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Review

Recent Advances in the Multifunctional Natural Gum-Based Binders for High-Performance Rechargeable Batteries

by
Vinod V. T. Padil
1 and
Jun Young Cheong
2,*
1
Department of Nanomaterials in Natural Sciences, Institute for Nanomaterials, Advanced Technologies and Innovation (CXI), Technical University of Liberec (TUL), Studentská 1402/2, 461 17 Liberec, Czech Republic
2
Bavarian Center for Battery Technology (BayBatt) and Department of Chemistry, University of Bayreuth, Universitätsstraße 30, 95447 Bayreuth, Germany
*
Author to whom correspondence should be addressed.
Energies 2022, 15(22), 8552; https://doi.org/10.3390/en15228552
Submission received: 12 October 2022 / Revised: 7 November 2022 / Accepted: 12 November 2022 / Published: 15 November 2022
Browse Figures
Versions Notes

Abstract

:
Natural gum derived from the natural surrounding (gum arabic, guar gum, xanthan gum, gellan gum, fenugreek gum, karaya gum, and acacia gum) is one of the most abundant polysaccharides currently present around the world. As natural gum dissolved solution can be very sticky in nature, its role as a binder for both anodes and cathodes in rechargeable batteries have been recently significantly researched. Although much research has been delved into using natural gum as a feasible binder for rechargeable batteries, little investigation so far has taken place to compile, summarize, analyze, and evaluate the current status-quo of the natural gum-based binder research, as well as understanding some of the obstacles and issues that may need to be addressed. This review gives a comprehensive review on the natural gum-based binder that was used for both anode and cathode in rechargeable batteries and how each kind of natural gum improved the electrochemical performance in terms of cycle retention and rate capabilities. Furthermore, more systematic analysis and future projections for the research on natural gum-based binders are presented, which will serve to further the promising research related to utilizing natural gum as an efficient binder for rechargeable battery systems.

1. Introduction

Over the last three decades [1], the concept of a “rechargeable energy storage system” has incurred numerous research outputs, including not only Li-ion batteries but also other alternative batteries. This is in an agreement with the global trends that rechargeable energy storage systems have been sought as a next-generation power source for electric vehicles and electronics, as reported in previous works [2,3]. To realize stable high-energy-density batteries, it is important to fabricate advanced rechargeable batteries that can maintain their capacity for a long duration of time [4]. In this sense, a binder plays a pivotal role, as many of battery characteristics, such as irreversible capacity losses, cycling stability, rate capabilities, are highly dependent on the properties of binders [5,6]. By definition, a binder is composed of one or more polymers that are electrochemically inactive but are possible to provide mechanical strength between active materials and the current collector. Here, the role of a binder is providing strong adhesion between the active material and current collector, which will lead to more stable electrochemical performance. Therefore, it is integral to use a suitable amount and type of binder, because its functional groups, mechanical properties, and ionic transport—its key properties—are dependent on it.
Up to the present, the conventional electrode materials have been combined with polyvinylidene difluoride (PVdF), but some critical issues are present. For some prospective anode materials, such as Si, PVdF suffers from its weak van der Waals interaction [7], which should be improved for a more efficient binder. To overcome the limitation of PVdF, a number of materials have been utilized as a binder, and many of them showed some degree of potential. For instance, Liu et al. reported on multifunctional cellulose nanocrystals [8], which had a high aspect ratio and provided robust binding energies. Along with that, attempts to replace non-aqueous PVdF with various aqueous binders were also present, some of which include lithium polyacrylic acid [9], chitosan sulfate ethylamide glycinamide [10], sodium alginate [11], fluorine acrylic hybrid latex [12], dextrin [13], and cyanoethylated carboxymethyl chitosan [14]. Additionally, other works reported on combining different binders together to improve the electrochemical performance, such as polyacrylic acid/carboxymethyl cellulose [15], polyvinyl alcohol/sodium alginate [16], polyacrylic acid/polyvinyl alcohol [17], chitosan-rGO [18], chitosan-g-polyacrylic acid [19], and DNA-alginate [20]. Alongside with such attempts, highly elastic binders were also devised to improve the mechanical strength between the active material and current collector [21], resulting in improved electrochemical performance. Nevertheless, most of these newly devised binder materials either are synthesized chemically and/or underwent complicated synthetic process, showing great limitations. In this aspect, it is important to probe into sustainable materials that can be constantly produced from nature and are abundant.
Green materials are materials that are local and renewable, which are not chemically synthesized from precursors. Among various green materials, gums mainly derived from natural surrounding are eco-friendly polysaccharides possessing a wide range of functional and structural properties [22,23]. Of course, surface modification/treatment can take place in order to tune the physicochemical properties of green materials, where they are considered “green” if the original material is from nature. Due to the intrinsically viscous properties of gums, it is hypothetically reasonable to assume that natural gum-based materials could be utilized as functional binders. In order for natural gum to become a binder, it needs to be mechanically robust, chemically stable, thermally stable, and have good dispersion in a solution to ensure uniform distribution of binder across the electrode—regardless of the battery types. Moreover, since different natural gums are produced from diverse set of natural surroundings, they have a widespread variation in the length of linear chain, branching characteristics, and molecular weight [24]. Attributed to their diverse characteristics, they have shown different electrochemical performances as functional binders for rechargeable batteries, not only limited to Li-based batteries but also in Na-ion batteries. In this review, we would like to delve into the physicochemical properties of various types of natural gums used as binders for rechargeable batteries, how they were utilized in different rechargeable battery system, and we would like to evaluate and project some of the future research directions for natural gum-based binders. Throughout this review, it is expected that a more rationally designed approach can be built up for natural gum-based binders prior to experiments, which can greatly enhance the overall speed at which research on natural gum-based binders can proceed.

