Open access peer-reviewed chapter - ONLINE FIRST
Abstract
Electrochemical energy conversion and storage technologies play a crucial role in ensuring a sustainable energy future. In these regards, nanostructured carbon-based materials (NCMs) are very critical in the development of novel energy technologies and devices. NCMs include CNTs, graphene, fullerene, and ordered mesoporous carbon materials, which exist in different morphologies. NCMs offer great opportunities for effective modifications through surface functionalization, doping with heteroatoms, and fabrication of composites with organic or inorganic species. Particularly, the composites of NCMs with inorganic materials such as metallic NPs, metal oxide NPs, and their other derivatives (MNPs) have gained considerable recognition in electrochemical energy applications. These materials demonstrate distinct properties, including excellent thermal and electrical conductivity, large surface area, and chemical stability. Herein, we have highlighted some of the trends and outlooks in this exciting area, including fundamentals of these substances according to material science perspective. Besides, the latest research and development of multifunctional MNPs@NCMs composites for electrochemical energy applications have also been illustrated. Particularly, the utilization of these composites from the perspective of different electrochemical energy applications has been summarized, such as energy conversion processes like hydrogen evolution reactions (HER), oxygen reduction reactions (ORR), and energy storage devices like batteries and supercapacitors.
Keywords
- nanocomposites
- carbon based materials
- graphene
- energy applications
- water splitting
1. Introduction
Currently, significant research is being carried out in materials science to develop new substances that can be used for various energy storage and energy conversion applications [1]. One such area of focus is the development of high-performance materials with specific features which are suitable for different energy purposes including for energy devices and energy processes [2]. In these regards, carbon-based materials (graphite, hard carbon, glassy carbon, and carbon black) have been extensively used, particularly in electrochemical energy storage systems [3]. This is mainly due to their excellent physicochemical properties such as, excellent electrical conductivity, strong chemical stability, and efficient abilities of adopting to different interface processes [4]. Interestingly, carbon-based materials are sp2-hybridized and typically possess several unique structural characteristics including high crystallinity, diverse morphologies, excessive porosity, and distinct texture [5]. These features are important in determining and enhancing the electrochemical performance of carbon-based electrodes and electrocatalysts [6]. As of now, scientists are still striving hard to explore in-depth structure-function relationship of carbon-based materials, which is crucial for developing better, more effective functional materials [7]. The need for enhanced performance of electrochemical devices in energy applications has led to the development of a variety of carbon-based materials with tailored structures and porosity [8, 9]. This has been typically achieved by the preparation of various carbon-based materials and their respective composites such as, activated carbon, graphene, CNTs etc. [10, 11, 12].
Apart from these, several other approaches have also been applied to enhance the electrochemical performances of these materials including the selection of appropriate synthetic methods and carbon precursors, modifications of the post-synthetic treatment conditions, and by the implementation of activation and functionalization processes [13]. Extensive studies are available in the literature describing the application and efficiency of the diverse carbon derivatives as electrode material in different electrochemical processes. Among various carbon derivatives, graphite and activated carbon are the most commonly applied materials in various energy storage devices such as lithium ion batteries (LIBs), supercapacitors etc. [14, 15]. However, the advancements in the preparation of different types of high-quality inorganic nanomaterials have further revealed the effectiveness of carbon derivatives [16]. Since, when used alongside other functional nanomaterials, nanocomposites made from carbon derivatives show immense promise for powering advanced energy storage devices and facilitating energy conversion processes [17].
Notably, carbon nanomaterials can be broadly classified into two different categories i.e., nanostructured carbon materials involving reduced size of bulk carbon substances, such as the conversion of graphite into graphene, and the second one is the creation of new morphologies at low dimension like carbon nanotubes or fullerenes [19]. In the context of materials science, the conversion of bulk carbon into nanostructured carbon materials, generally creates two different types of size effects on the properties of resulting material [20]. The first type is known as “trivial size effects”, which are based on changes in size such as, the decreased diameter of nanoparticles or the reduced thickness of layers [21, 22]. These changes result in altered volumes and increased surface-to-volume ratios [23]. The second type is called “true size effects”, which are based on the modification of local properties of materials [24]. Indeed, these effects are clearly visible in various nanostructured carbon derivatives, such as, fullerenes, graphene, and CNTs which hugely differ from classical carbon materials due to the significant role of true size effects they exhibit [25]. These types of nanocarbon materials exhibits unique and extraordinary properties which can be attributed to their distinct dimensionalities, surface areas, and porosities [26].
