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化学进展 2023, Vol. 35 Issue (12): 1807-1846 DOI: 10.7536/PC230502 前一篇   后一篇

• 综述 •

金属有机框架及其衍生纳米负极材料

马浩天1,2, 田如锦1,*(), 文钟晟2   

  1. 1 大连交通大学材料科学与工程学院 大连 116028
    2 大连海事大学材料科学系 大连 116026
  • 收稿日期:2023-05-04 修回日期:2023-09-19 出版日期:2023-12-24 发布日期:2023-12-18
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Metal-Organic Frameworks and Their Derivative Nano Anode Materials

Haotian Ma1,2, Rujin Tian1,*(), Zhongsheng Wen2   

  1. 1 College of Materials Science and Engineering,Dalian Jiaotong University,Dalian 116028, China
    2 Department of Materials,Dalian Maritime University,Dalian 116026, China
  • Received:2023-05-04 Revised:2023-09-19 Online:2023-12-24 Published:2023-12-18
  • Contact: *e-mail: rjtian_88@163.com

负极是锂离子电池的重要组成部分之一,较低的离子-电子电导率、明显体积效应以及容易粉化等问题限制着传统负极材料的发展和广泛应用。金属有机框架(MOFs)及其衍生材料的丰富孔隙有利于离子快速迁移,较大的比表面积提供更多的电化学反应活性位点,尤其是能通过改变合成工艺实现结构和化学组成调控,有效提高锂离子电池的可逆容量和循环稳定性。本文系统地总结和归纳了近年来MOFs及其衍生纳米负极材料的研究进展,梳理了不同合成方法、形貌结构与电化学性能间的相互关系,分析了这类负极材料急待解决的关键问题和面临的机遇与挑战。在尽可能充分发挥各自优势的基础上,结合有机配体和金属中心的多样性以及结构的多变性和特殊性,提出了一些改善储锂性能的有效措施和工业化应用的解决方案,展望了这类新型多孔纳米负极材料的未来发展趋势和应用前景。

关键词： 锂离子电池, 负极, 金属有机框架, 衍生材料

Anode is one of the important components for lithium ion battery. Many technical bottlenecks (such as lower ionic-electronic conductivity, huge volume effect and easy pulverization resulted from long-term charge/discharge process) prevent the development and large scale application of traditional anode materials. As a novel kind of advanced multi-functional materials, Metal-organic frameworks (MOFs) and their derivative materials behave enough pore structures promoting rapid migration of Li+ and electron, and high specific surface areas providing abundant active sites for electrochemical reaction. Importantly, tunable structure and chemical composition of the MOFs and their derivative materials can be further optimized by changing parameters of synthesis process, thereby markedly increases specific capacity and cycle stability of lithium ion batteries. Herein, the recent progress in the MOFs and their derivative materials used as anode for lithium ion batteries are reviewed systematically, and the relationships between their preparation methods, microstructures, morphologies and corresponding electrochemical properties are summarized detailly. The urgent problems and challenges of this class of anode materials for lithium ion batteries are also analyzed. On the basis of resonable choosing organic ligands and metal centers, some effective measures for improving performances of lithium storage are proposed by combining with the variability and particularity of structure of the MOFs and their derivative materials, and the feasible strategies for commercialization application are suggested. Finally, the perspective and future development in design and fabrication of the new types of nano porous anodes with high energy efficiencies in relation with the next generation lithium ion battery are further discussed.

