Abstract

Four different types of crystalline and fibrillar nanocellulosic materials with different functional groups (sulfate, carboxylate, amino-silane) are produced and used to disperse commercial multiwalled carbon nanotubes (MWCNT). Aqueous nanocellulose/MWCNT dispersions are drop-cast on tetrahedral amorphous carbon (ta-C) substrates to obtain highly stable composite electrodes. Their electrochemical properties are studied using cyclic voltammetry (CV) measurements with Ru(NH3)62+/3+, IrCl62–/3– redox probes, in electrolytes of different ionic strengths. All studied nanocellulose/MWCNT composites show excellent stability over a wide potential range (−0.6 to +1 V) in different electrolytes. Highly anionic and more porous fibrillar nanocellulosic composites indicate strong electrostatic and physical enrichment of cationic Ru(NH3)62+/3+ in lower-ionic-strength electrolytes, while lesser anionic and denser crystalline nanocellulosic composites show no such effects. This study provides essential insights into developing tailorable nanocellulose/carbon nanomaterial hybrid platforms for different electrochemical applications, by altering the constituent nanocellulosic material properties.

Highlights

  • The term “electrochemistry” was coined in 1814, and researchers in the 19th and 20th centuries have spearheaded tremendous advancements in the field of electrochemical applications including batteries, electroplating, mineral processing, electrolysis, and electroanalytical sensing.[1,2] Despite research interests spanning over more than two centuries, the novelty and developments in this field remain unexhausted as the advances in material processing, and especially, the development of functional nanomaterials, have given rise to several new electrochemical application fields

  • Article nanocellulosic matrices to obtain functional hybrid nanocomposites for various applications.[16−22] We have previously demonstrated that the presence of a high density of negatively charged sulfate functional groups on the nanocellulose can significantly improve the selectivity of multiwalled carbon nanotubes (MWCNTs) in the composite electrode, toward the cationic dopamine molecule.[23]

  • Elemental sulfur and nitrogen contents per gram of dry sulfated cellulose nanofibrils (SCNF), sulfated cellulose nanocrystals (SCNC), and amino-silanized cellulose nanocrystals (ACNC) nanocellulosic materials were estimated by elemental analysis

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Summary

INTRODUCTION

The term “electrochemistry” was coined in 1814, and researchers in the 19th and 20th centuries have spearheaded tremendous advancements in the field of electrochemical applications including batteries, electroplating, mineral processing, electrolysis, and electroanalytical sensing.[1,2] Despite research interests spanning over more than two centuries, the novelty and developments in this field remain unexhausted as the advances in material processing, and especially, the development of functional nanomaterials, have given rise to several new electrochemical application fields. We produce four different nanocellulosic materials, namely, sulfated cellulose nanofibrils (SCNF), TEMPO (2,2,6,6-tetramethylpiperidin-1-oxyl)-mediated oxidized cellulose nanofibrils (TOCNF), sulfated cellulose nanocrystals (SCNC), and APTMS ((3-aminopropyl) trimethoxysilane)-mediated amino-silanized cellulose nanocrystals (ACNC) The choice of such vastly different nanocellulose functionalization chemistries and starting materials is intentional, to investigate (i) the efficacy of such a wide range of nanocellulosic materials in dispersing MWCNT and (ii) the nanocellulose-dependent variations in the electrochemical properties of the resultant composites. Essential insights into designing such hybrid electrode materials for various applications

EXPERIMENTAL SECTION
RESULTS AND DISCUSSION
CONCLUSIONS
■ ACKNOWLEDGMENTS
■ REFERENCES
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