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2222材料工程  2021, Vol. 49 Issue (9): 27-40    DOI: 10.11868/j.issn.1001-4381.2020.000599
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基于MOFs的碳纳米管复合材料的制备和应用进展
乔俊宇, 李秀涛()
中国民航大学 民航热灾害防控与应急重点实验室, 天津 300300
Progress in preparation and application of carbon nanotube composites based on MOFs
Jun-yu QIAO, Xiu-tao LI()
Key Laboratory of Civil Aviation Thermal Hazards Management and Emergency Response, Civil Aviation University of China, Tianjin 300300, China
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摘要 

碳纳米管（CNTs）作为纳米材料研究中的一个重要发现，自其诞生以来就成为碳材料领域的研究热点之一。金属有机框架（MOFs）凭借其独特的多孔结构，近年来在各领域的应用已经成为研究前沿之一。随着材料科学的不断发展，对具有不同功能特性材料的复合技术研究，已经成为解决材料应用领域中关键问题的主要方法。而碳纳米管和金属有机框架作为目前材料领域两类十分重要的纳米材料，通过复合技术将碳纳米管的高导电特性和金属有机框架材料的高比表面积、丰富孔道分布特性相结合是研究与应用的必然趋势。本文综述了近年来金属有机框架和碳纳米管的主要复合形式和制备方法，整理了复合材料在超级电容器、锂电池、催化、吸附等领域的最新研究进展，对两种材料性能的协同提升方面进行了讨论和总结，并指出CNTs与MOFs材料的复合以及CNTs的生长分布具有很高的随机性，对其实现进一步控制是未来的技术研究重点。
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乔俊宇
李秀涛
关键词 ： 碳纳米管,  金属有机框架,  复合材料,  原位生长    
Abstract：

Carbon nanotubes(CNTs), as an important discovery in the research of nanomaterials, have become a research hotspot in the field of carbon materials since their birth. With its unique porous structure, metal-organic frameworks (MOFs) has been developed into one of the frontiers of research in recent years. With the continuous development of materials science in recent years, the research on composite technology of materials with different functional characteristics has become one of the main methods to solve key problems in the field of materials applications.CNTs and MOFs are two very important types of nanomaterials in the current material field. Combining the high electrical conductivity of CNTs with the high specific surface area and rich pore distribution characteristics of MOFs through composite technology is an inevitable trend for future research and application in the field of materials. In this paper, the main composite forms and preparation methods of MOFs and CNTs in recent years were reviewed, and the latest research progress of composites in the fields of supercapacitors, lithium battery electrodes, catalysis, adsorption, etc. was summarized. The synergistic improvement of the performance of the two materials was discussed and analyzed, and it was pointed out that the composite of CNTs and MOFs materials and the growth and distribution of CNTs have a high degree of randomness, and further control of them is the focus of future technical research.
Key words： carbon nanotube    metal-organic framework    composite    in-situ growth
收稿日期: 2020-07-01      出版日期: 2021-09-17
中图分类号:  O6-1  
基金资助:中国民航大学科研启动费项目(2020KYQD06)
通讯作者: 李秀涛     E-mail: xiutaolee@163.com
作者简介: 李秀涛(1984-), 男, 讲师, 博士, 研究方向: 基于MOFs的多功能材料, 联系地址: 天津市东丽区中国民航大学民航热灾害防控与应急重点实验室(300300), E-mail: xiutaolee@163.com
引用本文:   
乔俊宇, 李秀涛. 基于MOFs的碳纳米管复合材料的制备和应用进展[J]. 材料工程, 2021, 49(9): 27-40.
Jun-yu QIAO, Xiu-tao LI. Progress in preparation and application of carbon nanotube composites based on MOFs. Journal of Materials Engineering, 2021, 49(9): 27-40.
