Carbon Materials as Cathode for Dual-Carbon Lithium-Ion Capacitors

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1		Dong Sui	--	3016	2022-12-06 02:12:44	\|
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3	format correct	Jessie Wu	-11 word(s)	3007	2022-12-06 05:19:01	\|

This entry is adapted from the peer-reviewed paper 10.3390/nano12223954

Lithium-ion capacitors (LICs) have drawn increasing attention, due to their appealing potential for bridging the performance gap between lithium-ion batteries and supercapacitors. Especially, dual-carbon lithium-ion capacitors (DC-LICs) are even more attractive because of the low cost, high conductivity, and tunable nanostructure/surface chemistry/composition, as well as excellent chemical/electrochemical stability of carbon materials. Based on the well-matched capacity and rate between the cathode and anode, DC-LICs show superior electrochemical performances over traditional LICs and are considered to be one of the most promising alternatives to the current energy storage devices. The mismatch between the cathode and anode could be further suppressed by applying carbon nanomaterials.

DC-LICs carbon cathode lithium-ion capacitors

1. Introduction

Based on the energy storage mechanism of fast ion adsorption/desorption at the electrode/electrolyte interface, the capacitor-type cathodes are expected to provide high power density and ensure long-term durability in lithium-ion capacitors (LICs). Bearing this in mind, porous carbon materials with high specific surface area (SSA), rich interconnected pores, excellent electrical conductivity, and stable structure are investigated as cathodes. Thus, traditional porous carbons (AC, biomass/polymer-derived porous carbon) and novel nanosized carbons (graphene, carbon nanotubes (CNTs) and their composites) are commonly adopted. The typical examples are summarized in Table 1.

Table 1. Typical carbon cathodes and the electrochemical performances of dual-carbon lithium-ion capacitors (DC-LICs).

Carbon Cathodes			Performances of DC-LICs				Ref.
Materials	Specific Capacity (mAh g⁻¹)	Rate Capability (mAh g⁻¹)	Voltage (V)	Maximum Energy Density (Wh kg⁻¹)	Maximum Power Density (kW kg⁻¹)	Cycling Stability	Ref.
Commercial AC (YP-50F)	48	35 @ 1 A g⁻¹	2.0−4.0	73.0	/	85% after 1000 cycles	^[1]
KHPC−K	100.5	75 @ 10 A g⁻¹	0.01–4.0	169.0	97.0	77.7% after 5000 cycles	^[2]
NHCN-2	125	98 @ 15 A g⁻¹	2.0–4.5	146.0	52.0	91% after 40,000 cycles	^[3]
LPCs-3	80	26 @ 10 A g⁻¹	2.0–4.0	97.0	11.4	92.3% after 5000 cycles	^[4]
DPC-MK	149	69 @ 50 A g⁻¹	1.0–4.2	160.6	39.7	95.6% after 8000 cycles	^[5]
0.1-BNC	113	63 @ 10 A g⁻¹	0.02–4.5	220.0	22.5	81% after 5000 cycles	^[6]
S-NPC-40	95.9	43.2 @ 10 A g⁻¹	0–4.0	176.1	20.0	82% after 20,000 cycles	^[7]
CHPC	132	100 @ 8 A g⁻¹	0.01–4.2	220	66.9	70% after 3000 cycles	^[8]
N/S-CNF0.25	133	102 @ 10 A g⁻¹	1.0–4.3	154.0	18.6	92% after 6000 cycles	^[9]
PHNCNB	72	51 @ 10 A g⁻¹	1.0–4.0	148.5	25.0	90% after 8000 cycles	^[10]
NHPCS	74	64 @ 5 A g⁻¹	0–4.2	151.0	10.7	96.3% after 3000 cycles	^[11]
NCNs-2	115	62 @ 10 A g⁻¹	0–4.5	218.4	22.5	84.5% after 10,000 cycles	^[12]
BNC	75.2	51.4 @ 5 A g⁻¹	1.0–4.0	115.5	10.0	71.6% after 2000 cycles	^[13]
ANCS	113	67 @ 10 A g⁻¹	0–4.5	206.7	22.5	86.6% after 10,000 cycles	^[14]
NPCS-1	97.4	51.3 @ 10 A g⁻¹	0–4.0	135.6	10.0	82% after 10,000 cycles	^[15]
NPCNF	122	53 @ 100 A g⁻¹	1.0–4.3	143.0	45.0	83.1% after 10,000 cycles	^[16]
URGO	35	29 @ 1.1 A g⁻¹	2.0–4.0	106.0	4.2	~100% after 1000 cycles	^[17]
PRGO	171	92.3 @ 8.71 A g⁻¹	0.01–4.0	262.0	9.0	91% after 4000 cycles	^[18]
NGF-0	82	61 @ 8 A g⁻¹	1.0–4.0	147	48.9	87% after 10,000 cycles	^[19]
GPC	95	40 @ 5 A g⁻¹	0–4.2	142.9	12.1	88% after 5000 cycles	^[20]
SGCs	257.1	147.7 @ 6 A g⁻¹	0–4.0	249.9	19.62	95.4% after 10,000 cycles	^[21]
A-N-GS	104	57 @ 5 A g⁻¹	0–4.5	187.9	11.25	93.5% after 3000 cycles	^[22]
MRPG/CNT	108	83.3 @ 5 A g^{− 1}	0–4.5	232.6	45.2	86% after 5000 cycles	^[23]
Zn₉₀Co₁₀-APC	118.8	50 @ 5 A g^{− 1}	2.0–4.0	108	15.0	86% after 10,000 cycles	^[24]