2. Physicochemical Properties of Various Types of Gums

Not all types of natural gums have yet been utilized as a binder for rechargeable batteries, but some of them have shown tremendous improvement in the overall electrochemical performance, while using the same electrode materials. The schematic illustration on the chemical structure of gum arabic (GA), guar gum (GG), xanthan gum (XG), gellan gum (GEG), fenugreek gum (FG), karaya gum (KG), and acacia gum (AG) is shown in Figure 1, each showing a unique chemical structure [25,26,27,28,29,30]. Although these are chemical structures mentioned in previous literature, depending on the extraction methods and the condition of the natural gums and where they were extracted, more diverse chemical structures are possible to incur. Moreover, many chemical modification methods are possible to turn natural gum into multifunctional gum with different physicochemical properties.
For example, XG possesses abundant hydroxyl groups, and graft copolymerization can be employed to modify the physicochemical properties of XG [31]. Various functional properties such as adsorption efficiency, swelling, and pH-sensitivity were modified through graft copolymerization, which also has the possibility to be employed when gum is employed as a binder for rechargeable batteries. Various enzymatic, physical, and chemical modification methods were described in a review paper for XG [32], where it is expected to chemically modify the properties of various gums present. This is also the case for FG [28], GA [33], GG [34], GEG [35], KG [36], and AG [37], which is an important aspect to be considered. In addition to the chemical modification of each respective gum, research has indicated the use of a combination of natural gum with other chemicals such as soy protein hydrolysate [38], polyvinylidene pyrrolidone (PVP)/dextrin [39], starch [40], sodium carboxymethyl cellulose and silicon dioxide [41], and hydroxymethyl cellulose/red cabbage pigment [42].