Contents

1 Introduction

1.1 Conversion mechanism

1.2 Insertion/extraction mechanism

1.3 Absorption/desorption mechanism

2 Pristine MOFs

2.1 Co-MOFs

2.2 Zn-MOFs

2.3 Mn-MOFs

2.4 Fe-MOFs

2.5 Ni-MOFs

2.6 Cu-MOFs

2.7 Sn-MOFs

2.8 Other metal-based MOFs

3 MOFs-derived metal compounds

3.1 Monometal oxides

3.2 Bimetal oxides

3.3 Other metal compounds

4 MOFs-derived porous carbon

5 MOFs-derived composites

5.1 MOFs/metal compounds

5.2 MOFs/carbon-based materials

5.3 Metal oxide/metal oxide

5.4 Metal oxide/carbon-based materials

5.5 Metal sulfide/carbon-based materials

5.6 Other metal compound/carbon-based materials

5.7 Metal/metal oxide/carbon-based materials

6 Conclusion and outlook

Key words: lithium ion battery, anode, metal-organic frameworks, derivative materials
()
图1 锂离子电池MOFs及其衍生负极材料的发展时间轴
Fig. 1 Brief summary of the development history of MOFs and their derivative anode materials for Li-ion batteries
表1 MOFs本体负极材料及其电化学性能
Table 1 Pristine MOFs as anode materials and their electrochemical performances
Materials Voltage range (V) Current density (mA/g) Cycle number Overall capacity (mAh/g) Initial discharge/
charge capacity
(mAh/g)		 Initial coulomb
efficiency
(%)		 Specific surface area
(m2/g)		 ref
CoBTC-EtOH 0.01-3.0 100/2000 100/500 856/473 1790.3/879 49.15 17.7 19
S-Co-MOF 0.01-3.0 100/500/1000 200/700/1000 1021/601/435 1964/1564 80.4 10.4 10
H-Co-MOF — 100/2000 100/700 1345/828 2147/1432 66.7 49.9 20
u-CoTDA 0.01-3.0 100/1000/2000 100/300/400 946/790/548 1631/- 75.2 52.6 22
[Co1.5L(H2O)4]n 0.01-3.0 50 50 431 1978/869 — — 23
Co2(DOBDC) 0.01-3.0 100/500 100/200 878.5/526.1 1409/785 56 — 24
Co-BDCN 0.01-3.0 100 100 1132 1439/1015 70.54 24.5 25
Co-BTC 0.01-3.0 100 200 750 1739/622 36 18.5 26
CoTPA 0.005-2.8 60 100 700 1938/1004 51.8 — 27
Co2(OH)2BDC 0.02-3.0 50 100 650 1385/1005 72.8 — 28
CoC6H2O5(H2O)2 0.05-3.0 100/1250 95/499 549.8/513.4 -/- — — 29
Zn3(HCOOH)6 0.005-3.0 60 60 560 1344/693 — — 30
BMOF — 100 200 190 -/- — 821 31
Mn-LCP 0.01-2.5 50 50 390 1807/- — — 32
CMPS-1 0.05-3.0 400/500 250/650 645.7/588.3 1631.8/- — — 33
Mn-BTC 0.01-2.0 103/1030/2060 100/100/100 694/400/250 1717/694 40.4 23.8 34
Mn-PBA 0.01-3.0 200 100 295.7 1123.7/544.5 48.5 499.8 35
Mn-1,4-BDC@200 0.01-3.0 100 100 974 1746/706.4 40.5 6.135 36
Mn-UMOFNs 0.01-3.0 100/1000 100/300 1187/818 -/- 57 32.65 38
Fe-BTC 0.01-3.0 100 100 1021.5 1765.5/683.2 38.7 1125 42
MIL-88A 0.01-3.0 10 4 40.5 140.5/5.3 4 — 43
Fe-MIL-88B 0.005-3.0 60 400 744.5 1507/949.9 63 — 44
Fe-BDC@300 0.01-3.0 100 120 324.1 1330.6/- 45
Ni-UMOFNs 0.01-3.0 100 100 546 1833/1226 67 15.04 38
Ni-MOF 0.01-3.0 100 100 620 1984/1369 — — 46
Ni-Me4bpz 0.01-3.0 50 100 120 320/- — 67 14
[Cu2(C8H4O4)4]n 0.01-2.5 48 50 161 1492/194 — 747 48
Cu3(BTC)2 0.05-3.0 96/191/383 50/50/50 740/644/474 1497/641 — 489.4 49
[Cu2(cit)(H2O)2]n 0.01-3.0 100/2000 500/500 608.5/321.5 -/- — — 50
Sn-MOF 0-3.0 20 200 610 1017/450 — 67.437 51
Sn-MOF 0.01-3.0 50 100 250 -/- — 16.96 52
Al-FumA MOFs 0.01-3.0 37.5/37500 100/100 392/258 1509/899 45.5 260.1 53
Pb-MOF 0.01-3.0 100/500 500/500 489/380 1522/678 38 725 16
Cd-MOF 0.1-3.0 100 100 302 710/435 — 821 18
