Research progress of MOFs-derived materials as the electrode for lithium–ion batteries — a short review
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摘要: 金屬有機框架材料 (Metal-organic frameworks，MOFs）是一種新穎的多孔晶體材料，具有比表面積大、孔隙率高、結構可設計性強等優點，但是，MOFs的低電導率以及在電解液中的穩定性等問題限制了其作為電極材料的應用。近年來，如何結合MOFs的優勢進行鋰離子電池電極材料的設計與合成受到了越來越多的關注。目前，通過自犧牲得到的多孔碳骨架和金屬化合物等MOFs衍生復合電極材料，不僅解決了電導率低的問題，而且保留了MOFs的高比表面積和復雜多孔結構，為鋰離子的插入/脫出、吸附/解吸等過程提供了豐富的活性位點；與此同時，從結構單元和化學組成方面增加了材料結構的復雜性，開放性的孔隙結構可以緩沖體積膨脹帶來的機械應力，對外來離子存儲和多離子傳輸具有重要的意義。本文綜述了MOFs及其衍生物在鋰離子電池電極材料的設計和研究中取得的最新進展，重點闡述了針對鋰離子電池電極材料的要求進行MOFs形貌控制和修飾的方法，以及具有多孔、中空或特殊結構的MOFs衍生電極材料的制備關鍵影響因素及其結構特性對電化學性能的影響。最后，分析了MOFs衍生電極材料的研究挑戰和發展方向。Abstract: Owing to their high surface area, excellent electrolyte permeability and ample diffusion pathways for charge transport, porous and hollow-structured electrochemically active materials attract more attention as the electrodes. In general, the process of template preparation method is used to achieve hollow structured materials over the last few decades. However, the complicated preparation process including removal of template and surface modification often results in poor uniformity, low reproducibility, and high cost of porous structure. Moreover, it incorporates functional chemicals with specific homogeneity and dispersity into the hollow porous intercrystalline structure. These problems hinder the development and application in energy storage and conversion devices of the diversified porous and hollow-structured materials. The metal-organic frameworks (MOFs), consisting of organic linkers and coordinated inorganic clusters, appear as an excellent collection of porous crystal material series with high surface areas, high porosity, and tunable structures. However, their low conductivity and electrolyte instability limit the further use of MOFs in the field of LIBs. Recently, how electrode materials for Lithium–ion batteries (LIBs) are designed and prepare using MOFs has attracted more attention. The composite materials derived from MOFs including nanostructured porous carbons and metal oxide uaing self-sacrificial template synthetic route not only solves the problem of low conductivity but also maintains the high surface area and porous structure of MOFs, providing abundant active sites for insertion/deinsertion or adsorption/desorption; Furthermore, composite materials derived from MOFs increase the complexity of nanostructures in terms of structural units and chemical components. In particular, large pore volume and open pore structure are critical to loading guest species, accommodating mechanical strains and facilitating mass transport. In this paper, we briefly examined the production of MOF-derived materials for applications in LIBs. The optimization and modification of an MOFs morphology were implemented according to the electrode material requirement for LIBs. Moreover, the preparation of MOFs-derived electrode materials with porous, hollow, or complicated construction and their effects on electrochemical performance were described. Finally, the challenge and trend in production of electrode materials derived from MOFs were analyzed.