3. Applications in Rechargeable Batteries

3.1. Li-Ion Batteries

Natural gum-based binders have been used in various active materials for Li-ion batteries, both in anode and cathode system. For the anode part, natural gum-based binders have been extensively used for Si-based electrode material [43], and a number of interesting results have resulted. Jeong et al. employed a millipede-inspired design principle to combine XG together with Si, which resulted in extraordinarily outstanding electrochemical performance [43]. Chemical structures of various polysaccharide binders, including XG, are presented in Figure 2a, where they can be further divided into neutral (cellulose, amylose, and amylopectin) and charged groups (carboxymethyl cellulose (CMC), alginate, Na/Li-XG, and XG). Based on the experiments, when native XG is used as a binder, it exhibits outstanding electrochemical performance, far superior to other polysaccharides reported at the time. Such enhanced electrochemical performance could be ascribed to the supramolecular ion–dipole interactions in each side chain of XG, which acts as a millipede’s adhesive role (Figure 2b). Stronger adhesive force found in charged groups is further verified through film adhesion test (Figure 2c), where charged groups (native-XG, Na-CMC, and alginate) exhibit high adhesion force attributed to strong ion–dipole interactions. Native-XG shows the highest load (N), demonstrating its strong adhesion property. Furthermore, XG exhibits good binding also with the Cu current collector, where a bare Cu surface did not appear for XG even after peeling, while two other samples (Si-Na-CMC and Si-alginate) did appear (Figure 2d). Attributed to the ion–dipole interactions of XG that enables more compact points of adhesion between XG and Si as well as strong binder–current-collector interaction, an Si electrode with XG exhibits outstanding cycle retention characteristics (Figure 2e) and rate capabilities (Figure 2f), even at 12 C rate.
Along with this inspiring work came a number of more updated studies utilizing natural gum as a functional binder together with Si and other anode materials. For example, Ling et al. discovered that AG could also be used as a dual-functional binder together with Si, attributed to its hydroxyl groups and mechanically stable glycoprotein chains [44]. In another study, GG was used as a functional binder for Si nanoparticle, which resulted in an initial discharge capacity as high as 3364 mAh g−1 with an initial coulombic efficiency of 88.3% [45]. It was further utilized for Si-C composite anodes, also delivering specific capacities of 780 mAh g−1 and 600 mAh g−1 at 0.05 A g−1 and 0.2 A g−1, respectively [46]. Furthermore, KG was also employed as a functional binder together with Si, which resulted in excellent electrochemical performance (specific capacity of 2421 mAh g−1 at 1.5 A g−1) [47]. The multi-branched structure and abundant polar groups of KG enable superior electrochemical performance, with a more stable electrode structure. FG was also found to show its potential as a novel binder [48], where hydroxyl and carbonyl groups of FG led to excellent electrochemical stability and higher specific capacity. Additionally, modified GEG also acted as a functional binder to boost up electrochemical performance of Si [49], where the modified polysaccharide chain forms strong hydrogen bonding with the surface of Si. Combinatorial effects of natural gums with other researched binders were also proven, in the case of mixing carboxymethyl cellulose (CMC) together with GG. By modulating the mass ratio of two different components (GG and CMC), the electrochemical performance could be optimal [50], combining synergistic effects of two components. To summarize, Si has been the most frequently used active material together with various kinds of natural gum-based binders, which showed much enhanced electrochemical performance.
Natural gum-based binders have also been utilized in other kinds of anode materials for Li-ion batteries. One prominent example is ZnCo2O4, which exhibited superior electrochemical performance [51,52,53]. GG was utilized as a binder for ZnCo2O4 anode material, which resulted in superior electrochemical performance [54]. To understand the interaction between GG and ZnCo2O4, FTIR spectra were plotted and analyzed (Figure 3a). After mixing GG with ZnCo2O4, a shift of bands to 3432, 1158, 1087, 1046, and 1627 cm−1 took place, while a new peak at 1121 cm−1 appeared. Such a shift and formation of new peak hinted the strong hydrogen interaction between the hydroxyl group of GG and oxygen part in ZnCo2O4, leading to more mechanical stability compared with PVdF binder that had weak van der Waals interactions with ZnCo2O4. Within GG chains, various interaction sites are apparent, combined together with metal oxide (e.g., ZnCo2O4) (Figure 3b). As a result, ZnCo2O4 combined with GG binder not only exhibits much enhanced cycle retention characteristics (Figure 3c) but also excellent rate capabilities (Figure 3d). Ex situ SEM analyses before and after the first cycle (Figure 3e–i) further demonstrate that minimal volume change (<20%) took place after the first cycle, while no signs of cracks and pulverization were present. The implementation of a natural gum binder was also applied for NiFe2O4 [55], graphite [56], and Co3O4 [57], leading to much improved electrochemical performance through enhanced mechanical properties by the introduction of a natural gum binder.
The application of natural gum-based binders was not restricted to anode materials; they were also extended to cathode materials. For example, Zhang et al. reported on utilizing XG as a double-helix-superstructure aqueous binder to operate a Li-ion battery, showing a much-improved electrochemical performance [58]. Schematic illustration on the overall postmortem morphology of Li[Li0.144Ni0.136Co0.136Mn0.544]O2 with PVdF (Figure 4a) and XG (Figure 4b) binder after cycling is shown, where introduction of XG leads to highly stable structure. As theoretically expected, Li[Li0.144Ni0.136Co0.136Mn0.544]O2 used with XG shows stable electrochemical performance both at 0.1 C (Figure 4c) and 0.5 C (Figure 4d). Indeed, even after cycling, the overall morphology of Li[Li0.144Ni0.136Co0.136Mn0.544]O2 did not alter significantly (Figure 4e), attributed to the introduction of the XG binder. The influence of XG on the electrochemical performance was also demonstrated for LiFePO4 [59], where the introduction of XG led to favorable electrochemical kinetics, more homogeneous distribution of active materials and black carbon, and good maintenance of structural integrity. XG was also recently adopted for Li[Li0.2Co0.13Ni0.13Mn0.54]O2 (NCM) cathode [60], which showed the effectiveness of aqueous binder on cathode. Non-XG type gum was also investigated as a functional binder. GG was applied for Li-rich cathode (Li1.14Ni0.18 Mn0.62O2) [61], which also led to significantly suppressed voltage and capacity fading. Li1.14Ni0.18 Mn0.62O2 combined with GG binder maintained considerable reversible capacity up to 250 cycles at 0.1 A g−1, attributed to the stabilization of Ni2+/Ni4+ region during cycling. As such, gum macromolecular binders were utilized for both anode and cathode materials, which resulted in significantly enhanced electrochemical performance.

