Abstract

Cellulose-based hydrogels, obtained by tuned, low-cost synthetic routes, are proposed as convenient gel electrolyte membranes. Hydrogels have been prepared from different types of cellulose by optimized solubilization and crosslinking steps. The obtained gel membranes have been characterized by infrared spectroscopy, scanning electron microscopy, thermogravimetric analysis, and mechanical tests in order to investigate the crosslinking occurrence and modifications of cellulose resulting from the synthetic process, morphology of the hydrogels, their thermal stability, and viscoelastic-extensional properties, respectively. Hydrogels liquid uptake capability and ionic conductivity, derived from absorption of aqueous electrolytic solutions, have been evaluated, to assess the successful applicability of the proposed membranes as gel electrolytes for electrochemical devices. To this purpose, the redox behavior of electroactive species entrapped into the hydrogels has been investigated by cyclic voltammetry tests, revealing very high reversibility and ion diffusivity.

Highlights

  • Hydrogels derived from natural polymers, especially polysaccharides, are very interesting materials since they find application in many fields [1] with the advantage of being prepared starting from environmentally-friendly, renewable, and low cost raw materials

  • Fourier Transform Infrared spectroscopy (FTIR) spectroscopy has been extensively used in the study of cellulose materials, since it allows for obtaining direct information on the main modifications that occur in cellulose during various chemical and physical treatments [33]

  • It has been demonstrated that the synthesis of cellulose hydrogels, with tunable characteristics of the final materials, can be successfully achieved

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Summary

Introduction

Hydrogels derived from natural polymers, especially polysaccharides, are very interesting materials since they find application in many fields (agriculture, tissue engineering, drug delivery, biosensors, etc.) [1] with the advantage of being prepared starting from environmentally-friendly, renewable, and low cost raw materials. By tuning the crosslinker and cellulose concentrations, it is possible to optimize the hydrogel mechanical properties and swelling capabilities Thanks to these recent developments and due to the growing importance of green chemistry, versatile materials derived from cellulose, such as hydrogels and aerogels, have raised renewed interest in the field of electrochemical devices involving energy generation and storage [20,21,22]. To the best of our knowledge, electrochemical data on pure cellulose hydrogels are almost absent in the literature, or limited to particular hybrid hydrogels and electrolytes [20,32] In this framework, the present work reports on hydrogels obtained exclusively from unsubstituted celluloses crosslinked with epichlorohydrin (ECH) through optimized steps to achieve both the best solubilization and crosslinking. Swelling capability and electrochemical properties, investigated in terms of ion conduction ability and redox behavior of absorbed electroactive species, will be discussed, as well, to demonstrate the potential of the cellulose hydrogel membranes as ion-conducting, gel polymer electrolytes

Results and Discussion
Experimental Section
Conclusions
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