Sensors International 1 (2020) 100035

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Sensors International
journal homepage: www.keaipublishing.com/en/journals/sensors-international

Novel materials for electrochemical sensing platforms

Achi Fethi
Laboratory of Valorization and Promotion of Saharan Resources (VPRS), Kasdi Merbah University, Ouargla, 30000, Algeria

A R T I C L E I N F O A B S T R A C T

Keywords: Electrochemical sensors are a useful tool for healthcare monitoring in real time. The continuous progress in
Sensor nanomaterial synthesis leads to further improvement on catalytic properties of sensing platforms. Tremendous
MXene recent efforts have been made in design of novel sensing platforms with two-and three-dimensional nano-
2D materials
composites using variety of materials like MXene, graphitic boron nitride (h-BN), metal-organic frameworks
MOFs
TMD
(MOFs) and transition metal dichalcogenides (TMD). The functionalization of nanomaterials provides even more
Electrochemical high analytical performance of sensors which extends their application in environmental monitoring. The paper
3D-printed electrodes highlights the recent progress in designing micro-tools with variety of shapes and flexible structures for
biomedical and healthcare applications and recent advancements in functionalizing 2D and 3D nanomaterials for
electrochemical sensing applications are discussed. The discussion was extended to cover the main challenges in
printing strategies to get wearable and flexible sensors with the emphasis on innovative methods and fast
experimental protocols, highlighting even more the effect of electroanalytical parameters on the performance of
sensors.

uniform distribution of nanomaterials at solid interfaces with sizing

control [12]. However, chemical compatibility between solvent, surfac-
1. Introduction
tants and precursors should be intensely analyzed [13]. On the other
hand, hydrothermal process is favorable for crystallizing materials
Monitoring of chemical compounds by micro-analytical tools be-
directly from aqueous solution, in which by optimizing working tem-
comes nowadays a helpful choice when real-time sensing of compounds
perature range and reaction time, it becomes easier to design a specific
is required on-site. Sensors are devices offering this opportunity and
structure [14–19].
several daily-used tools are successfully commercialized [1]. However,
These strategies make widespread application of 2D nanomaterials
their performance highly depends on the catalytic conducting interfaces
for sensors in healthcare areas and cancer diagnosis [20,21]. Accord-
for the selective interaction with the target of interest [2,3]. Thus,
ingly, different kinds of transition metal dichalcogenides (TMD) cover
nanocomposites based on 2D nanomaterials offer highly sensitive sensors
large areas including biomedical [22], photocatalysis [23–25], capacitors
using variety of materials such as carbon materials [4], metal-oxides [5],
[26], environment, oncological and cancer therapy [27–29]. In addition,
conducting polymers [6]. Accordingly, a growing number of new
MXene as 2D catalyst is beneficial in sensing areas displaying high cat-
methods were applied to the design and synthesis of innovative nano-
alytic activity [30–33]. Besides, potential use of metal-organic frame-
materials for use in sensing applications [7,8].
works (MOFs) in preparing sensors because of its ultra-thin 2D
Recently, the use of one-step methods easily synthesis two-
nanosheets with crystalline polymer network. MOFs are designed by
dimensional (2D) sensing platforms with low-cost materials. In prac-
hydrothermal method using an appropriate ratio of inorganic salts
tice, large use of solvo- and hydrothermal methods, which are two similar
and/or metal cations with organic linkers [34,35].
methods with a bit difference in the nature of solvents. In solvothermal
Sensing platforms based on functionalized 2D nanomaterials reach
process, reactants are highly soluble in a stable solvent and crystallinity
rapid attomolar determination of chemical compounds in real samples
level increases displaying various kinds of morphologies with better
[36,37]. Furthermore, electrochemical analysis frequently exhibits
control of structures [9–11]. Moreover, solvothermal approach offers

E-mail addresses: achi.fethi@univ-ouargla.dz, achifethi@hotmail.fr.

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https://doi.org/10.1016/j.sintl.2020.100035
Received 25 June 2020; Received in revised form 22 August 2020; Accepted 22 August 2020
Available online 26 August 2020
2666-3511/© 2020 The Authors. Production and hosting by Elsevier B.V. on behalf of KeAi Communications Co., Ltd. This is an open access article under the CC BY-
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A. Fethi Sensors International 1 (2020) 100035

