随着不可再生能源的过度消耗，全球正面临着能源短缺与生态污染的双重挑战。在此背景下，构建高效的储能装置以实现可再生能源的有效收集与利用，已成为解决能源问题的关键途径。开发高性能电极材料以提升超级电容器的储能性能，对于应对日益增长的能源需求具有重要意义。纤维素作为自然界中储量最丰富的天然高分子化合物，其独特的多层次结构特征，为其在储能领域的应用提供了良好的基础。然而，传统纤维素材料主要依赖双电层电容机制进行储能，且多局限于负极应用，这严重制约了其在超级电容器领域的进一步发展。针对上述问题，本研究以基于纤维素开发高性能电极材料为目标，通过引入金属有机框架（MOF）和金属氧化物等活性组分，对电极材料的物理化学性质进行调控，从而优化其导电性能与电化学特性。MOF是一种由金属离子或金属簇与有机配体通过配位键连接而成的具有框架结构的材料，具有高比表面积、可调控的孔径结构以及丰富的活性位点等优点，通过将MOF与纤维素材料复合，可以有效提高电极材料的比表面积和孔隙率，从而增强其电化学活性。此外，金属氧化物（如MnO、Bi₂O₃等）因其高理论比容量和优异的氧化还原活性，也被广泛用作超级电容器电极材料，通过引入金属氧化物可以提升纤维素基复合材料的赝电容性能，从而提高其能量密度。具体研究内容及结果如下：

1. 通过溶剂热法和超声法设计得到基于微晶纤维素的正负极材料。将微晶纤维素与具有独特孔道结构的镍基MOF（5-N-TPPA-MOF）复合，成功制备了一系列复合正极材料，并通过研究掺杂量对电化学性能的影响，制备了具有优异性能的cello-MOF-5-N，并且在微晶纤维素表面负载铋金属，开发了新型cello-Bi负极材料。基于这一设计思路，构建了以微晶纤维素为基底的不对称双电极体系，该体系不仅有效地缓解了电极间的电势差问题，还地提升了导电性能。实验结果表明，在0.2 A g^-1电流密度下，该双电极体系的比容量达到222 C g^-1，在1 A g^-1的电流密度下，功率密度达749 W kg^-1时，能量密度达到40 W h kg^-1。对电极材料在循环前后结构与价态的变化进行分析发现，微晶纤维素的引入增强了电极材料的导电能力，提升了电荷与离子在材料表面的转移效率；MOF材料中三齿长臂配体的引入，增强了镍活性中心的分散性，提高材料的氧化还原能力，强吸电子集团的存在能够有效提高材料的离子传输能力；掺杂在负极材料中的金属铋带来了丰富的电化学反应位点。

2. 通过在正极材料的MOF中引入氨基化功能配体，在负极材料中引入MnO材料，开发基于微晶纤维素的电极材料，由上述电极材料构筑的不对称超级电容器体系在电流密度为0.2 A g^-1时，比容量达到400 C g^-1，在电流密度为1 A g^-1时，该体系的功率密度为723 W kg^-1，能量密度为43 W h kg^-1。正极材料中，氨基化功能配体的引入，提高了材料的亲水性，增强了离子与电荷在材料表面的传输，提高了材料的导电性能，而且MOF材料中直径7 Å的一维螺旋孔道结构对于电荷与离子在材料表面的运输也起到了关键作用。负极材料中，氧化锰在纤维素基材料表面的均匀分布且二者以较强化学键相连，既促进了金属活性中心在材料表面的分散性，提升了复合材料的氧化还原活性，同时减少了氧化锰在电解液中的溶出，增强了复合材料的稳定性。