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Key words:
- lithium ion battery /
- electrode material /
- metal organic frameworks /
- porous structure /
- cycle life
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圖 1 本綜述主要內容的示意圖，主要包括具有多孔、中空及特殊結構的MOFs衍生鋰離子電池電極材料
Figure 1. Schematic of the main contents of the review, including porous, hollow, and complicated construction of electrode materials derived from MOFs
圖 2 不同尺寸的聯吡啶基有機配體合成金屬有機框架的示意圖（a）[18]；ZIF?8經過溶劑輔助更換配體后孔徑擴張示意圖（b）[20]；利用不同熱穩定性的連接體制備HP?UiO?66的示意圖（c）（A~J代表著不同配體的熱穩定性）[21]
Figure 2. Schematic diagram (a) of the synthesis of metal organic frames using different sizes of bipyridyl organic ligands[18]; aperture expansion in ZIF?8 via solvent-assisted linker exchange (b)[20]; versatility of linker thermolysis to construct HP?UiO?66 using various linkers (c) (A–J showing different thermal stability)[21]
圖 4 具有豐富氮摻雜的ZIF?8衍生碳粒中額外鋰離子存儲機理示意圖（a）[36]；MIL?88?Fe的掃描電鏡圖，合成紡錘狀多孔α-Fe2O3的流程圖，以及在200 mA·g?1電流密度下紡錘狀多孔α-Fe2O3和塊狀Fe2O3循環性能對比（嵌入圖）（b）[46]；合成CoxP?NC多面體的流程示意圖，以及CoxP?NC?700, CoxP?NC?800和CoxP?NC?900電極材料倍率性能的對比圖(c)[47]
Figure 4. Schematic representation (a) of extra Li storage in N-doped ZIF?8 derived carbon particles[36]; SEM image of as-prepared MIL?88?Fe, the illustration of the fabrication of spindle-like porous α-Fe2O3, and comparative cycling performance of the final spindle-like α-Fe2O3 and bulk Fe2O3 at 200 mA·g?1 (inset) (b)[46]; Schematic illustration of the formation of CoxP?NC polyhedra, and rate performance of the CoxP?NC?700, CoxP?NC?800 and CoxP?NC?900 electrodes at different rate current densities (c)[47]
圖 5 交織異質結構示意圖，Co3O4?C@FeOOH交織中空多面體結構的形成過程，以及微觀形貌和循環性能對比圖（a）[56]；NiO/Ni/石墨烯復合材料合成示意圖，以及NiO/Ni/石墨烯復合材料的掃描電鏡圖（b）[59]。
Figure 5. Schematic of interwoven heterostructure, schematic showing the formation process of crystalline–amorphous Co3O4/FeOOH interwoven hollow polyhedrons structure, and SEM image and cycling performance (a)[56]; Schematic of the formation of NiO/Ni/Graphene composites, and SEM images of NiO/Ni/Graphene composite (b)[59]
圖 6 鐵基MOFs及其衍生的Fe2O3納米結構的掃描電鏡圖像（a）[68]；3D中空CoS@PCP/CNTs的合成示意圖，以及0.3?10 A·g?1不同電流密度下CoS@PCP/CNTs的放電比容量（b）[69]。
Figure 6. SEM images (a) of Fe-based MOFs and their derived Fe2O3 nanostructures[68]; schematic for the formation of 3D hollow CoS@PCP/CNTs, and rate capabilities of CoS@PCP/CNTs at various current densities between 0.3 and 10 A·g?1 (b)[69]
表 1 熱解后得到的MOFs材料HP?UiO?66的孔隙參數[21]
Table 1. Porosity parameters of HP?UiO?66 created by linker thermolysis[21]
Sample SBET/(cm3·g?1) Dmeso/nm V(meso)/V(micro) HP?UiO?66?AD 1022 9.8 0.83 HP?UiO?66?BD 1012 7.5 0.60 HP?UiO?66?CD 825 7.2 0.82 HP?UiO?66?AE 702 5.5 0.79 HP?UiO?66?AF 571 6.0 1.00 HP?UiO?67?GH 2185 14.8 0.66 
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表 2 幾種以MOFs為前驅體制備的多孔納米碳基電極材料
Table 2. Some porous carbon-based electrode nanomaterials prepared using MOFs
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表 3 幾種以MOFs為前驅體制備的多孔金屬化合物或金屬化合物/碳復合電極材料
Table 3. Some porous metal compounds or metal compound/carbon composite electrode materials prepared using MOFs
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久色视频表 4 幾種以MOFs為前驅體制備的具有中空結構的復合電極材料
Table 4. Some hollow composite electrode materials prepared using MOFs
Sample Precursor Capacity/(mA·h·g?1) Cycle number Voltage / (V vs Li/Li+) Current density /(mA·g?1) Reference Multishell microsphere Co3O4@C Ni/Co?MOF 1701 60 0.01?3 100 [60] CoSe@C nanoboxes ZIF?67 787 100 0.01?3 200 [61] Hollow CoS2 ZIF?8/67 549.9 200 0.01?3 1000 [62] Hollow Fe2O3/SnO2 PB 500 100 0.05?3 200 [63] Double-Shelled Nanocages CH@LDH ZIF?67 653 100 0.01?3 65 [64] Microboxes Fe2O3 PB 950 30 0.01?3 200 [65] Nanobubble Hollow CoS2 ZIF?67 737 200 0.05?3 1000 [66] Nanobowls CMS/NSC NB 218.6 8240 0.01?2.5 5000 [67]
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