2. Traditional Porous Carbon Cathode

2.1. Activated Carbon

As a conventional porous carbon material used in supercapacitors (SCs), AC has the advantages of acceptable SSA, porous structure, low cost, and mature fabrication technology. Typically, ACs are prepared from carbon-rich materials through activation with KOH, H₃PO₄, ZnCl₂, H₂O, and/or CO₂ at high temperature ^[25]. In the early studies of LICs, AC was usually used as the cathode. For example, the first protype of LIC was fabricated with AC as the cathode and nanostructured Li₄Ti₅O₁₂ as the anode ^[26]. The obtained asymmetric hybrid system shows high energy density, an extended cycle life, and fast charge/discharge capability. Later, several groups developed DC-LICs by pairing AC with graphite ^[27], hard carbon ^[28]^[29], or graphene ^[30]. However, conventional ACs still suffer from low capacity and poor rate capability, due to small SSA and low conductivity, resulting in inferior energy and power densities. Hence, it is highly urgent to develop advanced ACs with high conductivity and desired microstructure.

To further improve the capacity and rate of AC, compositing with nanosized carbons is a feasible method. For example, Ma et al. designed graphene/activated carbon (G/AC) composites through a fast, self-propagating, high-temperature synthesis (SHS) process, which combined the advantages of the two components ^[31]. The conductivity of the prepared G/AC was largely enhanced from 389 to 2941 S m⁻¹, and a remarkable rate performance with 84% capacity retention at 10 A g⁻¹ was achieved, compared with 65% for pure AC. Based on this cathode, the assembled LICs with graphene/soft carbon anode demonstrated a greatly improved energy density of 152 Wh kg⁻¹ and power density of 18.9 kW kg⁻¹.

2.2. Biomass-Derived Porous Carbon

Recently, biomass-derived porous carbons (BDPCs) are emerging as cost-effective electrode materials for DC-LICs, due to their abundance, renewability, and sustainability ^[4]^[32]. Biomass is an economical and environmentally friendly raw material for preparing porous carbon and has the following merits: (1) the diversity of biomass with different nanostructure and morphology provides many choices for preparing porous carbon with desired electrochemical performances; (2) the inherent ordered porous structure of biomass facilitates the activation process to form porous carbon with high SSA and large pore volume; (3) the heteroatom doped porous carbon could be facilely realized via a self-doping strategy ^[33]^[34]^[35]. Particularly, heteroatom doping has multiple advantages. The study by Lee et al. revealed that heteroatom doping is beneficial to the betterment of electrical conductivity and pore generation, which eventually enhances the electrochemical properties of carbonaceous materials ^[36].

