Graphene-Carbon Nanotube Hybrids: Synthesis and Application

Journal of Environmental Treatment Techniques

2021, Volume 9, Issue 1, Pages: 224-232

J. Environ. Treat. Tech.

ISSN: 2309-1185

Journal web link: http://www.jett.dormaj.com

https://doi.org/10.47277/JETT/9(1)232

Graphene-Carbon Nanotube Hybrids: Synthesis

and Application

Khadije Yousefi*

Department of Materials Science and Engineering, School of Engineering, Shiraz University, 71348-51154 Shiraz, Iran

Received: 06/08/2020

Accepted: 08/11/2020

Published: 20/03/2021

Abstract

Graphene and CNTs have gained considerable concern and research attention. In addition to preventing the aggregation of these

carbon compounds, graphene CNT hybridization would also make full use of the synergistic relationship between graphene and CNT.

This chapter discusses the different carbon nanomaterials and their special properties, and a thorough analysis of the graphene-CNT

derivatives is observed. It would also discuss in detail the methods and their properties used to create graphene-CNT hybrids. Their

applications are also described particularly in device sensing, energy/supercapacitors, and material science.

Keywords: Carbon nanotubes, graphene, CNT-graphene hybrid

are highly satisfactory(10). Theoretical and experimental

Introduction

studies on individual SWCNT show significantly strong tensile

strength (150–180 GPa) and tensile modulus (640 GPa–1

TPA), more powerful than popular carbon fibers (11). Also,

they display off enormous thermal and electric properties a

number of the great mechanical properties associated with

CNTs: thermally stable in vacuum up to 2800°C, thermal

conductivity two times as proper as concrete, electronic present

day output 1000 extra times than copper wires (12). CNTs may

be single-walled or multi-walled structures, figure 1 shows an

image of MWCNT nanostructure transmission electron

microscope (TEM), in which several graphical carbon layers

and a hollow core appear.

Completely carbon-based products from activated carbon,

carbon nanotubes (CNTs) to graphene have gained widespread

prominence due to their intricate nanostructures, physical and

chemical characteristics of high quality. Such features involve

a range of materials (powders, fabrics, aerogels, composites,

boards, monoliths, columns, etc.), extremely inert

electrochemistry, fast storage, and porosity regulation (1-3).

Graphene and CNTs generated tremendous attention and

involvement in science due to their remarkable physical

residences, such as extreme electrical conductivity, equal

thermal stability, and excellent mechanical efficiency (4).

Conversely, due to the powerful vanderWaals forces among

them, the agglomeration of carbon materials, especially

graphene and CNTs, is unavoidable. Graphene CNT

hybridization often does not help to inhibit the association of

such carbon compounds, but may also show synergistic results

between graphene and CNT(5, 6). Research has shown that

hybrid graphene-CNT nanomaterials have more electrical

conductivity, superior surface structure, and improved catalytic

properties relative to standard CNT or graphene (6, 7). The

hybrid system is efficient and can be assembled using a range

of techniques like simple solution assembly, chemical vapor

deposition, and CNT discharge (8, 9). This chapter

demonstrates and discusses methods for hybridizing CNTs

with graphene, characterization, and hybrid alertness.

3 Graphene Nanosheets

Graphene is a 2D single-atom-thick film of carbon atoms

assembled hexagonally(13, 14). The carbon bonds are sp

hybridized where the in-plane σC–C bond is one of the most

strong links to the substance and the out-of-plane relation is

responsible for the conduction of graphene electron

contributing to a delocalized electron network. Graphene has

shown remarkable physical properties due to the specific

structural qualities which have provided substantial attention to

research in both science and technology communities (15-18).

Graphene has been used as a building block for many of such

carbon allotropes in extraordinary lengths, as visible in

Figure.2 (19). For example, with a spacing of 0.33–0.34 nm,

D graphite is composed of graph nanosheets layered at each

Carbon Nanotubes

other's pinnacle. One-dimensional (1D) carbon allotropes,

CNTs which include SWCNTs and MWCNTs can be produced

in miles by rolling the graphene into single or multi-walled

tubular nanostructures. Wrapping a piece of graphene like a

ball often has effects in zero-dimensional (0D) fullerenes.