3.2. Li-S Batteries

Li-S batteries have attracted considerable attention, due to their high theoretical capacity (1675 mAh g−1), high theoretical energy density (2600 Wh kg−1), and low cost of S [62]. On the other hand, several critical issues of S are present: (i) large volume change of S, (ii) polysulfide dissolution that leads to shuttling effect, and (iii) the insulating nature of S. To overcome these issues, it is important to come up with a suitable binder for advanced Li-S batteries [63], which can best address some of the issues presented above. By using a suitable binder that can capture polysulfides and provide more mechanically stable electrode structure, improved electrochemical performance is expected. One prominent example of such binder is a L-Cysteine-modified AG (L-AG), which proved to be an efficient binder for high-performance Li-S batteries [64]. The chemical structure of L-AG is shown in Figure 5a, where AG is functionalized by L-Cysteine through chemical reaction between –SH bonding of L-Cysteine and –OH group of AG. Polysulfide (Li2S6) adsorption test (Figure 5b) shows that L-AG captures polysulfide best among various types of binders. Such capturing ability is attributed to the preferred binding characteristics of Li2S6, where it prefers to bind to L-AG with a cyclic structure (Figure 5c). When L-AG is compared with PVdF and AG for cycle retention tests (Figure 5d) and rate capabilities tests (Figure 5e), L-AG binder exhibited the most stable electrochemical performance as well as excellent rate capabilities. Ex situ SEM images of S electrode with PVdF, AG, and L-AG after cycling are shown in Figure 5f–h, where structural integrity is visibly seen for L-AG, in comparison with PVdF. Mechanical strength and polysulfide capture were simultaneously realized by the introduction of L-AG, leading to more stable electrochemical performance. Other types of natural gum-based binders, such as GG and GA, were also probed as binder in Li-S batteries [65,66,67], resulting in enhanced electrochemical performance.
Furthermore, a more innovative approach towards advanced natural gum-based binder for Li-S batteries also occurred. Liu et al. reported on combining GG and XG together (by stirring and mixing them in water) to make a mechanically robust network binder compared with either GG or XG, which provided unique physicochemical properties [68]. Such robust biopolymer network was fabricated by weaving, which was possible by the intermolecular binding of functional groups present in both GG and XG. High S loading was possible for this robust binder, which was also low cost and environmentally friendly. Li-S batteries using this hybrid binder exhibited a high S loading of 19.8 mg cm−2 and an areal specific capacity of 26.4 mAh cm−2, which was unprecedented among the state-of-the-art Li-S batteries.

