiCo2O4/NiO Formation of multilayer core-shells Supercapacitors 32
ZnMn 2-MeIm Immerse — Ar, 800, 1, 3 Mn@ZnO Improve the ion adsorption and charge-transfer Supercapacitors 33
CoCu H3BTC Solvothermal — Air, 450, 2, — Co3O4@CuO Unique yolk-shell structure,and the multistep Li+ storage Li-ion batteries 34
NiCo 3,5-pyrazoledi-carboxylic acid Solvothermal Vulcaniza-
tion		 TAA N2, 300, 1, 2 NiS/CoS Improve the structural stability Supercapacitors 35
ZnCo 2-MeIm Standing S N2, 800/600, 5/2,
2/5		 CoS2 Zn was evaporated to form the porous composites Supercapacitors 36
CoNi 2-MeIm Immerse Na2S N2, 350, 2, 3 NiCo2S4 Improve conductivity and structural stability Battery-Supercapacitor 37
ZnCo 2-MeIm Stirring S N2, 600, 2, 2 Zn0.754Co0.246S Zn-Co-S yolks deliver high capacity and the fabricated void spaces can alleviate the large volume change Li-ion batteries 38
CoZn 2-MeIm Stirring TAA Ar, 600, 2, 2 CoZnS Unique structure and synergistic effect of bimetallic sulfide Li-ion batteries 39
NiCo 1,10-phenanthr-oline Solvothermal Phospho-
rization		 NaH2PO2 N2, 450, 2, 5 NiCoP Have higher electrical conductivity and richer redox reactions Supercapacitors 40
NiCo formic acid Stirring NaH2PO2 N2, 350, 2, 2 NiCoP Formation of hollow structure Supercapacitors 20
CoNi 2-MeIm Standing NaH2PO2 N2, 300, 2, 2 NiCoP Improve the structural stability Li-ion batteries 41
NiCo trimesic acid Standing Selenization Se N2, 600, 2, 2 NiCoSe Improve the structural stability Li-ion batteries 42
MnFe CTAB Stirring Se N2, 500, 2, 1 FeMnSe Unique porous architecture and synergistic effect of the heterogeneous components K-ion batteries /Na-ion batteries 43
Fig. 2 A schematic diagram of the preparation of EC@NiCo2S4[44]
Table 2 Summary of electrochemical performances of Co-based bimetallic MOFs and some derivatives in the supercapacitors
Device Specific capacitance Cycling performance Specific energy/Specific Power ref
ZnCo2O4@NC/CTS//Fe3O4@r-GO ASC 2003.80 F·g-1 at 1.79 A·g-1 85.89% after 6000 cycles 2.32 mWh·cm-3 at 33.3 mW·cm-3 22
Co/Mn-MOF//AC 1176.59 F·g-1 at 3 mA·cm-2 93.51% afer 5000 cycles 57.2 Wh·kg-1 at 2000 W·kg-1 24
CoSx/Ni-Co-LDH//AC 1562 F·g-1 at 1 A·g-1 94.56% after 10,000 cycles 35.8 Wh·kg-1 at 800 W·kg-1 25
CuCo2O4//rGO 701 C·g-1 at 2 A·g-1 93.6% after 6000 cycles 38.4 Wh·kg-1 at 800 W·kg-1 30
EC@NiCo2S4//EC 1394.5 F·g-1 at 1 A·g-1 124% after 10,000 cycles 46.5 Wh·kg-1 at 801 W·kg-1 44
GNS/MC//Carbon black ASC 923.97 F·g-1 at 1 A·g-1 111% after 5000 cycles 82.13 Wh·kg-1 at 399.74 W·kg-1 31
Zn0.76Co0.24S/NiCo2S4//AC ASC 2674 F·g-1 at 1 A·g-1 91% after 5000 cycles 48.1 Wh·kg-1 at 837 W·kg-1 45
NiCo-A-S//FexOy@CNS ASC 213 mAh·g-1 at 1 A·g-1 83.5% after 5000 cycles 48.2 Wh·kg-1 at 840 W·kg-1 46