Carbon nanotubes are visible cylinders with one or two

additional graphene layers open or near ends (de-called

SWCNT, or MWCNT). The diameters of SWCNT and

MWCNT are usually 0.8–2 nm and 5–20 nm respectively,

whereas the diameters of MWCNT maybe 100 nm,

respectively. CNTs have low mass density, immoderate

durability, and high issue ratio (usually about 300–1000),

leading in mechanical, thermal, and electrical properties that

Corresponding author: Khadije Yousefi, Department of Materials Science and Engineering, School of Engineering, Shiraz

University, 71348-51154 Shiraz, Iran. E-mail: khadije.yousefi@gmail.com

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2021, Volume 9, Issue 1, Pages: 224-232

sheet and CNTs, where CNTs connect graphene sheets during

chemical vapor deposition via the catalyst particles (CVD). The

method of hybrid wrapping focuses on the contact between

graphene sheets and CNTs, as well as the number of CNTs

wrapped in graphene nanosheets. Graphene oxide (GO) or

functional graphene hybridization with CNTs is usually

achieved using different methods. The assembly process

practically blends graphene and CNT, while the approach in

situ consists of scraping CNTs from graphene sheets into CNT

GNR or CNT types. 4.1 Assembly Method

Because of their aromatic sp nanostructure, graphene and

Fig. 1: TEM micrograph demonstrating the layered structure of a

carbon nanotube with multiwalls (12)

CNTs are co-assembled for the assembly of hierarchical

structures by van der Waals, or similarities with π–π.

Considerably oxygenated mechanical moving surface groups

or mechanical CNT Groups(20). Graphene is used for

electrostatic or covalent assemblies; GNS graphene

nanosheets; graphene oxide reduced by rGO; Acid-dealing

with A-MWCNT MWCNT; PPD p-Phenylenediamine; SDBS

Sodium dodecylbenzene sulfonate. As illustrated in the

figure.4e, GO sheets with several conjugated clusters were

likely to interact with MWCNTs when the weight ratio of

MWCNT to GO sheets was 2:1, creating exfoliated GO sheets

with MWCNT coatings (Fig. 4f). Widespread MWCNT

agglomeration – GO complexes have been identified as

immoderate MWCNTs and twisted constant tubular CNTs on

moving sheets reducing the solubility of MWCNT – transfer

complexes. Because the load ratio of MWCNTs to sheets is 1:2

(

Fig. 4 g), the single GO sheet will always communicate with

loads of MWCNTs at first. Clear suspensions of MWCNT –

motion complexes were developed after the dynamic

equilibrium phase due to the long-term sonication (the inset

image in Fig 4 g). A small number of hair-like MWCNTs are

naturally fixed at the surface of GO sheets (Fig. 4h), raising the

hydrophilic MWCNT – GO complexes (21).

Fig. 2: Graphene, the building block of all graphic types, can be

covered in 0D buckyballs, formed in 1D nanotubes, and packed in 3D

graphite (19)

Liu et al.(22, 23) stated that the hybrid graphene oxide

nanoribbon/carbon nanotube (GONR / CNT) (Fig. 2.17a) has

become an easy method for unzipping. The left MWCNTs will

link to equipped-made GNRs to form interconnected 3-D

carbon networks with partially unwrapped MWCNTs. After

being chemically modified using hydrazine hydrate (65 S

cm−1), GNR / CNT hybrids can be produced with an advanced

conductivity of 120 S cm−1 compared to that of CNTs(22). As

seen in Fig. 5c similar weight ratios of GONRs in GONR / CNT

mixtures may be conveniently prepared and measured using

XRD styles where the GONR peak (2 = 11.28 °) is reduced

because the CNT peak (2 = 26.18 °) reduced.

Strategies for the Hybridization of CNTs with

Graphene

CNT and 2D graphene hybridization create

nanostructured hybrids with different topological architectures

10). Therefore, the CNT and graphene derivatives are

(

classified into three groups compatible with their different

nanostructures: As seen in Fig.3, CNTs are horizontally

adsorbed to the base of the graphene, CNTs adsorbed by the

graphene floor and CNT covered in particular graphene.