3.3. Na-Ion Batteries

Na-ion batteries have attracted considerable attention due to the low cost and high availability of Na [69]. In addition to the application of binders in Li-based batteries, that in Na-ion batteries was also present. Recently, Xu et al. reported on utilizing GA as a functional binder for Na-ion batteries, where it provided better mechanical strength and binding capabilities [70]. A schematic illustration of the fabrication process is shown in Figure 6a. Attributed to the higher mechanical strength provided by GA, α-Fe2O3 used together with GA provides higher friction coefficient (Figure 6b) and smaller indentation depth (Figure 6c). Except for the large irreversible capacity found in the first cycle (Figure 6d), α-Fe2O3 used together with GA presents not only enhanced rate capabilities (Figure 6e) but also a very reversible reaction with Li (Figure 6f). Natural gum-based binders were also utilized for different types of electrodes. Zhang et al. reported on utilizing XG to improve the cycling stability of Na2/3Mn2/3Ni1/3O2, maintaining 77.6% of capacity at 0.04 A g−1 and 66% of capacity at 0.1 A g−1 after 80 and 200 cycles [71]. Since XG contains a number of –OH and –COO- functional groups, it provides better adhesion between the active materials and the conductor, resulting in better electronic conductivity. Furthermore, XG was further suggested as one of the feasible binders in combination with organic electrode material [72]. Oxygen-rich active material, sodium rhodizonate dibasic (SRD), was combined with XG to improve the electrochemical performance, which led to stable electrochemical performance. Although utilizing natural gum-based binders for Na-ion batteries is still limited, further optimization of electrochemical performances is expected when more in-depth studies are carried out using suitable gum types.

4. Summary and Conclusions

In summary, natural gum-based binders have been utilized in various forms of the rechargeable battery, ranging from Li-ion batteries to Na-ion batteries. Employing natural gum-based binders leads to much-enhanced electrochemical performance, both in terms of cycle retention and rate capabilities. There are different reasons for why natural gum-based binders lead to improved electrochemical performance, which can be summarized as shown below, with appropriate lists of equipment and tests that were used:
  • Natural gum-based binders lead to better mechanical properties, hence resulting in better adhesion between the current collector and active materials (nanoscratch test, force-displacement test, Fourier-transform infrared spectroscopy (FTIR), scanning probe microscopy (SPM), scratch test, peeling test, scanning electron microscopy (SEM), proton nuclear magnetic resonance (1H-NMR), optical microscopy, adherence test, and nanoindentation test).
  • Natural gum-based binders lead to enhanced electronic conductivity, as it shows good adhesion between the active materials and conductive material (e.g., Super P carbon black), conductive material and current collector, and current collector and active material (Kelvin probe force microscope, electrochemical impedance spectroscopy (EIS) analysis).
  • Natural gum-based binders contribute to the formation of stable solid electrolyte interphase (SEI) layer, which allows more stable interface between the electrode and electrolyte (SEM).
  • Natural gum-based binders prevent the electrode corrosion from electrolyte. Particularly, for XG, such phenomenon takes place due to abundant hydroxyl/carboxylate functional groups as well as the special double helix structure (photographs of binders in electrolytes, FTIR, X-ray photoelectron spectroscopy (XPS), and 1H-NMR).
  • Natural gum-based binders demonstrate good thermal stability, leading to the safety of the rechargeable batteries (thermogravimetry analysis, differential scanning calorimetry analysis).
  • Natural gum-based binders show good flowability and allow effective dispersion of active materials and conductive materials, leading to uniform distribution of each component for slurry (rheology analysis).
  • Natural gum-based binders have fast transfer of Li ions and good ionic conductivity (cyclic voltammetry and others).
  • For Li-S batteries, natural gum-based binders are capable of capturing polysulfides, mitigating the shuttling effect arising from polysulfide dissolution (photographs, UV-visible spectrometer, simulation, XPS, and FTIR).
As can be shown above, natural gum-based binders have multifunctional roles in improving the electrochemical performance, and it is different from one study to another. Moreover, there is still no definitive answer as to which natural gum is best suitable to which electrode material. The fundamental mechanism on the interactions between gum binder and active material are mostly investigated experimentally, which can be enhanced by the combination with theoretical simulations. Electrochemical performance was summarized for each electrode material utilizing different natural gum-based binders (Table 1), where the electrochemical performance of the same type of natural gum varied from one place to another. To compare the electrochemical performance of electrode materials utilizing different natural gum-based binders, Si anode and S cathode were chosen. The electrochemical performance was evaluated for Si with different natural gum-based binders through cycle retention (Figure 7a) and rate capabilities (Figure 7b). GA shows considerable cycle retention characteristics, while FG shows the most outstanding rate capabilities. Similarly, for S electrode, GA exhibits the best cycle retention characteristics (Figure 7c) but GG shows the most outstanding rate capabilities (Figure 7d). Although the previous works were published in different time periods and the other variables (such as condition for electrolyte, loading amount of binder) are present, it can be suggested that GA seems to show the most stable cycling performance, while no key natural gum-based binders are present for high-rate capabilities. More in-depth studies should be carried out to further find out the optimal concentration at which each natural gum-based binder could be used, which can be applied to different types of electrode materials. Inspired from recent review papers on energy storage systems [73,74], it is also desirable to combine autonomous chemistry as well as artificial intelligence together with binder optimization for rechargeable batteries (energy storage system), which will yield significant advances in the given field. Lastly, as most of a binder is electrically insulating, more research effort should be present to find the optimal amount of binder that minimizes the use of binder as well as retain the improved mechanical properties by using the binder. Careful investigation on effect of different parameters of binder (e.g., functional group, molecular weight, concentration, glass transition temperature) on the properties of binder (good mechanical strength, chemical stability, thermal stability, and good dispersion) needs to be systematically performed.