Similar to conventional ACs, BDPCs are commonly prepared via a typical carbonization and activation processes ^[2]^[37]. Additionally, BDPCs have porous morphology, stable structure, heteroatom dopants, and high conductivity, endowing SCs or LICs based on them with high energy/power density and good cycling stability ^[35]^[37]^[38]. Several works have explored agricultural waste-derived porous carbons in LICs by pairing with non-carbon anodes, which demonstrate that BDPCs could serve as excellent cathodes ^[39]^[40]^[41]^[42]^[43]. Then, the applications of BDPCs in DC-LICs were investigated. Wang et al. prepared a sponge-like carbon (SLC) from gulfweed through KOH activation and used as electrode material for DC-LICs ^[44]. The obtained sample exhibited a sponge-like structure with rich porosity. Benefiting from the astonishing structure, rational pore size distribution (PSD), and heteroatom doping, the optimized device with SLC as both cathode and anode delivered a high energy density of 127 Wh kg⁻¹ and a peak power of 33.57 kW kg⁻¹. More importantly, an ultra-stable cycling performance with 99% capacity retention was achieved after 100,000 cycles. Ma et al. reported a cathode of N-doped hierarchical carbon nanolayer (NHCNs) through a facile, one-step template carbonization/activation from naturally abundant and renewable chitosan biomass ^[3]. NHCNs has a high capacity of 125 mAh g⁻¹, which could be ascribed to its hierarchically porous structure with large SSA (2350 m² g⁻¹) and high nitrogen doping level. Moreover, DC-LICs based on NHCNs show a maximum power density of 52 kW kg⁻¹ and an ultra-long cycling life of 40,000 cycles. Anyway, graphene is commonly introduced to further enhance the conductivity of BDPCs by forming composites, aiming to achieve higher specific capacity and better rate capability ^[39]^[45]^[46]. It should be noted that biomass-derived carbons have the disadvantages of uncontrollable impurity and element composition, due to the diversity of raw materials. Tedious post treatment is usually needed to obtain products with high purity and good batch stability.

2.3. Polymer-Derived Porous Carbon

Porous carbon materials could also be prepared through pyrolysis and the activation of polymers. Compared with the uncontrollable impurity and element composition of biomass-derived carbons, polymers could be designed and adjusted from the precursors, so that the structure and composition could be well-controlled. Thus, polymer-derived porous carbons receive increasing interests in energy storage devices ^[47]^[48]. For instance, Hung et al. designed a hierarchical porous activated carbon (H-HPAC) material through pyrolysis of polyvinylpyrrolidone (PVP)-derived hydrogel, using K₂CO₃ as both the initiator for hydrogel formation and the activator ^[49]. In the preparing process, the numerous water molecules captured within the PVP function as a green template during the formation of hydrogel, making this method a facile and eco-friendly strategy to design highly porous carbon. As a cathode, H-HPAC demonstrates a capacitance of 128.7 F g⁻¹, due to its high SSA (2012 m² g⁻¹) and large pore volume (1.16 cm³ g⁻¹). Wang et al. proposed a nitrogen-doped activated porous carbon by carbonization and activation of polypyrrole ^[50]. The product has a hierarchically porous structure with plenty of mesopores created by surfactant and micropores generated by activation. The all-carbon LIC delivers a high energy density of 167 Wh kg⁻¹, which still remains 88.9 Wh kg⁻¹ at an ultrahigh power density of 13.2 kW kg⁻¹. Similarly, Ajuria et al. reported an activated carbon from furfuryl alcohol-based polymer by a process of polymerization, carbonization, and activation ^[51]. The obtained cathode material showed a sponge-like surface with high SSA and broad pore distribution. Combined with a hard carbon anode made from the same furfuryl alcohol-derived polymer, the obtained DC-LICs offer a medium energy density of 110 Wh kg^–1 at 7 kW kg^–1 and keep 50 Wh kg^–1, even at an ultrahigh power of 50 kW kg^–1 (discharge in less than 10 s). Although polymer-derived porous carbons have demonstrated advantages over biomass, in terms of purity and controllable composition, the high cost and tedious synthesis process should not be ignored.