3. 通过进一步优化材料设计策略，引入具有独特三维结构和优异物理特性的细菌纤维素作为新型基底材料，开发了具有更高性能的超级电容器电极材料。将氧化铋与细菌纤维素衍生物复合，开发了bi-cello-Bi₂O₃负极材料，基于5-羟基间苯二酸的MOF材料（5-H-TPPA-MOF）与细菌纤维素结合，制备了高性能正极材料（bi-cello-MOF-5-H），二者组装构建的不对称超级电容器（bi-cello-MOF-5-H//bi-cello-Bi₂O₃）在0.2 A g^-1电流密度下的比容量为412 C g^-1，在1 A g^-1的电流密度下，该体系的功率密度为751 W kg^-1时，能量密度达到52 W h kg^-1。通过在材料体系中引入含羟基配体，其羟基官能团与细菌纤维素分子链上的羟基形成稳定的分子间氢键网络，这种相互作用不仅增强了复合材料的机械稳定性，而且促进了离子和电荷在材料表面的运输。引入具有多价态特性的铋复合氧化铋于负极材料中，通过循环前后XPS分析证实，Bi⁰/Bi³⁺/Bi⁵⁺氧化还原电对在充放电过程中表现出可逆的价态转变。

4. 通过引入对硝基苯甲酸作为有机配体，成功合成了正极材料（bi-cello-MOF-4-N）。在本章研究中，正极材料的设计得到了优化，还沿用了前一章设计的新型负极材料（bi-cello-Bi₂O₃），构建了不对称超级电容器双电极体系，即以细菌纤维素功能化的bi-cello-MOF-4-N作为正极材料，结合由细菌纤维素衍生物功能化的铋基复合材料（bi-cello-Bi₂O₃）作为负极材料，成功组装了高性能的不对称超级电容器。该体系在0.2 A g^-1电流密度下可以达到487 C g^-1的容量，在1 A g^-1的电流密度下，体系的功率密度达到750 W kg^-1时，能量密度可以达到87 W h kg^-1。本研究采用对硝基苯甲酸作为功能配体构筑MOF材料，材料中直径9 Å的孔道结构以及邻近的镍离子中心缩短了电荷在材料表面的传输路径，并暴露出更多具有氧化还原活性的金属位点。

实验研究表明，通过对微晶纤维素、细菌纤维素等不同来源纤维素进行功能化衍生和复合，所构建的纤维素基复合材料表现出较高的比电容量和循环稳定性，展现出优异的电化学储能性能。

With the excessive consumption of non-renewable energy resources, the world is currently facing dual challenges of energy shortages and ecological pollution. In this context, the development of efficient energy storage devices for the effective collection and utilization of renewable energy has become a crucial approach to addressing energy issues. As a novel energy storage device, supercapacitors have garnered significant attention due to their superior power density. However, constrained by the performance limitations of electrode materials, existing supercapacitors still struggle to meet practical application requirements in terms of energy density and other aspects. Therefore, the development of high-performance electrode materials to enhance the energy storage performance of supercapacitors is of great significance in addressing the ever-increasing energy demands. Cellulose, as an abundant natural polymer compound in nature, is considered a highly promising candidate for electrode materials due to its unique hierarchical structural features. Nevertheless, traditional cellulose materials primarily rely on the electric double-layer capacitance mechanism for energy storage and are mostly limited to negative electrodes applications, which severely restricts their further development in the field of supercapacitors. To address these issues, this study aims to develop high-performance cellulose-based electrode materials by introducing active components such as metal-organic frameworks (MOFs) and metal oxides, thereby regulating the physicochemical properties of the electrode materials to optimize their conductive and electrochemical characteristics. The specific research contents are as follows:

1. A series of positive electrode and negative electrode materials were designed based on microcrystalline cellulose using solvothermal and ultrasonic methods. By compositing microcrystalline cellulose with a nickel-based MOF (5-N-TPPA-MOF) featuring unique channel structures, a series of composite positive electrode materials were successfully prepared. The effects of doping content on electrochemical performance were investigated, leading to the fabrication of high-performance cello-MOF-5-N. For the negative electrode, a novel cello-Bi material was developed by loading bismuth onto microcrystalline cellulose. Based on this design, an asymmetric dual-electrode system using microcrystalline cellulose as the substrate was constructed, effectively mitigating potential differences between electrodes while significantly enhancing conductivity. Experimental results showed that at a current density of a current density of 0.2 A g^-1, the specific capacity of this dual-electrode system reached 222 C g^-1. At a current density of 1 A g^-1, the system achieved a power density of 749 W kg^-1 and an energy density of 40 Wh kg^-1. Analysis of structural and valence state changes before and after cycling revealed that microcrystalline cellulose significantly improved the conductivity of the electrode materials and enhanced charge/ion transfer efficiency. This study demonstrates that the incorporation of tridentate long-arm ligands in MOF materials significantly improves the dispersion of nickel active centers, thereby enhancing the redox activity of the material. The presence of strong electron-withdrawing groups effectively facilitates ion transport within the material framework. Furthermore, the doping of bismuth metal in the negative electrode material introduces abundant electrochemically active sites, leading to optimized energy storage performance.

2. By introducing amino-functionalized ligands into the MOF structure and incorporating MnO into the negative electrode material, a microcrystalline cellulose-based electrode material was successfully developed. The asymmetric supercapacitor system constructed with these materials achieved a specific capacity of 400 C g^-1, at a current density of 0.2 A g^-1. The system delivered an energy density of 43 Wh kg^-1 and a power density of 723 W kg^-1, at a current density of 1 A g^-1. The amino-functionalized ligands significantly improved the hydrophilicity of the material, facilitating ion and charge transport on the surface and enhancing conductivity. The one-dimensional helical pore structure (7 Å diameter) in the MOF also played a key role in charge/ion transport. In the negative electrode material, the uniform distribution of manganese oxide on the cellulose substrate and their strong chemical bonding not only promoted the dispersion of metal active centers, enhancing redox activity, but also reduced MnO dissolution in the electrolyte, improving stability.

3. By further optimizing the material design strategy, bacterial cellulose, a substrate with unique 3D porous structure and excellent physical properties, was introduced to develop higher-performance supercapacitor electrode materials. For the negative electrode, a bi-cello-Bi₂O₃ material was developed by compositing bismuth oxide with bacterial cellulose. For the positive electrode, a high-performance bi-cello-MOF-5-H material was prepared by combining bacterial cellulose with a 5-hydroxyisophthalic acid-based MOF (5-H-TPPA-MOF). The assembled asymmetric supercapacitor exhibited a specific capacity of 412 C g^-1 at a current density of 0.2 A g^-1. At a current density of 1 A g^-1, the system achieved an energy density of 52 Wh kg^-1 at a power density of 751 W kg^-1. The introduction of hydroxyl-containing ligands formed stable intermolecular hydrogen bonds with hydroxyl groups on the bacterial cellulose chains, enhancing mechanical stability and promoting ion/charge transport. The incorporation of multivalent bismuth-based oxides in the negative electrode was confirmed by XPS analysis, where reversible transitions of Bi⁰/Bi³⁺/Bi⁵⁺ redox couples during charge/discharge improved electrochemical performance.

4. By using p-nitrobenzoic acid as an organic ligand, a novel positive electrode material (bi-cello-MOF-4-N) was synthesized. Combined with the previously designed bi-cello-Bi₂O₃ negative electrode, an asymmetric supercapacitor system was assembled, achieving a specific capacity of 487 C g^-1 at a current density of 0.2 A g^-1. At a current density of 1 A g^-1, the system delivered an energy density of 87 Wh kg^-1 at a power density of 750 W kg^-1. In this study, p-nitrobenzoic acid was employed as a functional ligand to construct MOF materials. The resulting framework features 9 Å diameter pore channels and adjacent nickel ion centers, which collectively shorten the charge transport pathways across the material surface while exposing additional redox-active metal sites, thereby enhancing the electrochemical performance of the material.

Experimental studies demonstrate that functionalized cellulose-based composites derived from microcrystalline cellulose and bacterial cellulose exhibit high specific capacity, cycling stability, and excellent electrochemical energy storage performance.

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