Ti-MOF 0.01-3.0 200/400 200/500 296/175.34 1590.24/- — 621 54
Li/Ni-NTC 0.01-3.0 100 80 482 1084/601 — — 55
Zn1.5Co1.5(HCO2)6 0.005-3.0 60 60 510 1344/693 — — 30
图2 (a)CV曲线(0.1mV/s), (b) 潜在储锂位点 (Ⅰ 苯环; Ⅱ孔隙; Ⅲ层间空间), (c) 初始3次充放电曲线(0.2 A/g), (d) 倍率性能, (e)与其他负极在不同电流密度时的容量,(f) 0.2和0.5A/g时Ni-CAT NRs的循环性能[57]
Fig. 2 (a) CV curves (0.1 mV/s), (b) potential lithium-storage sites (Ⅰ, benzene rings; Ⅱ, pores; Ⅲ, interlaminar space), (c) initial three charge and discharge plots (0.2 A/g), (d) rate behaviour, (e) comparison of capacities with other anodes at various current densities, and (f) cycling properties at 0.2 and 0.5 A/g of the Ni-CAT NRs[57]
表2 MOFs衍生金属氧化物负极材料及其电化学性能
Table 2 MOFs-derived metal oxides as anode materials and their electrochemical performances
Materials Template/precursor Voltage range (V) Current density (mA/g) Cycle number Overall capacity (mAh/g) Initial discharge/charge capacity (mAh/g) Initial coulomb efficiency(%) Specific surface area
(m2/g)		 ref
CuO Cu(L-Phe)2 0.1~3.0 100/1000 200/500 505.3/116.7 -/- — — 62
CuO Cu-BTC 0.05~3.0 100 100 470 1208/- 40 49.6 63
CuO MOF-119 0.005~3.0 2000 40 210 1208/538 — — 64
CuO Cu-BTC 0.01~3.0 500/1000/2000 200/400/400 1062/615/423 1334.7/836.1 — 49.75 65
Mn2O3 Mn-MIL-100 0.1~3.0 200 100 755 1668/1003 — 40.45 66
Mn2O3 Mn-LCP 0.01~3.0 1000 250 705 1158/852 74 15.34 67
Mn2O3 Mn-MOF 0~3.0 400/1000 450/1200 1370/819.8 -/- — — 68
Mn2O3 Mn-BTC 0.01~3.0 100 60 582 3404/1559 46 38.5 69
Mn3O4 Mn-MOF-74 0.01~3.0 200/2000 400/400 890.7/437.1 1078.9/625.1 — 80.5 70
Co3O4 [Co3(HCOO)6](DMF)4 0.01~3.0 50/100 50/100 965/730 1118/- — 5.3 71
Co3O4 Co-MOF 0.01~3.0 1000/5000 350/600 628/412 1402/879 62.7 42 72
Co3O4 CoBDC MOF 0.01~3.0 100/1000 160/200 1477/775 1392/961 69.09 133.74 73
Co3O4 Co-BTC 0.00~3.0 100 60 886 2082/1061 51 10.44 74
Co3O4 Co-MOF 0.01~3.0 100 50 1115 1608/1080 — 43 75
Co3O4 PBA — 300 50 1465 1557/- — 66.5 76
Co3O4 MOF-71 0.001~3.0 200 60 913 1286.1/879.5 68 59 77
Co3O4 Co2(NDC)2DMF2 0.01~3.0 200/2000 100/100 1058.9/348 1504.2/976.7 40 78
Co3O4-a Co-MOF 0.01~3.0 100 90 470.3 1325.5/1003.5 75.7 22.6 79
Co3O4 ZIF-67 0.01~3.0 100/100 100/60 1335/1265 1735/1083 — 45 81
Co3O4 Co-MOF 0.01~3.0 100 100 1370 1324/1034 — 20.1 80
α-Fe2O3 MIL-88 0.01~3.0 200 50 911 1372/940 69 75 84
α-Fe2O3 Fe-MOF 0.005~3.0 100 40 921.6 1487/1024 — — 85
Fe2O3-2 MIL-53 0.005~3.0 100/1000 200/500 1176/744 1456/1048 — 93.1 86
Fe2O3 PB 0.01~3.0 200 30 945 -/- — 25.4 87
NiO MOF-C 0.005~2.5 500/1000 100/100 748/410 2134/1303 61 36 88
NiO Ni-MOF 0.01~3.0 15 100 380 900/480 — 24 89
NiO Ni-MOF 0.0~3 200 100 760 1149/850 28.6 90
TiO2 MIL-125 1.0~3.0 168/840/1680 500/500/500 166/106.5/71 168/- — 220 95
GeO2 Ge-MOF 0.005~3.0 100 350 1393 2079/1315 63.2 12.9 96
MnCo2O4 Mn-Co-MOF 0.01~3.0 100 100 929 1496/963 64 31.69 101
Zn-NPs ZIF-L 0.01~3.0 100 100 143 1245.9/692.2 55.6 47.6 97
ZnCo2O4 ZnCo-8-hydroxyquinoline 0.01~3.0 100/1500 50/25 1640.8/348.1 1710.2/1273.5 74.5 118 102
Mn1.8Fe1.2O4 Mn3[Fe(CN)6]2·nH2O 0.01~3.0 200 60 827 2312/1337 57.8 124 103
NixCo3-xO4 Ni-Co-BTC 0.005~3.0 100/1000/2000 100/300/300 1109.8/832/673 1619.2/1139.3 70 96.7 104