Author Contributions

Conceptualization, V.V.T.P. and J.Y.C.; methodology, J.Y.C.; software, J.Y.C.; validation, V.V.T.P. and J.Y.C.; formal analysis, V.V.T.P. and J.Y.C.; investigation, V.V.T.P. and J.Y.C.; resources, J.Y.C.; data curation, J.Y.C.; writing—original draft preparation, J.Y.C.; writing—review and editing, V.V.T.P. and J.Y.C.; visualization, J.Y.C.; supervision, J.Y.C.; project administration, V.V.T.P. and J.Y.C.; funding acquisition, V.V.T.P. and J.Y.C. All authors have read and agreed to the published version of the manuscript.

Funding

This work was supported by Bayerisch-Tschechische Hochschulagentur (BTHA) (BTHA-AP-2022-45).

Data Availability Statement

Not applicable.

Conflicts of Interest

The authors declare no conflict of interest.

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Figure 1. Chemical structures of (a) GA [25], (b) GG [26], (c) XG [26], (d) GEG [27], (e) FG [28], (f) KG [29], and (g) AG [30].
Figure 1. Chemical structures of (a) GA [25], (b) GG [26], (c) XG [26], (d) GEG [27], (e) FG [28], (f) KG [29], and (g) AG [30].
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Figure 2. (a) Chemical structures of various neutral and charged polysaccharide binders, ranging from cellulose to XG. (b) Wide-scale illustration of role of XG in contributing to strong adhesion to Si, through a series of multiple short side chains in native XG (colored in red). (c) Film adhesion tests (peeling test) based on different binders. (d) Optical images for different binders before and after peeling. (e) Cycle retention and (f) rate capabilities tests of Si electrode with XG binder [43].
Figure 2. (a) Chemical structures of various neutral and charged polysaccharide binders, ranging from cellulose to XG. (b) Wide-scale illustration of role of XG in contributing to strong adhesion to Si, through a series of multiple short side chains in native XG (colored in red). (c) Film adhesion tests (peeling test) based on different binders. (d) Optical images for different binders before and after peeling. (e) Cycle retention and (f) rate capabilities tests of Si electrode with XG binder [43].
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Figure 3. (a) FTIR spectra of GG and ZnCo2O4 mixed with GG. (b) Schematic illustration of the mechanically stable network formed between GG and metal oxides (ZnCo2O4). (c) Comparison of cycle retention characteristics of ZnCo2O4 used with GG and PVdF binder. (d) Rate capabilities tests of ZnCo2O4 used with GG binder. Cross-section SEM images of ZnCo2O4 with GG binder (e) before cycling and (f) after the first cycle. SEM images of ZnCo2O4 with GG binder (g) before cycling, (h,i) after the first cycle [54].
Figure 3. (a) FTIR spectra of GG and ZnCo2O4 mixed with GG. (b) Schematic illustration of the mechanically stable network formed between GG and metal oxides (ZnCo2O4). (c) Comparison of cycle retention characteristics of ZnCo2O4 used with GG and PVdF binder. (d) Rate capabilities tests of ZnCo2O4 used with GG binder. Cross-section SEM images of ZnCo2O4 with GG binder (e) before cycling and (f) after the first cycle. SEM images of ZnCo2O4 with GG binder (g) before cycling, (h,i) after the first cycle [54].
