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Progress in Chemistry 2020, Vol. 32 Issue (2/3): 298-308 DOI: 10.7536/PC190610 Previous Articles   Next Articles

Special Issue: 锂离子电池; 金属有机框架材料

Application of MOFs Derived Metal Oxides and Composites in Anode Materials of Lithium Ion Batteries

Haodeng Chen1,2, Jianxing Xu1, Shaomin Ji1,**(), Wenjin Ji1, Lifeng Cui2,**(), Yanping Huo1,**()   

  1. 1. School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006, China
    2. School of Materials Science and Engineering, Dongguan University of Technology, Dongguan 523808, China
  • Received: Online: Published:
  • Contact: Shaomin Ji, Lifeng Cui, Yanping Huo
  • About author:
    ** e-mail: (Shaomin Ji);
    (Lifeng Cui);
    (Yanping Huo)
  • Supported by:
    National Natural Science Foundation of China(61671162); National Natural Science Foundation of China(21975055); National Natural Science Foundation of China(21975053); Key Project of Educational Commission of Guangdong Province, China(2017KZDXM025); Technology Plan of Guangdong Province(2019A050510042)
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As the secondary battery with the highest specific energy, lithium ion battery is widely used in portable electronic devices, new energy vehicles and large-scale energy storage power stations. Currently, commercial lithium-ion batteries are facing some technical bottlenecks, such as low energy density and short service life. There are many reports about the anode materials of lithium ion batteries, but most of them cannot overcome the shortcomings such as the huge volume expansion before and after lithium, the pulverization of electrode materials, and the large electrode impedance. However, metal oxides derived from metal-organic frameworks(MOFs) and composites are widely used in lithium ion batteries due to their low level charge-discharge potential platform, high capacity and stable cycle performance. Therefore, in this paper, metal oxides derived from MOFs and composites are divided into four modules: mono-metal oxides, bi-metal oxides, bi-component metal oxide composites and metal oxide/carbon composites. The relationships between their synthesis methods, morphologies and electrochemical properties are summarized, and the opportunities and challenges for their future development are forecast.