As a class of organic porous polymers, conjugated microporous polymers (CMPs), covalent organic frameworks (COFs), and their derivatives have been applied in various energy storage devices ^[52]^[53]^[54]^[55]^[56]^[57]. CMPs and COFs have the merits of well-defined crystal structure, plenty of nanopores, large SSA, and rich heteroatoms, making them the ideal platform to prepare high-performance carbon materials ^[58]^[59]. Therefore, CMPs and COFs could serve as excellent precursors to prepare self-doping porous carbons via a simple pyrolysis process. CMPs/COFs-derived porous carbons have been successfully used as electrode materials in LIBs and SCs ^[60]^[61]^[62]^[63]. However, there are very few reports covering the application of CMPs/COFs-derived porous carbons in LICs or DC-LICs. Hence, more efforts could focus on this field in future research.

3. Nanosized Carbon-Based Cathode

Traditional AC and biomass/polymer-derived porous carbons usually suffer from low capacity, due to too many inaccessible micropores, resulting in inferior energy density. Moreover, their amorphous structure with numerous pores and defects leads to low electrical conductivity and, thus, poor power output. Therefore, nanosized carbons, such as graphene, CNTs, and their composites, are emerging as excellent cathodes for DC-LICs because of their inherently high conductivity and large theoretical SSA.

3.1. Graphene-Based Cathode

Graphene, as a novel two-dimensional (2D) nanosized carbon material, has drawn intensive attention, ever since its discovery and has found numerous applications in energy conversion and storage ^[64]^[65]^[66]. Graphene possesses the following advantages. First of all, the layered structure with long-range conjugation endows graphene with large SSA, high electrical conductivity, and outstanding mechanical strength ^[67]. Anyway, the rich surface chemistry coupled with the 2D structure also makes graphene an excellent substrate for forming composites with other materials ^[68]^[69]^[70]. As a result, graphene-based materials have been adopted as an excellent cathode in LICs ^[71]^[72].

Graphene oxide (GO) is an appealing precursor of graphene-based cathode. GO can be easily dispersed in polar solvent, due to the abundant oxygen-containing groups on the surface or at the edge ^[73]. Moreover, the oxygen-containing functional groups could provide extra capacity via redox reaction ^[65]. Generally, GO should be reduced by high temperature, hydrothermal reaction, or reductants to recover the conjugation structure before being used as cathode ^[17]^[18]^[74]. After the treatment, the reduced GO demonstrates enhanced electrical conductivity. Besides the typical double-layer adsorption/desorption charge storage, the remaining functional groups exhibit reversible Li⁺ binding and facilitate electrolyte infiltration, which largely improves the specific capacity and rate capability ^[17]. Several reports have explored the application of reduced GO-based cathodes in LICs ^[75]^[76]^[77]^[78]. As a typical example, Dubal et al. prepared a partially reduced GO (PRGO) by thermal annealing ^[18]. The obtained sample presented three-dimensional (3D) interconnected networks with open-porous nanosheets, which is expected to contribute a fast charge/discharge rate. Moreover, the partial reduction strategy maintains a substantial amount of C=O redox groups, which could undergo redox reaction with consequent Li⁺ uptake ^[79]. Accordingly, PRGO shows an astonishing capacity of 171 mAh g⁻¹, with an excellent rate of 92.3 mAh g⁻¹ at 8.71 A g⁻¹. The DC-LICs using PRGO as cathode deliver an ultrahigh energy density of 262 Wh kg⁻¹, which keeps 78 Wh kg⁻¹ at a high power density of 9 kW kg⁻¹.