Graphene acted as a non-stop layer matrix for CNTs

horizontally adsorbed to graphene surfaces to retain the

graphene-CNT hybrids, the most common type. For CNTs

perpendicularly adsorbed to the graphene surface, this process

can be due to a single point of contact between the graphene

Fig. 3: Three types of the hybrids of graphene and CNTs (9)

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2021, Volume 9, Issue 1, Pages: 224-232

The significance of their function peaks and can deliver as-

organized GONR / CNT derivatives to the GONR weight ratios

as 16, 55 and 85 percent respectively can be derived from a

relationship curve. They were described for simplicity as

GONR16 in step with cent / CNT, GONR55 in keeping with

cent / CNT, and GONR85 in keeping with cent / CNT. The

GNR / CNT combination TEM and SEM stats (Fig. 6) with

different GNR weight ratios indicate that within the hybrids

GNRs are aligned with CNTs and independent GNRs are

simply proved as the unzipping diploma decreases.

we'll describe the applications of this amazing CNT-graphene

hybrid tool.

5.1 Sensors

The developing variety of diabetic sufferers round the

sector has sparked interest in medical biosensing, and in that

regard, the supremacy of glucose biosensors. The biosensor

detects enzymes usually through amperometry, although the

latest instances of non-enzymatic detection of glucose have

been recorded. For instance, GO electrode (27, 28) and Pt

nanoflowers covered on the in situ CNT-graphene hybrid (29)

have been utilized in non-enzymatic blood glucose sensing. For

non-enzymatic blood glucose sensing hybrid CNT-graphene

(

29) was observed. As described, the enzymatic glucose

biosensors use glucose oxidase (GOx) due to its balance and

specificity to glucose. The chemistry for this technique may be

contained under literature(30). The enzyme Flavin adenine

nucleotide (FAD) is at the energetic center of the redox

reaction(30). Due to enzymatic action, the electrode-generated

has been transformed into electrochemically detected,

starting with designed glucose biosensors, although the

production of H is based on oxygen, requiring excessive

2 2

detection potential which interferes with other redox

composites. In second-generation biosensors, but, oxygen

dependency is eliminated way to redox mediators. Such

mediators are in continuous movement and can be connected to

an enzyme that movements electrons to the electrode or diffuse

without FAD impediments or spherical the other manner,

ensuing in amperometric signal manufacturing. Glucose

biosensing in third-generation biosensors can be achieved at a

lower capability without the want for redox mediators via direct

electron transfer (DET) from the redox core to the electro.

Table 1 summarizes the efficiency of various recorded

graphene hybrids in totally glucose-based biosensing DET.

Direct electron transfer with bare electrodes of GOx

enzyme is difficult to accomplish because FAD is deeply

embedded inside the structure. For robust electron transfer

kinetics and enzyme immobilization to mediator-loose DET for

GOx, CNT-graphene hybridized shape provides a distinctly

conducive and methodical matrix with superb effects on

glucose sensing. While the exact role of DET remains unclear,

the advanced electrochemical properties of the extremely

conductive graphene and CNT-graphene hybrid contiguous

graphene provide treasured guidelines. The lifestyles of FAD

redox tops in cyclic voltammetry with average potential

approximating the usual electrode capacity of GOx are a huge

indicator of the GOx DET scheme (31). Glucose is then

measured by calculating the increase in the top contemporary

of certainly charged FAD in glucose oxidation reaction or the

decrease in the peak current of the negatively charged FAD due

to the use/decline of oxygen. Glucose evaluation the usage

of oxygen may be carried out at low capability as an

example of mediator-loose sensing and hence extraordinary of

sensors of the third generation. CNT-graphene hybrid offers

enzyme immobilization with an extended floor position and

produces 3-d conductive matrix for efficient electron transfers

to neighboring moleculesGOx is immobilized from the redox

enzyme motion center at the CNT-graphene electrode and DET

in the course of the oxidation mechanism as shown in figure 7.

It has been shown to a great extent that CNT-graphene hybrid,

built using physical means using CNTs, achieves DET for GOx

through cathode-based oxygen-biosensing glucose (32, 33).

Fig. 4 a–d: A schematic for the formation of the GO–MWCNT hybrids.

TEM images of GO– MWCNT hybrids by adjusting the initial weight

ratio of MWCNTs to GO sheets with 2:1 e, f and 1:2 g, h at low and

high magniﬁcations (21)

.2 In Situ Method

The results of assembly methods are usually less specific

and this slowly influences the conductivity and surface region,

since this approach is less complex than in situ development.

