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Layered double hydroxides (LDHs) have been widely used in the past years due to their unique physicochemical properties
and promising applications in electroanalytical chemistry. The present paper focus exclusively on magnesium-aluminum
and zinc-aluminum layered double hydroxides (MgAl & ZnAl LDHs) in order to investigate the property and structure of
active cation sites located within the layer structure. The MgAl and ZnAl LDH nanosheets were prepared by the constant
pH co-precipitation method and uniformly supported on carbon-based electrode materials to fabricate an LDH electrode.
Characterization by powder X-ray diffraction, Fourier transform infrared spectroscopy, scanning electron microscopy
and transmission electron microscopy revealed the LDH form and well-crystallized materials. Wetting surface properties
(hydrophilicity and hydrophobicity) of both prepared LDHs were recorded by contact angle measurement showed hydrophilic
character and basic property. The electrochemical performance of these hybrid materials was investigated by mainly cyclic
voltammetry, electrochemical impedance spectroscopy and chronoamperometry techniques to identify the oxidation/
reduction processes at the electrode/electrolyte interface and the effect of the divalent metal cations in total reactivity. The
hierarchy of the modified electrode proves that the electronic conductivity of the bulk material is considerably dependent
on the divalent cation and affects the limiting parameter of the overall redox process. However, MgAl LDH shows better
performance than ZnAl LDH, due to the presence of magnesium cations in the layers. Following the structural, morphological
and electrochemical behavior studies of both synthesized LDHs, the prepared LDH modified electrodes were tested through
microbial fuel cell configuration, revealing a remarkable, potential new pathway for high-performance and cost-effective
electrode use in electrochemical power devices.