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化学进展 2022, Vol. 34 Issue (2): 460-473 DOI: 10.7536/PC201113 前一篇   后一篇

• 综述 •

双金属MOFs及其衍生物在电化学储能领域中的应用

王雨萌1, 杨蓉1,2,*(), 邓七九2, 樊潮江1,2, 张素珍1, 燕映霖1   

  1. 1 西安理工大学复合材料及其产品智能制造技术国际联合研究中心 西安 710048
    2 西安理工大学材料科学与工程学院 西安 710048
  • 收稿日期:2020-11-09 修回日期:2021-03-09 出版日期:2022-02-20 发布日期:2021-07-29
  • 通讯作者: 杨蓉
  • 基金资助:
    国家国际科技合作专项项目(2015DFR50350); 国家自然科学基金项目(51702256); 中国博士后面上资助项目(2019M653706); 陕西省科技厅“创新人才推进计划-科技创新团队”项目(2019TD-019); 陕西省博士后科研资助项目(2018BSHEDZZ120)
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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:2020-11-09 Revised:2021-03-09 Online:2022-02-20 Published:2021-07-29
  • 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)

双金属有机骨架及其衍生物一方面具有单金属有机骨架孔道丰富、比表面积大、结构可调、活性位点丰富等特点,另一方面具有双组分与多孔结构之间的协同效应,因而受到了研究人员的密切关注,在储能、催化、分离、传感器、医药、气体存储等领域广泛应用。和单金属MOFs类似,双金属MOFs的导电性不佳、结构易坍塌,这极大地限制了其在电化学储能中的应用。通过对双金属MOFs进行热处理,易得到分布均匀的多孔碳@双金属氧化物/硫化物/磷化物/硒化物等衍生物,不仅保持了独特的多孔结构,而且提高了材料的导电性和结构稳定性,有利于在电化学储能中的应用。因此,本文从双金属MOFs中的主要金属离子入手,综述了双金属MOFs及其衍生物用于超级电容器、锂离子电池、钠离子电池、金属空气电池等电化学储能器件的最新应用进展。在此基础上,总结了双金属MOFs在电化学储能应用中的优势,并对其制备、作用机理和后处理研究提出了建议。

关键词： 双金属MOFs, 衍生物, 电化学储能

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
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图1 不同金属空气电池的理论能量密度
Fig. 1 The theoretical energy densities of different metal-air batteries
表1 双金属MOFs及其衍生物的制备
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
图2 EC@NiCo2S4的合成示意图[44]
Fig. 2 A schematic diagram of the preparation of EC@NiCo2S4[44]
表2 钴基双金属MOFs及其衍生物在超级电容器中的电化学性能
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
图3 NiCoP的(a, b)SEM,(c, d)TEM,(e)高分辨率TEM图像[41]
Fig. 3 (a, b) SEM images, (c, d) TEM images, (e)High resolution TEM image of NiCoP[41]
图4 (a)Co3O4@CuO@GQDs的合成示意图,(b)Co3O4@CuO@GQDs和Co3O4@CuO在0.1 A·g-1下的循环性能[34]
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]
图5 M-FeCo-N-C-X催化剂的制备工艺[13]
Fig. 5 Illustration of the overall fabrication process for the M-FeCo-N-C-X catalysts[13]
表3 镍基双金属MOFs的微观形貌
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
图6 以FeNi3Cx-Pd-7%和Pt/C+RuO2为空气阴极的RZABs的性能。(a)自组装RZAB的原理图,(b)放电极化曲线和相应的功率密度图,(c)开路电压图,(d)10 mA·cm-2时的恒电流放电比容量曲线,(e)10 mA·cm-2下的恒电流充放电循环曲线,每次循环持续10 min,(e)的插图是由两个串联的RZABs供电的LED的光学照片,使用负载FeNi3Cx-Pd-7%的碳纤维纸作为空气阴极[29]
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]
图7 (a)NPC-300-900和NPC-5-900的N2等温吸-脱附曲线,(b)NPC-300-900和NPC-5-900的孔径分布[65]
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]
图8 Mn@ZnO/CNFs制备示意图。上排:静电纺丝装置、Mn@ZnO/CNFs的SEM图像、为LED供电的柔性电极照片;下排:CNFs负载Mn@ZIF-8、Mn@ZIF-8的原子结构、显示电极样品柔韧性的照片[33]
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]
图9 CNCo-5@Fe-2催化剂对ORR的电催化机理[66]
Fig. 9 Electrocatalytic mechanism of CNCo-5@Fe-2 catalyst for ORR[66]
图10 (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的SEM图像[70]
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]
图11 MnS-(ZnCo)S/N-C复合材料的SEM图像[73]
Fig. 11 SEM images of the MnS-(ZnCo)S/N-C composite[73]
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