Ni-Co S/ACC//AC 2392 F·g-1 at 1 A·g-1 82% after 10,000 cycles 30.1 Wh·kg-1 at 800.2 W·kg-1 47
Porous NiCo2S4//N-doped Carbon 241 C·g-1 at 1 A·g-1 84.8% after 2000 cycles 51.98 Wh·kg-1 at 800 W·kg-1 37
Fe-doped Co3O4//N-doped Carbon 118.4 F·g-1 at 1 A·g-1 90% after 4000 cycles 37 Wh·kg-1 at 750 W·kg-1 48
Fig. 3 (a, b) SEM images, (c, d) TEM images, (e)High resolution TEM image of NiCoP[41]
Fig. 4 (a) Preparation of Co3O4@CuO@GQDs, (b) Cyclic performance of Co3O4@CuO@GQDs and pristine Co3O4@CuO at 0.1 A·g-1[34]
Fig. 5 Illustration of the overall fabrication process for the M-FeCo-N-C-X catalysts[13]
Table 3 Morphology of Ni-based bimetallic organic frameworks
Metals Organic ligands Solvent Preparation method Morphology ref
Ni/Co 2,5-Dihydroxyterephthalic acid DMF/H2O/EtOH Hydrothermal Layered 55
Ni/Co Trimesic acid H2O/C2H5OH Rest Bundle-like 42
Ni/Co Terephthalic acid DMF/H2O/EtOH Hydrothermal Triangle-like 56
Ni/Co Trimesic acid DMF/H2O/EtOH Stir Rod-like 57
Ni/Co 3,5-Pyrazoledicarboxylic acid H2O/EtOH Hydrothermal Layered 35
Ni/Co 1,10-phenanthroline EtOH Heating reflux Irregular polygon 40
Ni/Co Trimesic acid DMF Stir Hexagonal plate-like 58
Ni/Fe Terephthalic acid DMA Hydrothermal Rod-like 59
Ni/Fe Trimesic acid H2O/EtOH Stir Rod-like 29
Ni/Fe Benzene-1,3,5 tricarboxylate EtOH Rest Rod-like 60
Fig. 6 Performances of RZABs employing FeNi3Cx-Pd-7% and Pt/C+RuO2 catalysts as the air-cathode. (a) Schematic illustration of the self-assembled RZAB. (b) The discharge polarization curves and the corresponding power density plots. (c) The open-circuit potential plots. (d) Galvanostatic discharge specific capacity curves at 10 mA·cm-2. (e) Galvanostatic charge-discharge cycling curves at 10 mA·cm-2 with a duration of 10 min per cycle. Inset into the panel (e) is the optical photo of a LED powered by two RZABs connected in series, using FeNi3Cx-Pd-7% loaded carbon fiber papers as air cathode[29]
Fig. 7 (a) N2 adsorption-desorption isotherms of NPC-300-900 and NPC-5-900, (b) pore size distribution of NPC-300-900 and NPC-5-900[65]
Fig. 8 Schematic of the fabrication of Mn@ZnO/CNFs. Upper row: Electrospinning setup, SEM image of Mn@ZnO/CNF, and photograph of flexible electrodes powering an LED. Lower row: Loading of Mn@ZIF-8 over CNFs, atomic structures of Mn@ZIF-8, and a photograph showing the flexibility of an electrode sample[33]
Fig. 9 Electrocatalytic mechanism of CNCo-5@Fe-2 catalyst for ORR[66]
Fig. 10 SEM images of (a) Cu-BTC, (b) Cu@C, (c) Ni-BTC, (d) Ni@C, (e) CuNi0.25-BTC, (f ) CuNi0.25@C, (g) CuNi0.5-BTC, (h) CuNi0.5@C[70]
Fig. 11 SEM images of the MnS-(ZnCo)S/N-C composite[73]
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