However, the most important aspect which distinctly sets apart nanostructured carbon materials from classical carbon is the distribution of chemical bonding, which enables a combination of local electronic structures involving both sp2 and sp3 carbon [27, 28]. Easy tunability of the local electronic structures of carbon materials offers great deal of flexibility in the formation of desired local chemical bonding which facilitate the fabrication of materials with predictable mechanical and chemical properties [29]. Due to these properties, the nanostructured carbon materials have been extensively used as building blocks for the formation of different types of advance functional materials with diverse morphologies (cf. Figure 1) [30]. Besides, nanostructured carbon materials have been extensively combined with two or more different nanomaterials with diverse morphologies to form functional nanocomposites [31]. Indeed, the structure flexibility of carbon allows to fabricate multifunctional carbon-based nanocomposites with a variety of complex nanoarchitectures [32]. For instance, graphene layers can effectively encapsulate different types of nanoparticles to form 3D structures, carbon nanotubes (CNTs) can be used as containers or holders of active materials, or different types of functional nanomaterials can be efficiently dispersed into a carbon matrix [33]. Besides, other complex carbon based nanoarchitecture are also possible, involving the hierarchical arrangement of carbon nanostructured materials like CNTs, carbon nanowires, and carbon nanobelts in an array to create rambutan-like structures etc. [34]
Figure 1.
Different forms of nanocarbons demonstrating representative hybrid or hierarchical structures [
The excellent transport properties of carbon-based nanocomposites with various dimensions make them highly useful in energy storage applications that rely mainly on mass transport of ionic charges [35]. Additionally, their enhanced surface area provides easy access to active components, facilitating effective storage of active ionic components through intercalation [36]. Due to the excellent electronic conductivity, light weight and high-strength of carbon derivatives, carbon nanocomposites offer special benefits as active electrodes and current collectors during the assembly of high-performance electrochemical energy storage devices [37, 38]. In many cases, these types of composites also serve as multifunctional hosts for high-capacity metal anodes and cathodes for high-energy-density batteries [39]. Thus, carbon nanocomposites have gained significant recognition for portable electronics, electric vehicles, and aviation and aerospace equipment with a significant weight reduction and extension of the endurance [40]. Apart from energy storage applications, carbon nanocomposites have also played crucial role in the creation of affordable yet effective catalysts for different types of electrochemical energy conversion processes [41]. These nanocomposites have surfaced as a distinctive type of functional nanomaterials that exhibit visible electrocatalytic activity for several reactions, including hydrogen evolution reaction (HER), oxygen evolution reaction (OER), oxygen reduction reaction (ORR), and CO2 reduction reaction [42, 43]. These reactions are significant for water splitting, fuel cells, and metal-air batteries [44].
Primarily, the efficient electrocatalytic properties of carbon nanocomposites is attributed to the effective transfer of charges from the active nanocomponent to the parent matrix (carbon) [45]. This transfer varies depending upon the structures and morphologies of the nanocomponent, such as its elemental composition and core size, and the carbon matrix, such as its doping and layer thickness [7]. Especially, carbon nanocomposites based on (non-noble) metals and metallic compounds incorporated into carbon matrices have been found to exhibit enhanced electrocatalytic properties [46]. The enhanced properties of nanocomposites are mainly attributed to the presence of carbon matrix, plenty of active sites, and synergistic effect between the components involved [47]. This chapter highlights the most important electrochemical aspects and achievements of carbon-based nanocomposites in both energy storage and energy conversion applications. Particularly, nanocomposites involving different types of carbon nanostructures, like graphene, CNTs, activated carbon, ordered mesoporous carbons in combination with multifunctional nanomaterials such as, metal, metal oxide nanoparticles will be discussed in more detail. In this chapter, we will mainly focus on the materials science aspects of carbon nanocomposites, which are either applied as electrode materials or as electrocatalysts in different electrochemical energy applications, like, batteries, supercapacitors, HER, ORR etc. Finally, current challenges and future strategies will also be discussed.