Key words: metal-organic frameworks(MOFs), nanomaterials, metal oxide, lithium ion battery, anode material
Table 1 Metal oxides and composite materials prepared from MOFs applied in lithium ion batteries
MOFs Sample Voltage range
(V)		 RCa)
(mAh·g-1/cycles)		 CDb)
(mA·g-1)		 DCc)/CCd)
(mAh·g-1)		 CEe) ref
ZIF-67 Co3O4 0.01~3.0 1335/100 100 1735/1083 96% 31
MOF-71 Co3O4 0.001~3.0 913/60 200 1286.1/879.5 97% 32
{Ni3(HCOO)6·DMF} n NiO 0.01~3.0 760/100 200 1149/850 ~100% 33
Cu-BTC CuO 0.01~3.0 1085/100 100 1334.7/836.1 99% 34
Mn-MOF-74 Mn3O4 0.01~3.0 890.7/400 200 1078.9/625.1 ~100% 35
Mn-MOF-74 δ-MnO2 0.01~3.0 991.5/400 200 -/- 99.4% 35
MIL-88-Fe α-Fe2O3 0.01~3.0 911/50 200 1372/940 97% 36
MIL-53(Fe)-2 Fe2O3-2 0.005~3.0 1176/200 100 1456/1048 ~100% 37
Zn-Co-ZIFs ZnxCo3- x O4 0.01~3.0 990/50 100 1272/969 76.2% 38
Co/Ni-MOF-74 Ni0.3Co2.7O4 0.01~3.0 1410/200 100 1737/1189 - 39
Co/Ni-MOF-74 NiCo2O4 0.01~3.0 1157/200 100 1693/1057 - 39
Co[Fe(CN)6]0.667 CoFe2O4 0.01~3.0 1115/200 1000 1352/1190 85.3% 40
NMOFs NiFe2O4 0.01~3.0 1071/200 1000 1245/1152 - 41
ZF-MOFs ZnFe2O4/ZnO 0.01~3.0 537/500 500 1156/839 ~100% 42
Ni-BTC CuO@NiO 0.005~3.0 1061/200 100 1218/856 ~100% 43
Co3[Fe(CN)6]2@Ni3[Co(CN)6]2 Fe2O3@NiCo2O4 0.01~3.0 1079.6/100 100 1311.4/902.7 96% 44
[Cu3(btc)2)] n CuO/Cu2O 0.01~3.0 740/250 100 727/513 - 45
MIL-101(Cr3+) Cr2O3@TiO2 0.05~3.0 510/500 500 1138/- - 46
IRMOF-1 ZnO QDs@C 0.002~3.0 1200/50 75 2300/- ~100% 47
Mn-doped MIL-53(Fe) MnO-Fe3O4@C 0.01~3.0 1297.5/200 200 1281.4/938.6 96.5% 48
ABO3-type MOF Fe3O4@C 0.01~3.0 1041/50 100 1714/1333 96%~99% 49
CoⅡ(2,3-chedc)(DABCO)0.5 CoO-NCNTs 0.01~3.0 450/300 500 1156/945 ~100% 50
Ni@ZIF-8 Ni@ZnO/CNF 0.01~3.0 1051/100 100 1547/1100 ~99% 27
Co-Ti-MOF Ti-CoO@C 0.01~3.0 1108/150 200 1749/830.7 86.6% 51
Zn-Mn-BTC Zn x MnO@C 0.01~3.0 1050/200 100 1565.9/954.6 99% 52
ZIF-8 C-ZnCo2O4-ZnO 0~3.0 1318/150 200 1311/898 ~100% 53
Fe/Mn-MOF-74 Fe-Mn-O/C 0~3.0 1294/200 100 1333/837 98.5% 54
Table 2 Full cell performance comparison of various nanostructured anode materials with different cathodes
Cathode Anode Current Density Capacity retention
(after n cycles)		 Specific capacity
(mAh·g-1)		 Energy density
(Wh·kg-1)		 ref
LiFePO4 bp-Fe2O3 0.1 A·g-1 (n=80) 421.2 247.03 66
LiMn2O4 Zn0.5MnO@C 0.1 A·g-1 70.4%(n=120) - 122 52
LiFePO4 Fe-MIL-88B 0.25 C 73.7%(n=100) 86.8 - 67
LiFePO4 Fe-MIL-88B 0.5 C 61%(n=200) 55.3 - 67
LiNi0.6Co0.2Mn0.2O4 Si@Sn-MOF 20 mA·g-1 87.8%(n=100) 117.7 - 68
LiCoO2 Ni0.62Fe2.38O4 0.25 A·g-1 70%(n=100) 94 213 69
Fig.1 Schematic of the fabrication processes of the 3D layer-by-layer MnO x hierarchically mesoporous micro-cuboids[35]. Copyright 2018,ACS
Fig.2 (A~C) SEM images at various magnifications,(D) TEM images,(E) HR-TEM images, and (F) SAED pattern of δ-MnO2 materials by Mn-MOF-74 templating at room temperature[35]. Copyright 2018,ACS
Fig.3 Electrochemical properties of the porous ZnxCo3- x O4 hollow polyhedra as electrodes in LiBs:(a) charge-discharge voltage profiles at a current density of 100 mA·g-1,(b) discharge capacities versus cycle number at a current density of 100 mA·g-1, and(c) rate capability at various current rates between 1 and 10 C[38]. Copyright 2014,ACS
Fig.4 Schematic illustration showing the one-step microwave-assisted synthesis of a bimetal organic framework and its derived mesoporous Co-Ni-O nanorod for lithium storage application[39]. Copyright 2015,Wiley
Fig.5 Electrochemical performances of multilayer CuO@NiO spheres:(a) cycle voltammogram profile,(b) first cycle discharge(lithium insertion) and charge(lithium extraction) curve,(c) cycling performance at a current of 0.1 Ah·g-1, (d) Nyquist plots for the first, third and 200 cycles, (e) TEM image of the anode after 200 cycles[43].Copyright 2015, ACS
Fig.6 Schematic illustration for the fabrication of hierarchical MnO-doped Fe3O4@C composite nanospheres[48]. Copyright 2018, ACS
Fig.7 (a,b) SEM images,(c,d) TEM images,(e,f) HRTEM images, and (g) elemental mapping images of Fe-Mn-O/C microspheres[54]. Copyright 2019,RSC
Fig.8 Schematic illustration of the detailed formation process of the AZT CNCs[29]. Copyright 2018, Wiley
Fig.9 a) Ultralong cycling performance of AZT-0, AZT-30, and AZT-60 at a high current density of 2.0 A·g-1. CV curves of b) AZT-0, c) AZT-30, and d) AZT-60 at a scan rate of 0.1 mV·s-1 after 10, 50, 100, 250, and 500 charge/discharge cycles[29]. Copyright 2018, Wiley
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