However, the reduced GO suffers from small SSA and poor conductivity because of the unavoidable sheet restacking and incomplete recovery of the conjugation structure, resulting in inferior electrochemical performance. Therefore, highly porous graphene cathodes with higher conductivity and larger SSA are developed by activation or the template-assisted chemical vapor deposition (CVD) method. As a pioneering work, Ruoff et al. developed a graphene cathode (a-MEGO) for LICs through the chemical activation of microwave-expanded graphite oxide to obtain a dense network of nanometer-scale pores surrounded by highly curved carbon layers ^[64]. The a-MEGO demonstrated the porous morphology with a pore size distribution of sizes between ~1 and ~10 nm. More importantly, a-MEGO had a very high SSA of 3100 m² g⁻¹, while retaining the high conductivity of graphene. As expected, the a-MEGO cathode exhibited a nearly symmetric charge/discharge curve and delivered a specific capacitance of 266 and 213 F g⁻¹ at 1.0 and 2.5 A g⁻¹, respectively. By pairing with graphite, the dual carbon-based devices presented a high energy density of 147.8 Wh kg⁻¹ ^[80]. Similarly, Zhang et al. fabricated porous graphene by activation of reduced GO ^[81]. The obtained product had a highly crumpled morphology and porous structure with abundant mesopores that contributed to a high SSA (2103 m² g⁻¹) and large pore volume (1.8 cm³ g⁻¹). This structure provides highly exposed active sites for ion adsorption/desorption and fast transport path for ions and electrons, leading to enhanced capacity and rate.

Besides chemical activation, porous graphene with high conductivity and outstanding structural stability could also be fabricated by chemical vapor deposition with the assistance of hard template ^[82]^[83]^[84]. For example, Xiao et al. synthesized S-doped graphene nano-capsules (SGCs) by CVD with the presence of a MgO template ^[21]. The SGCs exhibited an integrated nano-capsule structure with a uniform size of 50 nm, and no obvious cracked products were observed, indicating that SGCs have a good structural rigidity and stability. SGCs show an extremely high capacity of 257.1 mA h g⁻¹ at 1 A g⁻¹ and an appealing rate capability of 147.7 mA h g⁻¹ at 6 A g⁻¹, both of which are far better than those of the control samples. With SGCs as both cathode and anode, the assembled symmetric LIC delivers an ultrahigh energy density of 249.9 Wh kg⁻¹ at a high power density of 2.12 kW kg⁻¹, which still retains 149.8 Wh kg⁻¹, even at 14.99 kW kg⁻¹. The SGCs//SGCs also presents excellent long-term cycling stability with a retention of 95.4% after 10,000 cycles. It should be noted that the electrode still keeps an intactness and undamaged nano-capsules morphology, even after cycling for 10,000 times, verifying the superior structural stability of SGCs. The above excellent properties could be ascribed to the hollowed and stable structure with an abundant mesopore-dominant porosity, good electronical conductivity, enlarged interlayer spacing, and S-doping of SGCs.