2. Inorganic NPs and CNTs based (MNPs@CNTs) composites
Due to their exceptional physicochemical characteristics, carbon nanotubes (CNTs) have emerged as a fascinating component in various energy storage devices, including supercapacitors, fuel cells, and accumulators [48]. In particular, the conducting and microtextural properties of CNTs make them a notable material for different electrochemical applications [49]. CNTs consist of regular carbon network which is made up of graphitic layers that are cylindrically rolled and tightly entangled with nanotubes, providing good conductivity and accessibility. Apart from this, these materials also exhibit moderate surface area which is ranging from ~100 to 400 m2g−1 [50]. Various electrochemical processes are often associated with the accumulation of charge in the electrode/electrolyte interface, thus, the unique nanotubular shape of CNTs consisting of an easy available web is particularly beneficial [51]. The distinctive arrangement of carbon nanotubes (CNTs) grants them a range of exceptional characteristics, such as high resilience, remarkable tensile strength, excellent current carrying and heat transmission capabilities, as well as extraordinary electronic behavior [52]. Additionally, CNTs possess low density and exhibit very high stability [53]. Moreover, due to their mesoporous nature, CNTs have also been applied as effective support for catalytically active materials to obtain efficient electrocatalysts in various electrochemical energy applications [54].
To further enhance the electrochemical behavior of CNTs, they have been combined with various functional materials, particularly, for this purpose, the inorganic nanoparticles have gained considerable recognition [55]. Composites made of CNTs and inorganic nanomaterials demonstrate distinct characteristics involving the features of both the components, and may even display novel properties due to their synergistic effects [56]. As a result, these composite materials have great potential for a wide range of applications across various fields including electrochemical energy applications [57]. The CNTs based composites are mainly popular as electrode materials and electrocatalysts due the excellent electronic and electrical characteristics of CNTs and their high surface area, electrochemical stability, and a 1D geometric structure [58]. On the other hand, inorganic nanoparticles, have been frequently utilized as functional materials in energy applications, like, as electrocatalysts in electrochemical reactions etc. [59]. As a result, combining CNTs with inorganic nanomaterials has demonstrated significant potential in electrochemical energy applications [60]. Particularly, the nanoconfinement of metal nanoparticles (MNPs) in CNTs have demonstrated great potential, due to generation of unique properties that are distinct from original materials [60]. In electrochemical energy conversion applications, precious metal catalysts like Pt, Pt etc., are required for electrocatalytic reactions [61]. However, these catalysts are not only expensive but also have low reserves. MNPs@CNTs have garnered a lot of attention for their exceptional surface chemistry and high catalytic activity in significant electrocatalytic reactions such as OER, ORR, and HER [62].
But, in most of the cases, the redox reactions often tend to be expensive, due to significant energy losses caused by large overpotentials. Precious metal catalysts significantly improve the reaction kinetics by lowering the overpotential, but they are scarcely available and highly expensive. However, MNPs@CNTs demonstrate enhanced electrochemical performance due to the improved electronic structure of carbon and its stronger interactions with electroactive metallic species [63]. These stronger interactions have a significant impact on the reaction kinetics, catalytic stability and cyclability. While, the porous and conductive walls of CNTs allow easy transfer of electrolyte into metal species, and also facilitate the transport of electron. Moreover, the walls of CNTS also keep the surface of metal NPs safe from corrosion that may be caused due to direct contact with the electrolyte [64]. MNPs@CNTs have been extensively applied in various energy conversion processes, one such process is proton exchange membrane fuel cells (PEMFCs) which is an efficient conversion system and deliver high energy densities [65]. PEMFCs produce electricity through electrochemical processes for which they require hydrogen, methanol etc. [66]. For example, microwave mediated preparation of functionalized, single-wall CNTs decorated with Pt NPs based composites (Pt/FCNT) have exhibited enhanced catalytic performance that was superior to original materials [67].
In a recent study, functionalized CNTs supported hybrid catalysts including Pt, Fe and Ni NPs were fabricated and applied as electrocatalytic electrode for PEMFC cathode [68]. In this case, MNPs@CNTs accelerated the ORR, due to the high crystallinity, aspect ratio, low defect density, and unique electrical conductivity which enabled them to pass easily through the four-electron pathway. In another study, the surface of MWCNT was modified with nitrogen-containing compounds, which was further decorated with Pt NPs. The as-prepared hybrid has shown enhanced performance in electrochemical reaction which was performed by using a rotating disk electrode at 10–35°C in 0.1 M HClO4 as electrolyte in a hydrogen–oxygen PEMFC [69]. More recently, Zhao et al., have designed and fabricated a cheap electrocatalysts for ORR using Fe3N NPs which were encapsulated by N-doped CNTs and decorated on the surface of a flexible biomass-derived carbon cloth (Fe3N@CNTs/CC) [70]. Fe3N@CNTs/CC demonstrated unique structure and when used as electrocatalyst for ORR, it has exhibited high activity as well as excellent long-term stability and methanol resistance in alkaline media. Notably, Fe3N@CNT/CC has functioned as a gas diffusion layer and a cathode material in a Zn-air battery. Furthermore, it has exhibited superior electrocatalytic properties than a commercial Pt/C catalyst such as, excellent power density and high specific capacity. HER is another important energy conversion process where MNPs@CNTs have played crucial role. Apart from Pt, non-precious metal-based HER catalysts have been encouraged, but these metals are susceptible to acid leaching, which can be tackled by their confinement in CNTs. For instance, when cobalt NPs were confined in CNTs, the resulting hybrid showed efficient electrochemical performance such as an onsent potential of 89 mV and good overpotential (200 mV) due to the cooperative effects between graphene encapsulated Co NPs [71].
