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Modular Assembly of Cu- and Ni-based Micro- and

Nanostructures for Electrochemical Sensing and

Energy Applications

Thesis Submitted to AcSIR for the Award of the Degree of

DOCTOR OF PHILOSOPHY

In

CHEMICAL SCIENCES

By

M. KALEESH KUMAR

Registration Number: 10CC14A05005

Under the Guidance of

Dr. Shailendra Kumar Jha

CSIR - Central Electrochemical Research Institute, Karaikudi-630003, Tamil

Nadu, India

August-2019

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Chapter VIII Summary

M Kaleesh Kumar 178

Chapter VIII

Summary and future perspectives

A series of Cu- and Ni-based micro- and nanostructured materials have been prepared via in-situ

electrosynthesized protocol and investigated as catalysts for electrochemical sensing and energy

applications. The electrochemical sensing exeriments have been performed for the selective and

sensitive determination of dopamine, glucose and p-nitrophenol as well as the practical feasibility of

the as-prepared platforms is also shown in real-time samples and environment. On the other side,

some of the as-prepared electrocatalysts have been tested for the electrooxidation of methanol and

formic acid. Finally, a brief conclusion of each chapter is as follows:

Chapter II: Preparation of electro-reduced graphene oxide supported walnut shape nickel

nanostructures, and their application to selective detection of dopamine

The electroreduced graphene oxide supported walnut shape nickel nanocomposites (er-GO-Ni) have

been synthesized by an optimized electrodeposition route. Their applications for the selective

detection of dopamine unravel the facts related to the selectivity in the presence of interfering

species, especially for ascorbic acid (AA) and uric acid (UA). It has been attributed to (i) Nafion (1.0

%) film coating, (ii) repulsive electrostatic interaction with similar negative charge on residual

oxygen functionality of electroreduced graphene oxide (er-GO) and (iii) oxide or hydroxide Ni

species during deposition of sample. The fabricated electrochemical sensor has shown a detection

limit of 10 ± 0.03 nM for dopamine in the presence of interfering species and its applicability can be

explored for the healthcare management.

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Chapter VIII Summary

M Kaleesh Kumar 179

Chapter III: Facile in-situ electrosynthesis and high electrocatalytic performance of interconnected

layered double hydroxides/graphene hybrids for dopamine oxidation: a comparative study

A facile in-situ electrodeposition approach has been used to prepare a rational design of M-Al (M:Ni,

Co) layered double hydroxide (LDH)/reduced graphene oxide (G) hybrids and its superior

electrocatalytic activity has been tested for the electrooxidation of dopamine. The regular and

specific worm like interconnected nanochain architecture of NiAl-LDH/G hybrid sensor is

responsible for its improved conductivity, electrocatalytic activity and performance than the CoAl- LDH/G hybrid modified electrode for oxidation of dopamine. The proposed sensor has detected upto

9.8 nM of dopamine and shown the selectivity towards various foreign species, also furnished good

recovery for both the real world samples of human serum and dopamine drug samples.

Chapter IV: Elucidation of confined copper nanospheres within self-assembled curcumin-cysteine

and their electrocatalytic application

The novel combined self-assembly/electrodeposition approach has been explored for the construction

of surface-confined modular Cu metal-ion nanosphere deposited on curcumin-cysteine complex

conjugate monolayer modified gold electrode and tested for p-nitrophenol determination. The

protected copper nanospheres have been formed due its better complextaion with β-diketone of

curcumin in curcumin-cysteine complex conjugate. The optimized electrochemical platform has

shown two linear ranges from 0.97 to 1.76 mM and 0.1 μM to 0.90mM, low detection limits of 69

μM and 57 nM, and high sensitivity of 70.45 μA μM−1

cm−2

and 153.08 μA μM−1

cm−2

, respectively.

The practical feasibility of the electrochemical platform as proposed sensor has been also tested for a

real world samples (i.e., Lake water) and the recoveries of p-nitrophenol were found in the range of

93.2 % to 105.9 %. This combined self-assembly/electrodeposition approach will provide an