链接本文:  
http://jme.biam.ac.cn/CN/10.11868/j.issn.1001-4381.2020.000599      或      http://jme.biam.ac.cn/CN/Y2021/V49/I9/27
Fig.1  MOFs/CNTs复合材料制备方法示意图
Fig.2  HKUST-1@CNTs的SEM图(a)[42]，ZIF-67@MWCNTs的TEM图(b)[43]，HKUST-1@VACNT的SEM图(c)[45]和ZnO@NC@CNTs的TEM图(d)[46]
Mental salt Organic ligand Solvent Pretreatment Atmosphere Carbonization temperature/℃ Carbonization rate/(℃·min-1) Time/h Ref
Zn(CH3COO)2·2H2O
Co(CH3COO)2·4H2O		 2-methylimidazole Methanol － N2 800 2 5 [47]
Co(NO3)2·3H2O Sodium dicyanamide/pyrazine Hot H2O － N2 700-1000 10 3 [49]
Co(NO3)2·6H2O 2-methylimidazole Methanol/ethanol － Ar/H2 700-1000 2 3.5 [50]
Ni(CH3COO)2·4H2O 1, 4-benzenedi-carboxylic acid DMF － N2 800 － 8 [51]
Co(NO3)2·6H2O Bib/H2BDC CH3OH/H2O － N2 800 2 5 [52]
Zn(NO3)2·6H2O
Co(NO3)2·6H2O		 2-methylimidazole Methanol Double solvent N2 600 5 2 [53]
Co(NO3)2·6H2O 2-methylimidazole Methanol Grind dicyandiamide N2 700 2 2 [54]
Zn(NO3)2·2H2OFeCl3·6H2O 2-methylimidazole H2O Grind pyrazine/ impregnation N2 800 5 2 [55]
FeCl3·6H2O H2BDC DMF Grind melamine N2 600-800 10 5 [56]
Co(NO3)2·6H2O 2-methylimidazole Methanol Impregnation NaOH/CTAB N2 700-900 5 3 [48]
Table 1  MOFs原位生长CNTs制备方法
Fig.3  CoSe2@DC的TEM图(a)[47]，Co/Zn-ZIF-NPC(b)[57]和Co@BNCNTs[49]的SEM图(c)
Fig.4  CNT-UiO-66的SEM图(a)[61]，ZnO/CNT的TEM图(b)[66]及不同电流密度下Ni-MOF/CNTs的比电容(c)[62]
Composite Sample Current density Specific capacitance Max energy density Max power density Cycle/Retention Ref
MOF@CNTs CNTs@Mn-MOF 0.5 A/g 203.1 F/g 6.9 Wh/kg 2240 W/kg 3000/88% [60]
CNT-UiO-66 0.05 mA/cm2 4.9 mF/cm2 － － 2000/88% [61]
Ni-MOF/CNTs 0.5 A/g 1765 F/g 36.6 Wh/kg － 5000/95% [62]
RGO/CNTs-ZIF-8 1 mA/cm2 961 mF/cm2 3000/90% [63]
Ni-MOF@CNT/GN 1 mA/cm2 898 mF/cm2 0.34 mWh/cm2 － 4000/93% [64]
IITI-1@CNT 1.6 A/g 380 F/g － － 4000/63.63% [44]
MOF/CNTs Ni-CoP@C@CNT 1.0 A/g 708 F/g 17.4 Wh/kg － 3000/76.1% [65]
derived composite HKUST-1/CNT 2 A/g 194.8 F/g 9.1 Wh/kg 3500 W/kg 10000/95% [42]
ZIF-8/CNTs 1 A/g 250 F/g 23.6 Wh/kg 16900 kW/kg 3000/96.1% [66]
MOF in-situ Co/Zn-ZIF-NPC 2.5/Ag 286 F/g － － 10000/－ [47]
preparation of Ni-MOF@CNT 0.5 mA/cm2 272 mF/cm2 0.054 mWh/cm2 5.99 mW/cm2 5000/100% [51]
CNTs composite CoS2@CNTs 0.5 A/g 825 F/g － － 5000/82.9% [52]
Table 2  MOF@CNTs及其衍生复合材料电容器性能参数
Fig.5  CNTs/MOFs-C/Al2(OH)2.76F3.24/S的循环特性图(a)[69], CNT@Co-N-C/S的恒流充放电图(b)[54], MWCNTs/Co3O4(c)[43]和CZO@C/CNT(d)[53]的TEM图
Composite Sample Current density/(mA·g-1) Cycle Specific capacity/(mAh·g-1) Ref
MOF/CNTs derived Ni-Sn-P@C-CNT 100 200 704 [67]
composite CoP@C-CNTs 100 100 692 [68]
C/Al2(OH)2.76F3.24/S 500 300 889 [69]
ZCS@NC/CNTs 500 500 873 [70]
MWCNTs/MCo2O4 100 100 813 [43]
ZnO@NC@CNTs 100 100 850 [46]
MOF in-situ preparation CZO@C/CNT 100 100 758 [53]
of CNTs composite CNT@Co-N-C/S 0.2 C 500 970 [54]
Table 3  MOF@CNTs及其衍生复合材料电极材料性能参数
Fig.6  ZIF-8@CNTs(a)[73]和Co@BNCNTs(b)[57]的SEM图，ZIF-67/CNT和CoSe2@NC-NR/CNT微观结构示意图(c)[74]及双功能催化剂Co-N/PC@CNT的催化性能(d)[79]
Composite Sample ORR OER Loading/(mg·cm-2) Ref
Eonset/V E1/2/V Eonset/V E1/2/V
MOF@CNTs Co-MOF@CNTs 0.91 vs RHE 0.82 1.51 vs RHE 1.577 0.3 [72]
MOF/CNTs derived composite ZIF-8/CNTs 0.8-0.9 vs RHE － － － 0.3 [73]
MOF in-situ Co-ZnO@NC/CNT 0.90 vs RHE 0.86 － － 0.24 [77]
preparation of CNTs Co-CNT/PC 0.918 vs RHE － － － 0.5 [78]
composite Co@BNCNTs 0.93 vs RHE 0.82 － － 0.3 [57]
Fe3C/b-NCNT 0.96 vs RHE － － － 0.42 [55]
Fe/Fe3C@NGL-CNT 0.04 vs Ag/AgCl － － － [56]
Co-N/PC@CNT 0.92 vs RHE 0.78 1.45 vs RHE 1.63 0.25 [79]
Co/N-CNTs -0.005 vs Ag/AgCl ―0.154 － － 0.3 [48]
Table 4  MOF@CNTs复合材料催化性能参数
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