Electrochemical energy storage devices are being viewed as a viable alternative to the gasoline industry to meet the rising demand for energy [72]. These devices can potentially replace gasoline in various applications ranging from portable devices to the electric vehicle industry [73]. Indeed, there have been promising developments in recent years towards the use of MNPs@CNTs for energy storage devices [74]. The resulting tubular structures possess an active surface, redox-active confined metal species, porous walls, enough space for core volume expansion, and modified electronic transport [75]. Particularly, nanocrystal-confined CNTs containing metal oxides such as Fe, Ni, Co, Mn, Zn, and Sn have exhibited exceptional storage properties [76]. Although, metal oxides as electrodes demonstrate high electron storage capacity, but they usually suffer from poor electrical conductivity, which is addressed by the inclusion of CNTs [77]. Additionally, MNPs@CNTs that have been doped with heteroatoms (such as N) have shown to possess effective charge storage capabilities due to their unique properties such as confinement of reactive species, high electrical conductivity, large surface area, and strong M-π interactions [78].
Apart from these, the fast electron transport during reversible charge/discharge cycles is promoted by the porous outer walls of CNTs that confine inorganic species. This prevents metal surfaces from corroding and enhances the lifespan of batteries [75]. Such as, hierarchically structured carbon coated SnO2 NPs decorated on the surface of a CNTs to obtained a hybrid C–SnO2/CNT, which has showed superior electrochemical performance [79]. When used as an anode material in LIBs, the hybrid demonstrated an efficient reversible capacity up to 1572 mA h g−1 at 200 mA g−1 and strong stability. More recently, Lei et al., have fabricated a high-power, wearable zinc air battery (ZAB) using a new NiFe NPs embedded N-doped CNT (NiFe/N-CNT) as bifunctional electrocatalyst [80]. The as-prepared ZAB with the NiFe/N-CNT as air cathode showed an ultrahigh open-circuit potential (
Supercapacitor is another energy storage device in which MNPs@CNTs have been extensively applied to achieve quick route for energy storage with fast charge–discharge rates and high-power densities [82]. The electrode chemistries in supercapacitors have been advanced by confining metal oxides and hydroxides within CNTs, which offers an appealing topology where the electrolyte comes into direct contact with the CNTs, while protecting the metallic species from direct contact with the electrolyte. As a result, MNPs@CNTs demonstrate significantly more stable capacitive performances and higher energy densities. One of a pioneering report on the potential of using MNPs@CNTs in supercapacitors is presented by Wang et al., who have explored the impact of encapsulating MnO2 in CNTs on the capacitive performance of the materials [83]. It was revealed that MnO2 decorated CNTs exhibited close interactions between the interior walls of CNTs and inorganic species, which have affected the electronic structure of CNTs. More recently, Geuli et al., have fabricated a hybrid which was binder-free and consisted of NiOx deposited on MWCNTs and nickel foam decorated with NiCo2O4 NPs which was used to produce a stable supercapacitor [84]. The hybrid has offered competent electron transfer, high surface area and superior electrochemical performance, including high charge storage, high rate delivery and good cycling stability.
