Materials Today Energy
Volume 17, September 2020, 100441
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Cellulose nanofiber based flexible N-doped carbon mesh for energy storage electrode with super folding endurance

https://doi.org/10.1016/j.mtener.2020.100441Get rights and content

Highlights

  • The novel flexible N-doped carbon mesh can be prepared via the CNC wet spinning and carbonization process.

  • The flexible N-doped carbon mesh has welded microstructures at the intersection.

  • The flexible N-doped carbon mesh has wrinkle microstructures along the axially oriented orientation.

  • The flexible N-doped carbon meshes exhibit excellent folding endurance.

Abstract

A novel cellulose nanofiber based flexible N-doped carbon mesh was prepared via the simple computerized numerical control (CNC) wet spinning and carbonization process using celluose nanofiber, graphene oxide and silk fibroin as raw materials. The cellulose nanofiber based flexible N-doped carbon mesh not only has welded microstructures at the intersection, but also has highly wrinkle microstructures along the axially oriented orientation. The N-doped carbon mesh materials exhibit excellent electrical conductivity with good flexibility. When the carbonization temperature is 1200 C, the sheet resistance of the carbon-based flexible mesh is only 27 ± 10 Ω/sq. In addition, the maximum area specific capacitance of flexible N-doped carbon mesh symmetric interdigital solid supercapacitor is about 4.5 mF cm−2 at a current density of 2.5 μA cm−2. The N-doped carbon mesh also displays excellent folding endurance. The capacitance retention rate is up to 152% after folding 50,000 times.

Graphical abstract

The novel flexible N-doped carbon mesh electrode materials are prepared via the simple CNC wet spinning and carbonization process using celluose nanofiber, graphene oxide, and silk fibroin as raw materials, which exhibit good electrochemical and excellent folding endurance

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Introduction

The flexible electrodes have attracted much attention in industry and academia due to their great potential applications in the flexible electronics, such as wearable electronic devices [1,2], e-skins [3,4], implantable medical devices [5,6], flexible display [7,8], flexible energy storage devices [9,10], etc. Generally speaking, the flexible electrodes should possess some characteristics, such as super folding endurance, high conductivity, good performance, lightweight, stability, economical, easy-processibility, large scale production, etc. Especially, the flexibility, conductivity and performance are the most important performance for flexible devices.

Among all existing potential flexible electrode materials, the carbon-based flexible electrode materials have been extensively studied because of their excellence inherent performance (such as excellent conductivity, mechanical properties, stability, flexible, etc.), easy regulation microstructure and a huge variety of effective preparation methods [[11], [12], [13], [14]]. Therefore, a large number of the free standing carbon based planar and fiber-like flexible electrodes were successfully prepared. The free standing carbon based planar flexible electrodes not only exhibit excellent flexibility, but also exhibit some other advantages, such as mass production, lightweight, pattern designability, tailorable performance, high reliability, etc [15,16]. They can easy integrate with desired shapes. In addition to exhibiting good flexibility, the free standing carbon based fiber-like flexible electrodes can also exhibit excellent ignitability. Therefore, the fiber-like flexible electrode with different functions can be easily woven to form flexible textiles. However, they also have some shortcomings, such as low energy density, low reliability (easy suffer from mechanical damage), poor tailorability, difficult to prepare long enough fiber, etc. These shortcomings can be detrimental toward the widely applications of free standing carbon based fiber-like flexible electrodes. In addition to the above two structural topography, the novel flexible mesh electrode materials (with fiber-like and planar electrode characteristics) have attracted much attention due to their excellent transparency, conductivity and flexibility [[17], [18], [19], [20]]. They can be widely used in the field of optoelectronic devices (such as electronic displays, light emitting diodes, solar cells, touch screens and so on). At present, the flexible mesh electrode materials are mainly focus on metal-based flexible mesh electrode materials (such as Au, Ag, Cu, and Ni -based flexible mesh electrode material) [[21], [22], [23], [24]]. Compared with metal materials, the carbon materials show greater application potential in the field of flexible mesh electrode material due to their high surface area, porosity, excellent electrical properties, good chemical stability, low cost, and flexible designability. This kind of material may be more suitable to use as flexible energy storage electrodes. There are many methods for preparing mesh electrode material. However, these methods are usually cumbersome and involve costly patterning techniques [[25], [26], [27], [28]]. This shortcoming can be detrimental toward the widely applications of flexible mesh electrode materials. Therefore, it is necessary to explore a simple and efficient preparation method of carbon based mesh electrode materials.

In this study, we are committed to the preparation of carbon-based flexible mesh electrode material via the simple CNC wet spinning technology using celluose nanofiber, graphene oxide, and silk fibroin as raw materials. The carbon-based mesh electrode materials exhibit high electrical conductivity and good flexibility. The carbon-based flexible mesh electrode materials show broad application prospects in energy storage electrode materials.

Section snippets

Preparation of carbon-based flexible mesh electrode materials

Cellulose nanofiber, graphene oxide, and silk fibroin were prepared as mentioned in our previous papers [29,30]. The cellulose nanofiber (0.56 wt %), graphene oxide (1.16 wt %), and silk fibroin (9.35 wt %, the mass ratio of cellulose nanofibers: graphene oxide: silk fibroin is 55:40:5) were mixed by the high speed homogenizer to form the spinning solution. The uniform composite spinning solution was defoamed in a vacuum oven for 3 h (at ambient temperature), and then was stored at 4 °C before

Results and discussion

The CGS spinning solution exhibits excellent wet-spinning property, which can produce consecutive wet CGS fiber and then forms the wet CGS mesh. The wet CGS meshes can be take out from the coagulation bath by the steel wires in the four sides of the wet CGS mesh due to their good strength and then air-dried. During the drying process, the 2D constrained force field will gradually generate in the wet CGS mesh due to their shrinkage. This 2D force field is essential for obtaining high quality CGS

Conclusions

In conclusion, the cellulose nanofiber based flexible N-doped carbon mesh were prepared by the simple CNC wet spinning and carbonization process using celluose nanofiber, graphene oxide and silk fibroin as raw materials. The highly wrinkle morphology of the carbon fiber structural unit is exhibit preferred orientation along its own axial direction of the carbon fiber. Furthermore, the carbon fiber structural units of the CGS-X mesh are welded together at the intersection. The CGS-X meshes

Credit author statement

Linlin Liu: Conceptualization,Methodology,Validation,Formal analysis Writing, Original Draft.

Songqi Hu: Writing - Review & Editing, Supervision,Project administration,Funding acquisition.

Kezheng Gao: Investigation, , Data Curation,Visualization.

Declaration of conflict of interest

We have complied with Elsevier's ethical requirements: This work described has not been published previously (except in the form of an abstract or as part of a published lecture or academic thesis), that it is not under consideration for publication elsewhere, that its publication is approved by all authors and tacitly or explicitly by the responsible authorities where the work was carried out. If accepted, it will not be published elsewhere in the same form, in English or in any other

Acknowledgments

Financial support was kindly supplied by grants from National Natural Science Foundation of China (No. 21501154), Fundamental Research Funds for the Central Universities (No. 3102017zy007) and Natural Science Basic Research Plan in Shanxi Province of China (No. 2017JQ5068).

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