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Figure 4. Schematic illustration on the postmortem morphology of Li[Li0.144Ni0.136Co0.136Mn0.544]O2 after cycling using (a) PVDF and (b) XG as a binder. Cycle retention characteristics of Li[Li0.144Ni0.136Co0.136Mn0.544]O2 at (c) 0.1 C and (d) 0.5 C with a PVDF and XG binder. (e) Ex situ SEM images of Li[Li0.144Ni0.136Co0.136Mn0.544]O2 with XG as a binder after cycling, along with photographs of electrode (left top) and separator (left bottom) [58].
Figure 4. Schematic illustration on the postmortem morphology of Li[Li0.144Ni0.136Co0.136Mn0.544]O2 after cycling using (a) PVDF and (b) XG as a binder. Cycle retention characteristics of Li[Li0.144Ni0.136Co0.136Mn0.544]O2 at (c) 0.1 C and (d) 0.5 C with a PVDF and XG binder. (e) Ex situ SEM images of Li[Li0.144Ni0.136Co0.136Mn0.544]O2 with XG as a binder after cycling, along with photographs of electrode (left top) and separator (left bottom) [58].
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Figure 5. (a) Chemical structure of modified AG (L-AG). (b) Photographs of the Li2S6 adsorption by different materials, including L-AG. (c) Geometries and simulated binding energies of Li2S6 on the –NH2 and –COOH groups in L-AG. Comparison of electrochemical performance in terms of (d) cycle retention characteristics and (e) rate capabilities for electrode with different binders (PVdF, AG, and L-AG). Ex situ SEM images of electrode with (f) PVdF, (g) AG, and (h) L-AG after cycling [64].
Figure 5. (a) Chemical structure of modified AG (L-AG). (b) Photographs of the Li2S6 adsorption by different materials, including L-AG. (c) Geometries and simulated binding energies of Li2S6 on the –NH2 and –COOH groups in L-AG. Comparison of electrochemical performance in terms of (d) cycle retention characteristics and (e) rate capabilities for electrode with different binders (PVdF, AG, and L-AG). Ex situ SEM images of electrode with (f) PVdF, (g) AG, and (h) L-AG after cycling [64].
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Figure 6. (a) Schematic illustration of the electrode fabrication process with GA binder. (b) Friction coefficient and (c) load-displacement curves for α-Fe2O3 combined with PVdF and GA. (d) Charge and discharge profile of α-Fe2O3 combined with GA in the first, second, and third cycle at a current density of 0.2 A g−1. (e) Rate capabilities test of α-Fe2O3 combined with PVdF and GA. (f) Coulombic efficiency of α-Fe2O3 combined with GA [70].
Figure 6. (a) Schematic illustration of the electrode fabrication process with GA binder. (b) Friction coefficient and (c) load-displacement curves for α-Fe2O3 combined with PVdF and GA. (d) Charge and discharge profile of α-Fe2O3 combined with GA in the first, second, and third cycle at a current density of 0.2 A g−1. (e) Rate capabilities test of α-Fe2O3 combined with PVdF and GA. (f) Coulombic efficiency of α-Fe2O3 combined with GA [70].
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Figure 7. Comparison of various natural gum-based binders for Si electrode in terms of (a) cycle retention and (b) rate capabilities. Comparison of various natural gum-based binders for S electrode in terms of (c) cycle retention and (d) corresponding capacity vs. c-rate.