3. Inorganic NPs and graphene (MNPs@Gr) based composites
Among nanostructured carbonaceous substances, graphene (Gr), is another desirable material for electrochemical energy applications [85]. Due to its single-atom thick, hexagonal sp2 carbon matrix and a unique two-dimensional layered structure, graphene exhibits extraordinary physicochemical properties including excellent conductivity and strong mechanical and electrochemical stability [86]. These properties have garnered great research interest for graphene-based substances as suitable electrode materials and electrocatalysts for energy storage and conversion purposes [87]. Besides, the high specific surface area, graphene provides plenty of active sites, which allow fast reaction kinetics; and enables energy storage materials to achieve high power and energy densities [88]. Among other carbon nanostructures, graphene possesses a significant advantage due to the availability of every single atom, making it highly electrochemically active [89]. This feature also helps in reducing the resistance for ions to reach its surface, thereby making it a promising material for electrochemical energy applications [90]. Since the initial discovery of graphene through the Scotch-tape method, involving layer-by-layer peeling of graphene from highly-oriented pyrolytic graphite (HOPG), numerous facile and efficient methods have been developed for synthesizing graphene [91]. However, the challenge of producing graphene at a controllable size on a large scale still persists. To this end, several synthetic approaches have been developed so far, such as, thermal decomposition and chemical vapor deposition (CVD), mechanical and chemical exfoliation methods etc. [92]. Among these methods, for the large-scale preparation of graphene like structures, methods based on sequential oxidation of graphite and its subsequent reduction have gained decent recognition (cf. Figure 2) [93, 94].
Figure 2.
Graphical representation of the preparation of graphene with different methods [
To further improve the electrochemical properties of graphene, modification of graphene with other elements, inorganic nanoparticles (metallic and metal oxide NPs), polymers and other materials has been explored extensively [95, 96]. In these regards, doping of graphene with heteroatoms (e.g., N, B, P, or S), decoration with inorganic nanoparticles has been proved to extremely beneficial in tuning the electronic and geometric features of the resultant graphene materials [87]. These approaches have offered more active sites for stronger molecular adsorption and enhanced electrocatalytic properties due to the presence of electroactive metallic materials [97]. Especially, the incorporation of diverse inorganic nanoparticles, such as metal and metal oxide NPs, can boost the electrical and electronic properties of resultant composites [98]. Due to the combination of improved physicochemical properties and the cooperative interactions between Gr and inorganic MNPs, MNPs@Gr composites have significant potential in a variety of applications, particularly in energy storage and conversion devices [99]. Until now, significant attempts have been made to effectively blend various types of metallic and metal oxides nanoparticles with graphene and explore their usage in various fields including for energy conversion and storage purposes [47].
The deposition of metal and metal oxide nanoparticles (NPs) onto graphene, can be achieved through two methods:
Figure 3.
Graphical representation of the different methods of the binding of inorganic nanoparticles onto the surface of graphene nanosheets [
Such as, in a recent study, He et al., have demonstrated the preparation of bifunctional electrocatalysts involving ruthenium NPs which are decorated on Gr nanosheets. The resulting hybrid was further co-doped with Co and N by
MNPs@Gr composites have gained decent recognition for various energy conversion processes including HER, ORR and others [107]. HER is regarded as a promising energy conversion process due to release of H2, which is considered as clean energy source for the future [108]. Due to its high energy density (140 kJ g−1) and clean combustion product (H2O), researchers are particularly interested in the low-cost and eco-friendly process of the electrochemical reduction of water to obtain green H2 [109]. Out of several, HER electrocatalysts, graphene and Pt-based catalysts are very popular, due to the intrinsic HER activity of Pt [110]. However, the high cost and scarcity of Pt have greatly limited its wide applications [111]. To limit the use of Pt, scientists are striving hard for the development of low-cost, alternative metals-based graphene nanocomposites for the HER [109]. For instance, Bai et al. have developed Pd@Pt/Gr composite which showed high HER activity with less content of Pt [112]. Using this catalyst, a current density of up to 791 mA cm−2 at −300 mV (vs RHE) and a Tafel slope of 10 mV dec−1 was obtained. In another study, Co-Ni-Gr (Co-Ni-G) composite was fabricated as electrocatalyst for H2 generation [113]. The ternary electrocatalyst has shown four-fold higher electrocatalytic activity than binary catalyst without graphene. In this case, the highest current density reached 850 mA cm−2 (at 1.6 V) with a Tafel slope of 84.5 mV dec−1 at 40 mA cm−2.
