Layered double hydroxide materials coated carbon electrode: New challenge to future electrochemical power devices
Graphical abstract
Introduction
Microbial fuel cells (MFCs) are novel bioelectrochemical systems that exploit electrogenic bacterial to generate electrical power while degrading organic pollutants in wastewater [1], [2]. However, improving anode performance in MFCs remains one of the deciding factors for their applications, because the biological reactions mainly occur over its surface. During anodic bioelectrocatalysis, microorganisms oxidize organic matter and released electrons are transferred to the solid electrode material. Hence, the development of new and simple strategies to fabricate efficient anode materials to increase the bacterial loading capacity and improve substrate transport is of great interest and importance.
Nowadays, a major challenge for microbial fuel cells (MFCs) is to develop new anode materials for practical applications in bio-electroremediation devices. Commercial graphite-based materials such as carbon felt, carbon cloth, glassy carbon, carbon paper and graphite rods have been widely used as convenient materials for anode MFCs [3], [4], [5], [6]. Thus, improving anode performance is important for increasing power production. Previous research has shown that electrode performance can be improved through chemical modification of the anodes.
Clay’s minerals have emerged as one of the most promising modified electrode materials for developing high-performance due to their unique properties such as high metal dispersion, high surface area, controllable particle size and high thermal stability [7], all of which benefit the formation of highly stable and dispersed electrochemical active metal [8], [9]. Particularly interesting is the anionic clays, especially hydrotalcite-like compounds (HTs), which are relatively easy to synthesize and have an environmentally friendly nature. HTs exhibit a broad versatility which allows their synthesis with different ions for specific applications [10], [11], including degradation and adsorption of a wide variety of pollutants such as phenols, oxyanions and dyes [12], [13], [14]. Recently, Tonelli et al. [15] and Mousty et al. [16], [17] have reviewed the HT materials as electrode modifiers to be used for both electrochemical detection (chemical sensors and biosensors) and energy-storage devices.
The naturally occurring mineral hydrotalcite, Mg6Al2(OH)6CO3·4H2O, belongs to this class of materials, and consequently layered double hydroxides (LDHs) are also known as hydrotalcite-like materials. LDHs are a family of synthetic lamellar solids with positively charged brucite-like layers of mixed metal hydroxides separated by interlayer hydrated anions (Scheme 1) [18], [19], described by the general formula: [M(II)1-xM(III)x.(OH)2]x+[(An−)x/n,yH2O] (abbreviated as M(II)M(III)–A, where M(II) is a divalent metal cation, such as Mg, Mn, Ni, Zn, Co, Fe and Cu; M(III) is a trivalent metal cation, such as Al, Fe, Co, Ni, Mn and Cr; An− is an interlayer anion, such as Cl−, F−, CO32−, NO3− and SO42−; the value of x is between 0.2 and 0.33 generally represent the molar ratio M(II)/[M(II) + M(III)]).
As an inorganic clay that have been widely reported, layered double hydroxides (LDHs) have been subjected to intense research by the electrochemist community. However, the exploration of LDH-based materials as electrode modifiers is one of the important issues to be of concern [20], [21], [22], [23]. Previously, we reported that LDHs in which M(II) is a transition metal, undergoing a redox reaction in the range of applied potential, have been proposed as materials with improved charge transport [24], [25], [26], [27], [28]. Indeed, electron transfer within these Inorganic lamellar materials can further be promoted by two strategies: (i) the intercalation of redox active anions between the LDH layers and (ii) the presence of transition metal cations within the LDH intralayer domain, itself [17]. Accordingly, the modulation of the intrinsic properties of LDHs (electronic conductivity, redox or acid-base properties) is dependant on the nature of the cations in the layers [29], can render the LDH hybrid structure electroactive and endow redox properties to the LDH layers. However, to our knowledge, very few studies describe the electrochemical behavior of LDH in function of the cations. They have been dedicated to LDHs with Ni and Co divalent cations [28], [30], [31], [32], [33], [34], [35]. Because of their desirable properties including low cost, good biocompatibility, high catalytic activity, and high chemical stability, LDH materials could find application also as anode materials in the so-called biofuel cell, as very recently reported in literature [36], [37]. LDH modified electrodes are thus mainly prepared as a thin film coated on a working electrode surface through solvent casting, layer by layer assembly, or electrode position [38], [39], [40].
A comprehensive study of the electrochemistry of layered double hydroxides is evident to open new potentialities in regard to application in area of electrochemical devices. The current paper is devoted to investigate and hence improve electron transfer reaction using divalent cation metals containing LDH (Mg & Zn) supported on carbon electrodes. A special attention is paid on MgAl-LDH and ZnAl-LDH as illustrative examples of electrocatalyst materials in energy conversion. Furthermore, microbial fuel cell configuration has been tested.
Section snippets
Reagents
Aluminum chloride hexahydrate (AlCl3·6H2O), magnesium chloride hexahydrate (MgCl2·6H2O), nitric acid (HNO3), phosphate buffered saline tablet, potassium ferrocyanide trihydrate (K4Fe(CN)6·3H2O), sodium acetate (CH3COONa), sodium hydroxide (NaOH) and zinc chloride (ZnCl2) were purchased form Sigma–Aldrich. All chemical reagents were of analytical grade and used without further purification. Deionized water was employed for all the experiments.
LDH synthesis
MgAl and ZnAl LDH materials potentially intercalated
Structural characterization of MgAl and ZnAl LDHs
The X-ray diffraction patterns of prepared MgAl and ZnAl LDH are shown in Fig. 1. All diffraction patterns exhibit the characteristic reflections (003), (006), (009)(012), (015), (018), (110) and (113), corresponding to hexagonal LDH crystal structure with an Rm symmetry and suggesting that synthesized LDHs were crystallized with well-ordered structures. More intensive and sharper reflections of the (003) and (006) planes at low 2θ values (11−23°), and broad asymmetric reflections at higher 2θ
Conclusion
Layered double hydroxide MgAl and ZnAl materials were chemically synthesized and deposited over carbon electrode materials, and successfully tested as electrocatalysts for single chamber microbial fuel cell anodes. First, we introduced a structural and microstructural comparison between both samples, which is very meaningful for electrochemically fundamental research. Then, we showed that the dispersion of such LDH particles over carbon electrodes has a beneficial effect on the MFC performance
Conflict of interest
The authors declare no competing financial interest.
Acknowledgments
I would like to thank Dr. Martiane Cabié from “Centre Pluridisciplinaire de Microscopie Electronique et de Microanalyse (CP2M), Aix Marseille Université, 13013 Marseille, France”, for assistance with microscopy analysis. I would like to thank Dr. Soumya Elabed from “Laboratoire de Biotechnologie Microbienne, Faculté des Sciences et Techniques, 2022 Fez, Morocco”, for help with angle contact measurements. Finally, I would like to acknowledge graciously Aisha Gharsalli from “LECOM School of
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2023, Chemical Engineering JournalCitation Excerpt :The peaks of LDHs can be indexed as the (0 0 3), (0 0 6), (009/012), (0 1 5), (0 1 8), (1 1 0) and (1 1 3) reflections of the MgAl-LDH phase, which are consistent with the standard PDF#51–1525. The (0 0 9) reflection overlaps with the (0 1 2), which has also been shown in another study [44]. Besides, Fig. 1b displays the surface groups of LDHs by FTIR spectrum.
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