ZnxCo3-xO4 Zn-Co-ZIF 0.01~3.0 100 50 990 1272/969 76.2 65.58 105
CoFe2O4 Co[Fe(CN)6]0.667 0.01~3.0 — — — 1352/1190 85.3 102.692 106
NiFe2O4 Ni2Fe(CN)6 0.01~3.0 914 200 1071 1245/1152 — 260.9 107
Ni0.3Co2.7O4 Co/Ni-MOF-74 0.005~3.0 100/2000/5000 200/500/500 1410/812/656 1737/1189 — 28.5 108
Li4Ti5O12 MIL-125 1.0~3.0 500 700 120.3 184.9/149.1 80.6 — 109
图3 NCNFs在Li+半电池中的电化学性能: (a) NCNFs-800在0.1 mV/s时的CV曲线, (b) NCNFs-800在0.1 A/g时的充放电曲线, (c) NCNFs在电流密度0.1~10 A/g时的倍率性能, (d) NCNFs-800在2 A/g时的循环性能[128]
Fig. 3 The electrochemical performances of NCNFs in Li+ half cells. (a) CV curves of NCNFs-800 at 0.1 mV/s. (b)Discharge/charge profiles of NCNFs-800 at 0.1 A/g. (c) Cycling performances of NCNFs at 100 mA/g. (d) Rate capability of NCNFs at a current density from 0.1 to 10 A/g.(e) Cycling performance of NCNFs-800 at 2 A/g[128]
表3 MOFs衍生多孔碳负极材料及其电化学性能
Table 3 MOFs-derived porous carbon as anode materials and their electrochemical performances
Materials Template/precursor Voltage range (V) Current density (mA/g) Cycle number Overall capacity (mAh/g) Initial discharge/charge capacity (mAh/g) Initial coulomb efficiency(%) Specific
surface
area
(m2/g)		 ref
3D porous carbon Zn4O(BDC)3 0.01~3.0 100 100 1015 2983/1084 — 1880 114
porous carbon Zn-MOF 0.01~3.0 74 50 2016 -/2458 — 2587 121
Porous carbon Co-MOF 0.01~3.0 100 49 549 3066/946 — 688 124
Porous carbon Cd-MOF 0.01~3.0 300 300 1285 2486/1683 68 1796 125
Porous CNFs ZIF-8 0.01~3.0 100 200 520 570/390 68 — 126
Nitrogen-modified carbon Cu-MONFs 0.01~3.0 500/5000 800/1000 853.1/440 1584.4/942.1 59.5 7.275 127
N-C Cu-MOF 0.01~3.0 100/1000 100/1500 890/588 2037/1039 51 — 128
N-P-C Ni-ZIF 0.01~3.0 100 200 570 1497/725 48.5 320.8 129
N-NPC Al-MOF 0.01~3.0 1000 400 352 820/720 87.8 1244 130
N-C-550 Sr-MOF 0.1~3.0 100 50 736.8 1043/675 64.71 — 131
N-C-800 ZIF-8 0.01~3.0 100/5000 50/1000 1147/785 3487/2037 58.4 — 134
表4 MOFs/多孔碳复合负极及其电化学性能
Table 4 MOFs/ metal compound composites as anode materials and their electrochemical performances
Materials Voltage range (V) Current density (mA/g) Cycle number Overall capacity(mAh/g) Initial discharge/
charge capacity
(mAh/g)		 Initial coulomb efficiency(%) Specific surface area (m2/g) ref
Co-MOFs/CF 0.01~3.0 50 100 445.1 1621.3/976.7 60.2 163.4 136
MIL-101(Cr)/GO 0.01~3.0 200 40 40.3 445.7/- — 3081 137
Cu-MOF/RGO 0.01~3.0 50 50 520 872.7/- 45.8 — 138
F-Co-MOF/RGO 0.01~3.0 100/2000 50/550 1202/771.5 2464.2/1- 73.45 — 140
Fe-MOF/RGO(5) 0.01~3.0 500 200 1010.3 2055.9/891.1 43.3 — 141
MIL-53(Fe)@RGO 0.01~3.0 100 100 550 -/- 42.3 240.9 142
Co-BDC/CGr 0.01~3.0 100/1000 100/400 1368/818 2566/- 75.42 58.151 143
MOF/RGOn 0.01~3.0 100/1000 100/500 715/348 1677.5/732.6 43.7 — 145
图4 Fe2O3纳米管@Co3O4复合材料的合成示意图: (Ⅰ) MIL-88B纳米棒、Co2+和 2-methylimidazole (2-MIM)自组装成MIL-88B@ZIF-67复合材料; (Ⅱ) 经空气中热处理转变为Fe2O3纳米管@Co3O4复合材料[161]
Fig. 4 Schematic illustration of the formation process of the Fe2O3 nanotubes@Co3O4 composite. (Ⅰ) Self-assembly of MIL-88B nanorods, Co2+ ions, and 2-methylimidazole (2-MIM) to a MIL-88B@ZIF-67 composite. (Ⅱ) Transformation to Fe2O3 nanotubes@Co3O4 composite through thermal treatment in air[161]
表5 金属氧化物/金属氧化物复合负极材料及其电化学性能