Hybrid growth in situ graphene-CNT is more complex in

evaluation, but it maintains an extra impact on product content

and sensitivity to form the density, and hybrid shape. The

development of the graphene structures CNT-pillared go and

CNT-pillared was established (Fig. 5) (24). The cross-sectional

images are taken from the sample display nanostructures of

layers of CNTs as nanopillars among the move and graphene

surfaces. extended CNTs may be produced using growing the

quantity of the Ni catalyst while shorter CNTs may be obtained

by way of elevating the growth duration for CVDs. CNT-

pillared rGO composite substances display exceptionally

strong visible light photocatalytic efficiency in decaying dye

Rhodamine B, owing to the exceptional porous nature and

impressive electron transfer properties of graphene.

Application of Graphene-Carbon Nanotube

Hybrids

Carbon nanotube-graphene hybrid possesses the

outstanding capacity for a number uses (25, 26). In this chapter,

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2021, Volume 9, Issue 1, Pages: 224-232

Fig 5: Experimental methods pillar the go and graphene platelets using MWCNTs. B-GOCNT-30-17, c GOCNT-15-17, d GOCNT-30-9 and e GOCNT-

5-9, f RGOCNT-15-4 and g, respectively, RGOCNT-15-0.6. The final samples are named, respectively, for the CNT-pillared go and RGO composites

as GOCNT-X-Y or RGOCNT-X-Y. X illustrates here the CVD period (15 or 30 min) if Y refers to the catalyst of Ni / C mass loading (24)

Also, the electrochemically lively space for CNT-graphene

hybrid altered with ZnO nanoparticles has been multiplied,

increasing the possibility of stepped-up enzyme immobilization

and rapid electron switching (34). This technique employs

differential pulse voltammetry to come across glucose

taking benefit of oxygen depletion inside the system.

transfers photogenerated electrons from the semiconductor to

the outer circuit. Graphene converted into transferred in SSC to

both photoanode and counter electrode, serving excellent

positions. This can also be used as a clear conductive film in

the photoanode. As a conductive film, it can improve widely

used metal oxides, such as FTO and ITO, as it overcomes the

disadvantages of steel oxides, such because size, robustness,

chemical, and mechanical power and improved near-infrared

transmission (28, 36). It can also act as an additive to the

semiconductor surface for electrical bridging. Secondly,

graphene quantum dots can be used as the sensitizer has semi-

conductor residences such that photons excite electrons from

the HOMO to his LUMO. Ultimately, graphene will be part of

the counter-electrode, improve electron transport, and enhance

the redox attraction. Table 2 summarizes the average

performance, recorded in literature, of different types of SSCs

based on graphene derivatives.

.2 Sensitized Solar Cells

After Grätzel 's institution published nanostructured TiO

films on anode electrodes in 1991 (35), sensitized solar cells

SSCs) attracted considerable interest in the photoelectric

(

conversion of solar energy due to their fantastically low value

and incredible efficiency. SSCs are photoelectrochemical

structures with an electrolyte, a counter electrode, and a

photoanode; The photoanode is typically a semiconductor,

often ZnO and TiO , sensitized to photoactive materials such

as colorants (DSSC), biomolecules (BSSC), and quantum dots

QSSC), mounted on a transparent conductive surface which

(

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2021, Volume 9, Issue 1, Pages: 224-232

Fig. 6: A GNR / CNT mixed production flow model. B XRD clean CNT architectures, GONR / CNT mixture with separate weight ratios and GONR

simple architecture. C GONR weight ratio estimates in combinations GONR / CNT are based on GONR weight percentage and power ratio of

characteristic peaks in their XRD shape (22)

Table 1: Summary of performances of graphene hybrids in DET based glucose biosensors

Detection

range(mM)

Sensitivity(µAmM−1cm−2

)

LOD

(µM)

Type of Hybrid Electrode

GOx/electrochemically

Ks (s−1)

Refer

reduced G-

MWCNT/GCE with

FMCA

3.02

0.01–6.5

7.95

4.7

(37)

Graphene-CNT

GOx/chemically

Not

reported

Up to 8

1.27

0.266

79.71

(38)

(32)