Apart from HER, MNPs@Gr have also been applied for other energy conversion processes including ORR [114]. In particular, these reactions require high quality graphene-based electrodes (particularly metal oxides) to electrocatalyze this type of kinetically sluggish electrochemical reactions [115]. Such as, 3D Fe3O4/Gr (N-doped) composites showed superb electrocatalytic properties for the ORR in alkaline electrolytes [116]. This Gr based electrocatalyst demonstrated lower onset potential, higher current density, lower H2O2 generation and better durability. Recently, S and N doped graphene flakes were immobilized with cobalt spinel oxide (Co3O4) or manganese spinel oxide (Mn3O4) NPs to obtain ORR electrocatalyst [117]. The graphene based electrocatalyst exhibited superior ORR performance which was matching with the results obtained for commercial Pt/C electrocatalysts. In another study, Ag-MnxOy/C composite catalysts were decorated both on Gr and N-doped Gr to explore the activity and stability of the electrocatalyst in ORR, particularly with a focus on investigating the tolerance of the catalyst to ethanol in alkaline medium [118]. The Ag-MnxOy/rGO resulted in a more negative diffusion limiting current density of −3.01 mA cm−2 compared to Ag-MnxOy/NGO (cf. Figure 4).
Figure 4.
(a) Base CV of Ag-MnxOy/rGO and Ag-MnxOy/NGO catalysts at 10 mV s−1 in N2 purged 1 M KOH, (b) Potentiodynamic ORR curves of Ag-MnxOy/rGO and Ag-MnxOy/NGO catalysts [
Moreover, MNPs@Gr has been very attractive for broad application in electrochemical energy storage systems like electrochemical capacitors, different types of batteries systems etc., due to their distinct properties from both physical and chemical aspects [119]. Such as, to address the issues of low ionic conductivity, poor electrode kinetics and cyclic stability, CuO was decorated with Gr to obtain a composite electrode material for supercapacitor [120]. The hybrid electrode demonstrated a high specific capacitance of 326 F g−1 at a current density of 0.5 A g−1. In another study, Gr was combined with different types of metal oxides (ZrO2, WO3 and V2O5) to tackle their low electrical conductivity [121]. Thus, the composites of Gr with these metal oxides has offered efficient pathways for electron transport, increased the mechanical stability and also suppressed the degradation during cycling. In this case, the aforementioned metal oxides with diverse morphologies were decorated on PANI/Gr composites which have showed extended operating potential window (i.e. potential difference: 1.6 to 2.0 V) in 1 M electrolyte (Na2SO4) during the measurement (using three electrode system). The WO3/PANI/Gr and V2O5/PANI/Gr exhibited highest capacitance and energy density. Furthermore, doped graphene with MNPs have also been applied as composite electrode materials for energy storage systems [12]. Such as, in their study, Liu et al., have reported the preparation of Mn3O4 nanodots loaded N-doped Gr based composites [122]. The as-prepared composites have achieved a high specific capacitance of 158.9 F g−1 in a given ionic liquid and showed good rate capability. Upon fabricating a symmetric supercapacitor using the composite a high energy density of 90.7 W h kg−1 in the IL electrolyte was obtained.
Recently, MNPs@Gr composites have been considered as suitable alternatives as anode materials in commercial batteries, particularly in LIBs, as graphite is not able to meet the consumer requirements with its limited specific capacity and rate capability [123]. In these composites, the nanostructured metal or metal oxide particles like Si, Sn, SnO2 Cu2O and Fe3O4 are extremely capable of reacting with a large amount of lithium, while Gr can accelerate electron transport between nano-sized particles and the current collector [124]. The composite consisting of Cu2O nanobeads and hydrogen exfoliated graphene when used as an anode material in LIB, the Cu2O beads acted as a spacer in between the two-dimensional planes and increased the specific capacity of the LIB [125]. Due to the synergist effect between the substances, the initial discharge capacity of the battery enhanced to 2050 mAh/g. Additionally, the performance of MNPs@Gr composites has been further enhanced by designing of novel architectures like sandwich structure etc. [126]. These types of distinct structures improve the electron transfer rate in the composite and protect metal oxides against disintegration and aggregation during cycles. Fang et al., have fabricated a sandwich-structured MNPs@Gr composites consisting of ZnO, NiO on a large scale through self-assembly and subsequent thermal decomposition method [127]. In these composites, the nanostructured metal oxides were deposited between the layers of Gr sheets, which offered space for the accommodation of possible volume change of metal oxides during cycles, and improved the electronic conductivity of the composites. When applied as anode materials in LIBs, the sandwiched structured composites showed higher capacities, better cycle and rate performances. In another study, ultrafine Co3O4 NPs (<10 nm) were deposited through pyrolysis of graphene and MOF (ZIF-67) based hybrid [128]. When applied as anode material of LIB, the composite showed high rate behavior and long-term cycling stability. In another study, MOF derived hierarchical hollow NiO/Ni/Gr composite was fabricated using Ni based MOFs and successive carbonization and oxidation treatments. The composites showed superior performance as the anode in LIBs and sodium ion batteries (SIBs), the superior activity of the hybrid was attributed to the high storage of lithium and sodium in the distinct hierarchical hollow ball-in-ball structure of NiO/Ni/Graphene composites [129].