Table 5 Metal oxide/metallic oxide composites as anode materials and their electrochemical performances
Materials Template/precursor Voltage range (V) Current density (mA/g) Cycle
number		 Overall capacity (mAh/g) Initial discharge/
charge capacity
(mAh/g)		 Initial
coulomb
efficiency
(%)		 Specific surface area (m2/g) ref
5Co3O4/CeO2 Co-Ce-MOF 0.01~3.0 100/500 100/300 1131.2/901.4 1090.1/873.6 77.6 19.265 152
Fe2O3/SnO2 Fe-MOF 0.05~3.0 200 100 500 1751/904 — 43 153
ZnO/NiO Zn-Ni-MOF 0.005~3.0 100/500 200/1000 1008.6/592.4 1221.7/769.2 62.9 21.34 154
Co3O4/TiO2 ZIF-67 0.01~3.0 500 200 642 662/535 — — 155
CuO/Cu2O [Cu3(btc)2]n 0.01~3.0 100 250 740 727/513 — 9 156
CuO@NiO Cu-Ni-BTC 0.05~3.0 100 200 1061 1218/856 — 16.3 157
Cr2O3@TiO2 MIL-101(Cr)
@TiO2		 0.05~3.0 0.5C 500 510 1138/- — 146 158
CuO@TiO2 HKUST-1/TiO2 0.01~3.0 100 200 692 1092/780 71.4 88.9 159
Fe2O3-CuO PB 0.01~3.0 500 120 744 1070/795 74 — 160
NiFe2O4@Fe2O3 Fe2Ni MIL-88/
FeMIL-88		 0.01~3.0 100 100 936.9 1400.9/989.1 — 39.2 163
Fe2O3@NiCo2O4 Co3[Fe(CN)6]2
@Ni3[Co(CN)6]2		 0.01~3.0 100 100 1079.6 1311.4/902.7 — 12.72 164
Co3O4-CoFe2O4-12 MOF-74-FeCo-xy 0.01~3.0 100/500 80/80 940/598 1328/918 — — 165
ZnO/ZnCo2O4 ZnO@ZIF-8 NRAs 0.01~3.0 1000/2000 200/250 870/1016 1299/987 76 20 166
NiO/ZnCo2O4 Ni(OH)2@ZIF-8 0.01~3.0 2000 100 1002 -/- — 44 167
ZnO/ZnFe2O4 Zn3[Fe(CN)6]2 0.01~3.0 1000/2000 200/200 837/701 1892/1371 70 54.3 168
ZnO/ZnFe2O4 Prussian Blue 0.01~3.0 1000/2000 500/100 804/497 1293/826 63.8 39.0 169
ZnO/ZnFe2O4 ZnFe PBA 0~3.0 200 200 704 998.4/704.9 70.6 — 170
图5 In2O3/HPNC复合材料的形貌特征:(a)与(b) SEM图像;(c)与(d) TEM图像;(e) HRTEM图像(内部为SAED谱)(f~k) TEM暗场图像和相应元素分布[191]
Fig. 5 Morphological features of In2O3/HPNC composite: (a) and (b) SEM images, (c) and (d) TEM images, (e) HRTEM images, and the inset is the SAED pattern, and (f~k)Dark-field TEM image and corresponding elemental mapping[191]
表6 金属氧化物/碳基复合负极材料及其电化学性能
Table 6 Metal oxide/carbon-based composites as anode materials and their electrochemical performances
Materials Template/precursor Voltage range (V) Current density (mA/g) Cycle
number		 Overall capacity (mAh/g) Initial discharge
capacity/charge
capacity
(mAh/g)		 Initial coulomb efficiency(%) Specific surface area (m2/g) ref
Co3O4/C ZIF-67 0.01~3.0 200 120 1100 1209/864 71.0 179.4 171
ZnO@C PPy@ZIF-8 0.01~3.0 250/1000/2000 500/500/1000 526/397/275 1106.2/665.8 60.2 — 174
Co3O4/C PPy@ZIF-67 0.01~3.0 250/1000/2000 500/500/1000 721/372/272 1112/645 58 — 174
CuO/C Cu-MOF 0.01~3.0 100 200 789 1259/- 76 131.7 175
CuO/C [Cu3(btc)2]n 0.01~3.0 100 200 510.5 1150.9/450.4 46.2 16 176
Mn3O4/C Mn-PBA 0.01~3.0 200 500 1032 1500/1205 80.3 137 177
Mn3O4/C MOF 0.01~3.0 200/500/700 100/120/120 770/651/592 1186/722 60.8 8.0 178
MnO/C Mn-MOF 0.01~3.0 50/500 150/500 884/648 1321.6/779.2 59 313 179
MnO/C Mn(PTA)-MOFs 0~3.0 600/1000 100/200 804/800 -/- — 309 180
ZnO/C Zn-BTC 0.01~3.0 500 120 741 1205/715 59 198 181
Fe3O4/C Fe-MOFs 0.01~3.0 100 100 861 1044.2/- 82.4 27 186
Fe3O4@C Fe-MOF 0.01~3.0 100 80 776.8 1714/1333 78 4.57 187
SnO2@C HKUST-1 0.001~3.0 100 200 880 2134/1208 — 474 189
In2O3/C MIL-68(In) 0.01~3.0 100 150 720 1410/- 43 152 190