(39)

reduced G-CNT/GCE

GOx/MWCNT/GO

GOx-AuNP-chitosan-

graphene nanosheets

GOx/PAMAM

dendrimer/AgNP/RGO

GOx/AuNP/bilayer

graphene

reported

11.22

Not

0.1–19.82

.0021–0.0057

0.032–1.89

.1–10

0.7

4.5

reported

Graphene–metal

nanoparticle

8.59

75.72

(40)

(41)

7.74 ±

0.16

For Human serum:64 µA

mM−

Not

reported

GOx/CdS anoparticles

0.05–11

2–16

(39)

(42)

Graphene–SNMs GOx/CdS nanocrystals 5.9

1.76

700

.03 ±

.14

GOx/PLL/RGO/ZrO2

0.29–14

11.65 ± 0.17

130 ± 21 (23)

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2021, Volume 9, Issue 1, Pages: 224-232

Fig. 7: Schematic description of electron transfer from the redox core of the GOx molecule on CNT-graphene and glucose biosensing

Table 2: Graphene hybrids are used in photochemical/optical sensors

Electrode with

graphene/SNM hybrid

V (V)

FF (%)

n (%)

References

Jsc(mA/cm )

CE: rGO-CNT/FTO

15.25

14.24

11.27

14.0

0.68

51.05

62.4

5.29

6.05

(43)

(44)

(45)

(46)

(47)

(48)

(49)

(50)

CE: VACNT-graphene paper

PA: MWCNT-rGO-TiO2/FTO

CE: TiN-rGO-CNT/FTO

CE: CuInS2-rGO/FTO

PA: Graphene QD/TiO2/FTO

PA: N3/TiO2-rGO/

0.78

0.642

0.74

0.48

0.69

0.78

61.3

6.11

4.13

6.18

6.97

6.17

16.63

0.2

16.29

12.86

CE: CNT-rGO/graphite paper

.2.1 Graphene-CNT hybrids in SSCs

Graphene-CNT hybrid compounds have been evaluated for

quick charging and discharge rates, long cycle life, and

inadequate energy densities for batteries and fuel cells.

use in SSC mainly as a counter-electrode, but also as part of the

electrolyte and photoanode (51). RGO-CNT was integrated

into the counter electrode and noticed that CNT flake gaps and

increased electrical conductivity were bridged. The hybrid's

strong catalytic and electrical properties enabled the acquisition

of portable output, which was barely reduced but comparable

to the usage of a Pt counter electrode, taking into account the

cost benefits and mechanical versatility of carbon

nanomaterials. By partially unzipping MWCNT, Zhibin et.al

(

52) recorded better graphene nanoribbons- CNT hybrid

performance compared to Pt, which resulted in CNT being

bridged with very wide floor location. Another hybrid built

with VACNT was developed on Li et .al(44) converted

graphene paper. In advanced SSC counter-electrode allowing

cellular production to hit 83% of that with a Pt film electrode

and better-tangled CNT efficiency due to shorter transport

routes. Ming-Yu et al. (45) documented the benefits of

MWCNT and graphene mixing in photoanode, where MWCNT

adsorption confirmed a decrease in the recombination and

deposition of graphene sheets and improved the degree of

adsorption of dye. Although the combination of graphene and

CNT with ionic beverages in a quasi-solid electrolyte.

Kingdom has shown that Ahmad et al. (53) has significantly

increased the energy conversion performance of cell phones

from 0.16 to 2.5 percent because carbon nanomaterials serve as

charging transporters in ionic liquids and as catalysts for

Fig. 8: Assessment of different carbon products as electrodes for the

supercapacitor. (a) an Activated carbon. Activated carbon has a very

large surface area. Nevertheless, Electrolyte ions can not reach many

of the micropores. (b) CNT bundles. Usually, CNTs form bundles

which limit their surface area. Electrolyte ions may only reach the

outermost surface. (c) Pristine graphene. During the drying cycle,

graphene nanosheets are likely to agglomerate through van der Waals

interactions. Electrolyte ions would have trouble accessing ultrasmall

pores, especially for larger ions such as an organic electrolyte or at a

high charge rate. (d) Graphene-CNT composite. CNTs can serve as a

spacer between the nanosheets of graphene to provide the electrolyte

ions with rapid diffusion pathways. Electrical conduction may be

improved for the electrons. The CNTs often act as a binder to tie the

nanosheets intact to avoid the disintegration of the graphene structure

of graphene in electrolyte (4, 54).