4. Inorganic NPs and ordered mesoporous carbon (MNPs@OMC) based composites
OMCs are flexible carbonaceous substances offering well-organized interconnected channels which are beneficial for the diffusion of electroactive species in electrochemical processes [130]. Unlike other carbon materials, OMCs possesses distinct properties [131]. However, due to the lack of clarity in the nomenclature used to describe this class of mesoporous materials, the electrochemical potential of OMCs has not been fully recognized [132]. Despite having an ordered pore structure, the electrochemistry of OMC is still not completely understood [133]. Based on the IUPAC classification of porosity, mesopores materials are characterized by having pore sizes ranging between 2 to 50 nm, while the micropores are <2 nm, and macropores are >50 nm [134]. In the perspective of molecular diffusion and transportation of ions, OMCs are more compelling, due to their ideal pore size, which are accessible to these species [130]. In contrast, microspores may not be easily reachable, while macropores are too large, leading to small specific surface area. OMCs are typically synthesized by a variety of methods, including catalytic activation of carbon precursor using metal-containing species, carbonization of organic aerogels, utilizing mesoporous silica templates etc. [135]. Among various approaches, hard-template methods have gained considerable recognition which offer better control on the pore size leading to the formation of highly ordered structures [136]. OMCs are often used as the template for the preparation of mesoporous electroactive material by combining them with other functional materials including MNPs [137]. This leads to the formation of a uniformly distributed MNPs in the resulting electroactive nanocomposite. In these composites, OMCs not only contribute to the electrical conductivity but also facilitates the separation of electroactive materials to become more electrochemically accessible [138].
Typically, in the case of electroactive materials binders are applied for the fabrication of electrodes, which are often electrochemically inactive [139]. Besides, they usually hinder the diffusion of electroactive species leading to the decreased specific energy and electrochemical power. In these scenarios, OMCs improve the chances of interaction with electroactive materials due to their interconnected channeled structure [140]. MNPs@OMC offer a multitude of benefits, including a large surface area, customizable pore size and shape, a porous structure, and chemical stability [141]. Additionally, these materials provide optimal electrical conductivity, which can enhance catalyst efficiency and produce synergistic effects when used in electrochemical processes in different capacities like electrode materials, electrocatalysts etc. [142]. Primarily, OMCs are used as MNPs based electrocatalysts support in energy conversion devices like fuel cells etc., which facilitate uniform distribution of catalysts and offer high mesoporosity for the transistor of the medium, as well as high chemical inertness [143]. Especially, in the case of MNPs@OMC composites consisting of uniformly distributed MNPs, the ordered mesopores of OMC act as chemical reactors and provide sufficient catalytic performance [144].
For example, Yang et al., have demonstrated the improved activity and durability of the Pt@OMC based catalyst towards ORR. The electrocatalyst was prepared by deposition of PtCo NPs on hierarchically ordered OMC and applied in PEMFCs [145]. Zheng and co-workers [79] first prepared Mn3O4@polyaniline core/shell NPs using hydrothermal process and the resulting hybrid was subjected to heat treatment and partial acid leaching of MnO to obtain mesoporous structure material. As cathode material in fuel cell, the MnO-m-NC exhibited excellent ORR activity. In another study, Wang et al., developed FeOx@graphitic carbon core-shell structured NPs which were deposited in N-doped OMC (FeOx@GC-NOMC) [146]. When applied in fuel cell, the composite exhibited superior electrocatalytic activity in acidic media, followed a four-electron ORR process, and showed enhanced activity when compared with commercial Pt/C (20 wt %). Similarly, Zhang et al., have developed nanocomposites consisting of rock salt type nickel oxide and cobalt oxide and OMC, which were used as electrocatalysts for the OER in alkaline solution [147]. The NiCo2O3@OMC exhibited the lowest overpotential of 281 mV at 10 mA/cm2 in 1 M KOH, and showed a good durability without obvious attenuation after continuous operation test for 230 h.