MWCNTs/Co3O4 MWCNTs/ZIF-67 0.01~3.0 100 100 813 1171/812 — 62.9 192
MWCNTs/ZnO ZIF-8/MWCNTs 0.01~3.0 200 100 419.8 1477/854 — 94.13 193
NiO/CNTs-10 Ni-MOF/CNTs 0.005~3.0 100/2000 100/300 812/502 1100/- — 134.68 194
CNT/Co3O4 ZIF-67 0~3.0 1000/4000 200/200 782/577 1840/1281 — 93.9 195
CFs@Co3O4 CFs@ZIF-67 0.01~3.0 100 150 420 630/369.9 63 532.4 196
3DGN/CuO Cu-BTC 0.01~3.0 100 50 405 569/422 74 — 197
NiO/GF Ni-MOF/GF 0.01~3.0 100 50 640 903/612 67.8 119 198
Fe2O3/rGO MIL-88-Fe/GO 0.01~3.0 500/5000 200/500 846.9/610.3 1478/971 — — 199
RGO@Co3O4 GO@ZIF 0.01~3.0 100 100 974 1451/- 70 198.54 200
RGO/NiO GO/Ni-MOFs 0~3.0 100 200 440 681/678 99.49 — 201
MnO/C-N-500 Mn-PBI 0.01~3.0 300 100 1085 1507/1143 75.8 146.4 203
NiO@N-C Ni-NTA 0~3.0 50/4000 300/1200 921/450 1220/1009 82.3 — 204
Fe2O3@N-C Fe-ZIF 0.01~3.0 100/1000 50/100 1573/1142 1696/1368 80.7 27.1 206
NCW@Fe3O4/NC NCW@Fe-ZIFs 0.01~3.0 100/1000 170/600 1963/1741 2867/1585 55.3 52.7 208
Co3O4/N-C Co-TATB MOFs 0.0~3.0 1000 200 620 1062/- 75.0 — 209
Co3O4/N-C N-rich Co-MOF 0.01~3.0 1000 500 612 1210/613 51 21.5 210
Co3O4/N-PC ZIF-67 0.05~3.0 100 100 892 1730/1321 76.4 97 211
Co3O4@N-C Co-MOF 0.1~3.0 500 300 795 1385/1055 76 30.16 212
MS-Co3O4@PC Co-MOFs 0.01~3.0 100/1000 60/500 1701/601 1470/1188 80.8 22.1 213
CoO-NCNTs 2D-MOFs 0.01~3.0 500 2000 583 1156/945 81.7 86.26 214
Co3O4@NGN ZIF-67@NGA 0.01~3.0 200/1000 100/400 955/676 976/865 52.3 50 215
ZnO@C(30) ZnO@ZIF-8 0.02~3.0 100/1000 100/300 539/498 1065/664 62 — 216
Co-doped ZnO@C Co-MOF-5s 0.01~3.0 100 50 725 903/- — — 217
Ti-doped-CoO@C Co-Ti-MOF 0.01~3.0 200 150 1180 1749/830.7 — 241.4 218
C/CoTiO3 Co-MOF 0.005~3.0 100/2000 100/1400 630/610 -/- 75.8 62.2 220
NiFe2O4/N-C NiFe-MOF 0.005~3.0 100/500 50/50 760/610 1193/773 64.8 146.2 221
NiFe2O4/CNTs Fe2Ni MIL-88 0.01~3.0 100/2000 100/100 624.6/250 1348/1030 76.4 70.73 222
CNTs@ZnCo2O4 ZIF-8 0.01~3.0 100 100 750 682.7/435.6 — 78 167
CoFe2O4/GNS Co-Fe-BTC 0.01~3.0 100 100 1061.7 1413/1058 — 24.5 225
Zn0.5MnO@C Zn-Mn-BTC — 100/5000 200 /500 1050/408 1565.9/954.6 — 30.8 226
MnO-doped Fe3O4@C Mn-doped MIL-53
(Fe)		 0.01~3.0 200 200 1297.5 1281.4/938.6 73.3 63.3 227
Co3O4/NiO/C CoNi-MOFs 0.01~3.0 1000 1000 776 1522/907 — 136 229
Fe-Mn-O/C Fe/Mn-MOF-74 0.0~3.0 100 200 1294 1333/837 — 158.2 230
Co3O4@CuO
@GQDs		 Co-Cu-BTC 0.005~3.0 100 200 1054 1352/816 60 36 231
ZnO/ZnFe2O4/C MOF-5 0.005~3.0 500/2000 100/100 1390/988 1385/1047 75.6 140 232
ZnO/Ni3ZnC0.7/C Zn-MOF/Ni 0.01~3.0 500 750 1002 1743/1015 58.2 112 233
ZnO/ZnFe2O4@C ZFC 0.01~3.0 1000 500 718 1392/1059 76.1 80 234
C@ZnO/ZnCo2O4/CuCo2O4 Co-Cu-ZIF-8 0.01~3.0 300/3000/10000 500/500/500 1742/1009/664 2430/1967 80.1 549.7 235
图6 (a)合成过程示意图, (b) SEM图像, (c) 高分辨TEM图像,(d) 合成的MoS2?C的STEM-EDS分布 ((c)的内部为SAED谱)[261]
Fig. 6 (a) Schematic illustration of the fabrication process, (b) SEM image, (c) high-resolution TEM image and (d) STEM-EDS mapping of the as-synthesized MoS2?C hybrids (inset of (c) showing the corresponding SAED pattern)[261]
表7 金属硫化物/碳基复合负极材料及其电化学性能
Table 7 Metal sulfide/carbon-based composites as anode materials and their electrochemical performances