3−

electrochemical I reduction.

.3 Supercapacitors

The supercapacitors have considerably higher power

densities than traditional dielectric condensers and demonstrate

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Fig. 9: Supercapacitor architecture basing mainly on the 3-d G / CNT combination. BG / CNT supercapacitor output hybrid, with weight ratios of one-

of-a-kind. C strong special graphene capacitance of various G to CNT ratios in hybrid materials. D Schematic diagram of 3-Component hybrid device

configuration with CNT load spacer (55)

Owing to their extraordinary physical and chemical

properties, carbon-based materials such as activated carbon,

CNTs, and graphene were commonly used in supercapacitors

with double-layer electrochemical. Different carbon products

as electrodes for the supercapacitor have shown in figure 8. By

bridging the graphene sheets and decorating a typical

capacitive performance, the CNTs will significantly reduce the

electrode's electrical resistance to the interlayer. Also, the

CNTs can serve as a graphene interlayer spacer to hold away

from restacking relative to each individual, allowing available

electrolyte ions. The electrolyte ions can readily penetrate the

inner portion of the electrodes with the spacer device, and thus

greater electrochemically active products can be used (Fig. 8d).

However, CNTs may also be used as binders to connect the

graphene sheets and to facilitate the adhesion of electrodes to

the modern collector (54). The graphene-CNT hybrid-based

materials are also particularly suitable for processing electrode

items in EDLCs. Chen et al developed and synthesized a

hierarchical graphene(G) 3D structure using CNTs due to a

transparent and green hydrothermal route between the graphene

sheets. The materials of the 3D hierarchical structure were then

used for the production of supercapacitor devices as active

electrode materials (Fig. 9a), and high potential strength of 318

F g−1 was converted into graphene-weight materials with an

energy density of 11.1 W h kg−1. The influence of graphene on

supercapacitor performance to weight ratio CNT has been

studied closely (Fig. 9b, c). First, the maximum overall

graphene output is derived from the 1:1 ratio of the G / CNT

mixture, providing an unacceptable 318 F g−1 power, which is

64 percent of the theoretical value of the graphene. Indeed, the

green mechanical power of graphene declines and then rises

with the strain ratio of G to CNTs. The schematic image in Fig.

9d shows that the restacking of graphene will deteriorate as the

ratio of G to CNTs decreases. It may have a horrible influence

on the graphene fabric's effective surface area, thus reducing

graphene's effective contribution to the overall capacitance of

the entire electrode traveling fabric (G / CNT hybrid).

5.4 material science

Recently, Ahmad et al.(56) report exciting applications of

CNT-graphene reinforced ceramics in biomedical, aerospace,

automotive, and photonic technologies as a result of more

suitable longevity and multiple beneficial residences for hybrid

2 3

starting fabrics. In addition to the Al O improved output, the

considerably better resistance strength of the hybrids may be

desirable for a variety of automotive sliding and wearing

applications, such as piston rings, cylinder liners, and valve

seats(18, 57, 58). Additionally, the SiC, BaTiO3, and Si3N4

impregnated CNT systems were found to depend on properties

appropriate for structural use. The chemical and thermally

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stable ceramic hybrids will modify their extreme thermal

conductivity, making them appealing for high-temperature

applications(59). CNTs / graphene mixture is capable of

turning ceramics into usable substances for automotive and

aerospace applications. However, CNT-graphene hybrid out-

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Conclusion

The hybrid system is complex and can be designed by many

methods including simple solution assembly and process of

chemical vapor deposition. The chapter outlines and explores

methods for the hybridization of CNTs with graphene and

hybrid characterization. This also introduces potential

implementations of CNT-graphene hybrid architectures. CNT-

graphene has demonstrated superior efficiency in most cases

than individual pristine CNTs or graphene, indicating their

ability for numerous functional and research applications.

Whether as an electrode in mediator-free glucose biosensors,

capacitor collector device, electron transfer help, or photoactive

material, the usage and work understanding of CNT-graphene

hybrid has gradually grown and impacted modern-day carbon-

based electronics.

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