Apart from these, the MNPs@OMC have also been used as electrode materials in electrochemical energy storage devices like LIBs, supercapacitors etc., and exhibited excellent electrochemical performance due to the synergic properties of different materials involved [148]. The composites offered easy access between the electrode and electrolyte, enhanced the charge transfer which resulted in enhanced specific capacity [149]. In a recent study, Arya et al., have prepared TiO2@OMC composite electrodes for supercapacitor (SC) applications [150]. The composite electrode delivered a specific capacitance of ~280F/g (95% capacitance retention after 1000 cycles) which is attributed to faster charge dynamics within electrode material. In another study, Cao et al., have prepared well-defined Fe3O4@MNC composite as anode material for LIB [151]. The tubular structure of composite offered effective accommodation for the volume change, fast transport paths for electrons and ions, as well as good contact for electroactive NPs. The composite maintained a high specific capacity of ∼800 mAh g − 1 after 1000 cycles at 2000 mA g−1.
5. Inorganic NPs and fullerene (FL) based (MNPs@FL) composites
Fullerenes are a highly appealing form of carbon allotropes that possess a unique cage-shaped structure made up of conjugated network of sp2-hybridized carbon atoms [152]. These materials have gained significant interest in recent years due to their well-defined structures, exceptional electron-accepting capabilities, and superb ability of transporting electrons [153]. As a result, they are being used as fundamental building blocks to construct functional micro/nanostructures and supramolecular assemblies at variable scales with a variety of controlled synthetic approaches [154]. Notably, the properties of fullerene micro/nanostructures can be modulated or greatly improved by arranging fullerene molecules in a regular pattern [155]. There are several methods available for the production of fullerene derivatives, including solid-state methods, liquid-state methods, deposition, and spraying techniques etc. [156]. Among these methods, solid-state processing routes like powder metallurgy (PM) and friction stir processing (FSP) are the most commonly used for the fabrication of these materials [157]. The combination of fullerenes with other functional materials, such as, CNTs, inorganic nanoparticles (metal and metal oxide NPs), polymers, metal-porphyrins etc., has resulted in the creation of numerous useful hybrids and composites [158]. Over the last few decades, there has been significant research conducted on fullerene-based nanocomposites, which have shown great potential for several applications [159]. Some of these applications include energy conversion and storage, microelectronics, optics, and as thin films, organic polymers, and organic-inorganic nanocomposites etc. [160].
Recent research studies have suggested that fullerenes-based composites can be effectively used as alternate materials for electrochemical energy applications [161]. However, despite of highly symmetrical structure of fullerenes that contributes towards its stability, the poor specific surface area and low conductivity of fullerenes limit their potential applications in energy storage and conversion technologies [162]. Additionally, the poor specific surface area of fullerenes is another challenge issue, which has a direct impact on the material’s performance in energy and environmental applications [163]. Nevertheless, the composites of fullerene with metal and/or metal oxide nanostructures has exhibited promising outcomes in addressing these concerns [164]. These materials have shown remarkable ability of transporting electrons from one fullerene cage to another [165, 166]. On the other hand, the specific surface area and pore volume of fullerene materials can be effectively improved by introducing porous materials like metal oxides and so on [167]. This has led to the development of novel MNPs@FL composites with multifunctional properties which have created new opportunities in the field of energy applications (such as storage and generation) [168].
Recently, Benzigar et al., have incorporated ultra-small α-Fe2O3 NPs inside the channels of highly ordered mesoporous C60 [169]. The composite has shown distinct doughnut-shaped morphology, highly ordered porous structure and high specific surface area (∼598 m2 g−1) which resulted in enhanced electrochemical properties. In addition, the hybrid has delivered a specific capacitance of 112.4 F g−1 at 0.1 A g−1. In another study, Esmail et al., have prepared onion like MnO2-Fe3O4@Fl hybrids using an annealing method [170]. The nanocomposites showed enhanced electrochemical performance with very low charge transfer resistance (7 Ω) with a reversible specific capacity (456 F g−1 at a current density of 4 A g−1). Apart from these, MNPs@FL have also been successfully utilized for various energy conversion processes such as HER, ORR, etc. For example, a lattice-confined
6. Conclusion
This chapter, is a part of a book on
Acknowledgments
The authors extend their appreciation to the Deputyship for Research and Innovation, “Ministry of Education” in Saudi Arabia for funding this research work through the project number (IFKSUDR_E120).
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