Materials Template/precursor Voltage range (V) Current density (mA/g) Cycle
number		 Overall Capacity (mAh/g) Initial discharge capacity/charge capacity (mAh/g) Initial
coulomb
efficiency
(%)		 Specific surface area (m2/g) ref
H-Co9S8@C Co-MOF-74 0.01~3.0 100/500 250/50 900.5/655 1119.5/867.3 77.4 127.1 238
Co9S8@NMCN ZIF-67 0.01~3.0 100 80 988 1705/1125 66 76.9 239
Co9S8/N-C ZIF-67 0.01~3.0 544 400 784 1260/900 71.48 125.9 240
Co9S8/S-NC ZIF-67 0~3.0 1000 300 500 879.7/529.3 60.17 150.5 242
Co9S8/NSC Sulfonate-based Co-MOF 0.01~3.0 100/2000 200/1000 1179/789 1816.9/862 47.5 228.1 243
CoS@PCP/
CNTs-600		 ZIF-67 0.01~3.0 200 100 1668 2083/1246 — 101.5 245
NC/CoS2-650 ZIF-67 0.1~3.0 100/2500 50/50 560/410 1100/ — — 246
CoS2-N-C/3DGN Co-MOF 0.01~3.0 100 100 409.5 833.5/666.3 79.9 — 247
CoS2/NSCNHF ZIF8@ZIF67 0.01~3.0 100/1000 100/200 845/549.9 1155.6/739.6 64 234.25 248
Co3S4/MNCNT ZIF-67/MWCNT 0.01~3.0 200/2000 50/500 1281.2/976.5 1644.2/1055 64.17 112 249
Co1-xS/C Co-BTC 0.01~3.0 200/1000 100/700 791/667 1290/932 72 124 250
FeS/C Fe-MOFs 0.01~3.0 100 150 830 1702/972 57 0.015 251
FeS2@POC Fe-MOFs 0.01~3.0 100/2000 100/200 1074/607 1394/1115 80 44.2 252
C@Fe7S8 MIL-88 0.01~3.0 500 170 1148 1072/761 71 277 253
ZnS/PC MOF-5 0.01-2.5 100 300 438 1220/- — 296.8 254
ZnS@NC ZIF-8 0.01~3.0 200/500 150/450 521.8/853 1284.9/840.6 34.6 191.45 255
α-MnS/SCMFs/Cu Mn-MOF 0.01~3.0 200/1500 300/1000 1383/601 1115/- 69 109 258
MoS2@NC-2 ZIF-8 0.005~3.0 100 50 715 1864/- 50 — 259
ZnCoS@Co9S8/NC ZIF-67@ZIF-8/
ZIF-67		 0.01~3.0 500/2000 500/400 1814/1095 2895/2182 — 270.46 263
表8 其他金属化合物/碳基复合负极材料及其电化学性能
Table 8 Other metal compounds/carbon-based composites as anode materials and their electrochemical performances
Materials Template/precursor Voltage range (V) Current density (mA/g) Cycle
number		 Overall Capacity (mAh/g) Initial discharge
capacity/charge
capacity
(mAh/g)		 Initial
coulomb
efficiency
(%)		 Specific surface area (m2/g) ref
CoSe@PCP ZIF-67 0.005~3.0 200/1000 100/500 675/708.2 902/603 73.5 76.94 264
3DG/Fe7Se8@C 3DG/MOF 0.01~3.0 200/1000 120/250 884.1/815.2 — — — 265
Ni-Co-Se/C-600 Ni-Co-BTC 0.01~3.0 1000/3000 500/900 1514/852 821/634 77 127 266
Bi2Se3@C Bi-MOF 0.01~3.0 200/1000 200/5000 637/543 -/642 68 76 267
ZnSe/NC-300 ZIF-8 0.01~3.0 100 500 724.4 906.66/547.48 60.3 93.926 268
Ni2P/NC MOF-Ni 0.01~3.0 500 800 450.4 1240.5/649.5 — 34.5 269
CoP/C ZIF-67 0.01~3.0 500 1000 523 1522/1110 72.9 67.2 270
CoxP-NC-800 ZIF-67 0.01~3.0 100/1000 100/1800 1224/400 2450/1469 — 326.5 271
MoC@C-700 Mo3(BTC)2 0.01~3.0 1000 500 509.8 990.8/674.3 65.3 187 272
图7 (A) SnZCw前驱体和(B)不同放大倍数的SnZCw的SEM图像;SnZCw的(C) TEM图像、(D) HRTEM图像和(E) 选区电子衍射; (F) 不同放大倍数的SnZCd TEM图像[276]
Fig. 7 SEM images of (A) the precursor of SnZCw, and (B) SnZCw at different magnifications; (C) TEM image, (D) HRTEM image, and (E) the SAED pattern of SnZCw; (F) TEM images at different magnifications of SnZCd[276]
表9 金属/金属氧化物/碳基复合负极材料及其电化学性能
Table 9 Metal/metal oxide/carbon-based composites materials as anode materials and their electrochemical performances
Materials Template/precursor Voltage range (V) Current density (mA/g) Cycle
number		 Overall Capacity (mAh/g) Initial discharge