Despite the superb electrochemical performance for pure graphene-based cathodes, the high cost and tedious preparation procedure promotes researchers to explore graphene-based composites. This strategy overcomes the high cost of graphene, but keeps its inherently excellent properties. Moreover, forming composites with other materials could prevent the restacking and agglomerating of graphene. Chen’s group presented a simple and green, but very efficient, approach to prepare 3D graphene-based porous materials through in-situ hydrothermal polymerization/carbonization of the mixture of cheap biomass or industry carbon sources with GO, followed by chemical activation ^[68]^[85]. The optimal product presented a sponge-like morphology and porous microstructure. More importantly, it had an ultrahigh SSA (3523 m² g⁻¹), mesopore-dominated porosity, and excellent bulk conductivity (up to 303 S m⁻¹), thus contributing an outstanding electrode for SCs and LICs ^[72]^[86]. The 3D porous graphene-based cathode demonstrated a high capacity and outstanding rate ^[87]. Benefiting from the dual graphene-based electrodes, the obtained all-graphene LIC with optimized cathode/anode ratio delivered a maximum energy density of 142.9 Wh kg⁻¹ and a peak power energy of 12.1 kW kg⁻¹. Anyway, heteroatom doping was applied to enhance the electrochemical performances of graphene-based materials. For instance, Wang et al. designed 3D porous activated nitrogen-doped graphene sheet (A-N-GS) by aniline polymerization with GO and then KOH activation ^[22]. A-N-GS demonstrated a sheet-like structure with a rough surface and 3D interconnected porous network. Coupled with the 3D highly conductive pathway and high-level nitrogen doping, A-N-GS showed a much improved capacity and rate performance, compared with the non-doped or non-activated samples. With a graphene-based anode, the all graphene LICs could reach an ultrahigh energy density of 187.9 Wh kg⁻¹ at a power density of 2.25 kW kg⁻¹, which still remained at 111.4 Wh kg⁻¹, even at 11.25 kW kg⁻¹.

3.2. Carbon Nanotube-Based Cathode

As a typical one-dimensional nanosized carbon material, the carbon nanotube has exceptional conductivity, large aspect ratio, flexibility, and excellent mechanical strength ^[88]. All these merits make CNTs superior electrode material in various energy conversion and storage systems ^[89]. Particularly, CNTs are excellent substrates for fabricating flexible devices ^[90]^[91]. Nonetheless, similar graphene, CNTs usually demonstrate mediocre electrochemical performance, due to the severe agglomeration issue. As a consequence, forming composites with other materials is a feasible method, in which CNTs serve as either a spacer to increase the SSA or a conductive additive to enhance the electrical conductivity ^[92].

Several reports have verified that CNTs/graphene composites can solve the restacking issue of both the two components and form a 3D conductive network ^[93]^[94]^[95]. Additionally, the increased SSA and the well-distributed nanopores promote electrolyte infiltration and diffusion, endowing the obtained product-enhanced electrolyte accessibility. Hence, the high capacity and excellent rate could be expected for CNTs-based composites. Bai et al. proposed a CNT supported porous graphene (MRPG/CNT) by a facile microwave irradiation method ^[23]. CNT was uniformly distributed between graphene sheets to support the layer structure. The obtained MRPG/CNT cathode showed much improved capacity and rate capability, compared with MRPG. In addition, the DC-LIC with symmetric electrodes achieved a maximum energy density of 232.6 Wh kg⁻¹ and an extremely high power density of 45.2 kW kg⁻¹. The authors deemed that the excellent electrochemical properties could be explained by the 3D ion/electron channel model. CNT intercalation into graphene sheets inhibited the restacking of graphene, expanded the layer space, and improved the electrode conductivity, forming a well in-plane and cross-plane channels for both the ion and electron migration. This model is supported by the Nyquist plot and Bode plot. MRPG/CNT//MRPG/CNT LIC has a small equivalent series resistance of 18.0 Ω, which is beneficial for high rate of output and long-term cycling. Furthermore, the characteristic relaxation time constant τ was calculated to be 1.21 s, indicating the fast reaction kinetics and high-power capability of the full cell.

Overall, graphene/CNT-based cathodes have advantages in achieving high capacity and outstanding rate performance. However, nanosized carbons usually have relatively lower density (~0.3 g cm⁻³) than commercial AC (~0.5 g cm⁻³) because of their low tapping density, resulting in actually the same or even lower volumetric energy density than commercial ACs ^[96]. To overcome this dilemma, practical graphene technologies, such as the capillary drying process and rapid drying process, provide a promising solution to fabricate high tap density graphene-based composites ^[97]^[98]^[99].

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