Figure 7. Comparison of various natural gum-based binders for Si electrode in terms of (a) cycle retention and (b) rate capabilities. Comparison of various natural gum-based binders for S electrode in terms of (c) cycle retention and (d) corresponding capacity vs. c-rate.
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Table
Table 1. Summary of electrochemical performance of rechargeable batteries based on natural gum-based binders.
Table 1. Summary of electrochemical performance of rechargeable batteries based on natural gum-based binders.
Types of GumsLoading AmountActive MaterialCycle PerformanceRate CapabilitiesRef.
XG20 wt%Si~800 mAh g−1 at 6.0 C after 500 cycles~750 mAh g−1 at 12 C[43]
GA25 wt%Si1000 mAh g−1 at 1.0 C after 1000 cycles1000 mAh g−1 at 2.0 C[44]
GG15 wt%Si1561 mAh g−1 at 2.1 A g−1 after 300 cycles~1000 mAh g−1 at 12.6 A g−1[45]
GG8 wt%Si-C~600 mAh g−1 at 0.2 A g−1 after 111 cyclesN/A[46]
KG20 wt%Si2421 mAh g−1 at 1.5 A g−1 after 150 cycles1336 mAh g−1 at 4.0 A g−1[47]
FG5 wt%Si1790 mAh g−1 at 1.0 A g−1 after 200 cycles~1400 mAh g−1 at 10 C[48]
GEG20 wt%Si1138 mAh g−1 at 1.0 A g−1 after 200 cycles865 mAh g−1 at 4.0 A g−1[49]
GG1 wt%SiOx/graphite385.7 mAh g−1 after 100 cycles N/A[50]
GG10 wt%ZnCo2O4412 mAh g−1 at 1.2 A g−1 after 600 cycles248 mAh g−1 at 10 A g−1[54]
GA15 wt%NiFe2O4770 mAh g−1 at 5.0 A g−1 after 500 cycles 421 mAh g−1 at 5.0 A g−1[55]
XG6 wt%Graphite250 mAh g−1 at 0.5 C after 180 cycles275 mAh g−1 at 5.0 C[56]
XG15 wt%Co3O4742.5 mAh g−1 at 0.5 C after 50 cycles~750 mAh g−1 at 1.0 C[57]
XG10 wt%Li[Li0.144Ni0.136Co0.136Mn0.544]O2275.6 mAh g−1 at 0.1 C after 200 cycles261 mAh g−1 at 0.5 C[58]
XG5 wt%LiFePO4151.1 mAh g−1 at 0.2 C after 100 cycles87 mAh g−1 at 5.0 C[59]
XG5 wt%Li[Li0.2Co0.13Ni0.13Mn0.54]O2203.2 mAh g−1 at 0.2 C after 50 cyclesN/A[60]
GG10 wt%Li1.14Ni0.18 Mn0.62O2~180 mAh g−1 at 0.1 A g−1 after 250 cyclesN/A[61]
AG22.7 wt%S564.7 mAh g−1 at 1.0 C after 200 cycles500 mAh g−1 at 2.0 C[64]
GG15 wt%S777 mAh g−1 at 0.2 C after 150 cyclesN/A[65]
GG10 wt%S~900 mAh g−1 at 7.0 C after 150 cycles~1000 mAh g−1 at 10.0 C[66]
GA20 wt%S841 mAh g−1 at 0.2 C after 500 cycles460 mAh g−1 at 10.0 C[67]
GG and XG10 wt%S724 mAh g−1 at 0.5 C after 150 cycles737 mAh g−1 at 5.0 C[68]
GA15 wt%α-Fe2O3492 mAh g−1 at 5.0 A g−1 after 500 cycles372 mAh g−1 at 15.0 A g−1[70]
XG10 wt%Na2/3Mn2/3Ni1/3O2115.9 mAh g−1 at 0.2 C after 80 cyclesN/A[71]
XG15 wt%sodium rhodizonate dibasic~150 mAh g−1 at 0.05 A g−1 after 200 cyclesN/A[72]
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Padil, V.V.T.; Cheong, J.Y. Recent Advances in the Multifunctional Natural Gum-Based Binders for High-Performance Rechargeable Batteries. Energies 2022, 15, 8552. https://doi.org/10.3390/en15228552

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Padil VVT, Cheong JY. Recent Advances in the Multifunctional Natural Gum-Based Binders for High-Performance Rechargeable Batteries. Energies. 2022; 15(22):8552. https://doi.org/10.3390/en15228552

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Padil, Vinod V. T., and Jun Young Cheong. 2022. "Recent Advances in the Multifunctional Natural Gum-Based Binders for High-Performance Rechargeable Batteries" Energies 15, no. 22: 8552. https://doi.org/10.3390/en15228552

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