capacity/charge
capacity
(mAh/g)		 Initial
coulomb
efficiency
(%)		 Specific surface area (m2/g) ref
Co3O4/Co/C ZIF-67 0.01~3.0 100/2000 60/600 801/505 1158/867 75 183.9 274
Co/Co3O4@N-C-700 NUM-6 0.01~3.0 100/1000 100/100 903/774 1535/830 — 250.4 275
Sn/C-ZnO ZIF-8 0.01~3.0 100 50 515.6 1118.7/- 64.2 32.9 276
SnO2/Co@C CoSnO3 @MOF 0.01-2.5 200/5000 100/1800 800/400 1300/857 66 84 277
NiO/Ni/Graphene Ni-MOFs 0.005~3.0 2000 250 1180 1759/1144 — 104 278
Ni@ZnO/CNF Ni@ZIF-8 0.01~3.0 100 100 1051 1547/1100 71 38.6 279
表10 MOFs及其衍生负极材料的优点和缺点
Table 10 Advantages and disadvantages of MOFs and their derivative anode materials
Materials Advantages Disadvantages
MOFs abundant active sites
large specific surface area
high porosity
adjustable composition, morphology and structure
low cost		 low conductivity
poor structure stability
fast capacity decay
Porous carbon large specific surface area
high porosity
simple synthesis method and mild synthesis condition
high thermal stability
no subsequent complex physical or chemical activation		 insufficient capacity
uncontrolled structure evolution
inherent structure properties determined from micropore
Single metal oxide simple synthesis method
controllable synthesis path
Large specific surface area
high porosity
controlled structure and composition		 limited species
lower conductivity
easy volume expansion and pulverization
lower rate capability and cycle performance
Double metal oxides stronger synergistic effect between different metal elements
abundant redox sites
faster reaction kinetics and activity		 lower conductivity
easy volume expansion and pulverization
lower rate capability and cycle performance
Other metal compounds wide variety
good mechanical and thermodynamic stability
higher theoretical capacity		 complicated synthesis process
higher cost
lower reaction kinetics under high load
lower utilization
MOFs/ Metal oxide abundant active sites
high porosity
alleviated volume expansion and pulverization		 lower conductivity
MOFs/C high porosity
better structure stability
higher conductivity		 limited capacity
Metal oxide/Metal oxide stronger synergistic effect between different metal elements
improved electrode integrity
alleviated volume effect		 lower conductivity
easy volume expansion and pulverization
limited capacity and cycle stability
Metal oxide/C higher conductivity
better structure stability
faster electron transportation
stronger synergistic effect		 complicated synthesis method
uncontrolled synthesis condition
Metal sulfide/C higher conductivity
better structure stability
stronger synergistic effect		 slower reaction kinetics
faster capacity decay
Other metal compounds/C abundant active sites
higher utilization rate of active substances
faster electron transportation
stronger synergistic effect		 insufficient performance under high load
ambiguous reaction mechanism
Metal/Metal oxide/C higher conductivity
better structure stability
faster electron transportation
stronger synergistic effect		 complicated synthesis process
ambiguous reaction mechanism
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