Abbreviation L.R. linear range

LOD limit of detection
2-MeIM 2-Methylimidazole LPS Lipopolysaccharides
4-CP p-chlorophenol LSV linear sweep voltammetry
AA Ascorbic acid MP methyl parathion
AAP Ascorbic acid-2-phosphate N-DC Nitrogen-Doped Carbon
ALP Alkaline phosphatase NCL Nucleolin
Amp. amperometry NH2-BDC 2-aminoterephthalic acid
AMX amoxicillin NHS N-Hydroxysuccinimide
ATPA 2-aminoterephthalic acid PEDOT poly(3,4-ethylenedioxythiophene
BDC ¼ benzene-1,4-dicarboxylic acid POM Polyoxometalate
BPA Bisphenol A POX paraoxon
BTC 1,3,5-benzenetricarboxylic acid PSS polystyrene sulfonate
C.V. cyclic voltammetry PTA terephthalic acid
CA caffeic acid PTH Parathyroid hormone
CBZ Carbamazepine PTTBA 4,40 ,400 ,4’’’-(porphine-5,10,15,20-tetrayl)tetrakis benzoic
CBZm carbendazim acid
COF covalent-organic frameworks PVP polyvinylpyrrolidone
CPK-MB creatine kinase-MB RF Riboflavin
DMF Dimethylformamide Sens Sensitivity
DOX doxorubicin SER Serotonin
DPV Difference pulse voltammetry Stab stability
DZN diazinon T3 triiodothyronine
Ep Epinephrine T4 thyroxine
ETG ethylene glycol TBBPA tetrabromobisphenol A
ETTA 4,40 ,400 ,4000 -(ethane-1,1,2,2-tetrayl) tetraaniline TCAA Trichloroacetic acid
FZ furazolidone Tech Technique
Glc glucose TF taxifolin
GSH Glutathione TFA Trifluoroacetic acid
H2PyC 1H-pyrazole-4-carboxylic acid THF tetrahydrofuran
H2TCPP 5, 10, 15, 20-tetrakis (4-carboxyphenyl) porphyrin TNT 2, 4, 6-trinitrotoluene
H3BTC Trimesic acid TPAL terephthalaldehyde
HMT Hexamine Tyr Tyrosine
HPPF6 1-hexylpyridine hexafluorophosphate UA Uric acid
i-t intensity-time

superior electro-catalyst features of functionalized 2D materials dis-
playing novel sensitive platforms with variety of chemical properties
[38–42].
This review summarizes recent progress in novel nanomaterials
employed as catalysts nanocomposites in sensing platforms with an
evaluation of their effect on the analytical performance of electro-
chemical sensors. The emphasis is on describing the efficient strategies
for designing 2D nanomaterials with uniform interfaces and porous
structures. The last sections discuss progress made on the application of
cancer biosensors and wearable sensing tools with an emphasis on the
novel materials for flexible structure.
2. 2D sensing platforms
Recent useful methods construct 2D sensing platforms with variety of
nanomaterials such as TMD, MOFs or MXene. Also, carbon materials and
their derivatives like graphitic carbon nitrides (g-C3N4) as catalysts show
high catalytic activity (Table 1). To assess the improvements of 2D
sensing platforms, electrochemical techniques such as difference pulse
voltammetry (DPV) or electrochemical impedance spectroscopy (EIS)
visualize the efficiency of doping methods [43].
metal, A is an A-group element (specifically, elements 13–16), and X is
carbon and/or nitrogen [44]. Since the first development of MXene
sheets by Naguib et al., 2012, there has been a large use of hydrofluoric
acid (HF) as etching agent which leads to more corrosive medium [45].
Hence, in situ formation of fluorine ions is a strategy allowing MXene
delamination in low-concentrated aqueous medium [46]. More efficient
methods for MXenes synthesis such as thermal-assisted electrochemical
etching allow Ti3AlC2 delamination at room temperature with non-toxic
solution [47]. Therefore, the use of beneficial solvent with green acidic
treatment creates more catalytic sites and remove undesired function
groups [48,49].
Functionalizing strategies of MXene introduce negative charge groups
to perform electrocatalytic activity for sensing interfaces [31]. This can
be done by drop-casting of Ti3C2Tx at the surface of glassy carbon elec-
trode or by mixing it with mono or bimetallic nanoparticles (Au-Pd)
[50–53]. As shown in (Table 1), mixing Ti3C2Tx with Prussian blue shows
better analytical performance compared to other carbon materials for the
detection of hydrogen peroxide [54].
2.2. Graphitic carbon nitrides (g-C3N4)

The design of three-dimensional nanosheets of graphitic carbon ni-

2.1. MXene trides (g-C3N4) requires high-temperature treatment of melamine pow-
der (500–600 C ) for a time varies between (4–6 h) [55]. Then several
MXene is a 2D material obtained from etching MAX phases with a steps are consecutively applied to get stable colloids including, ambient
chemical formula of Mnþ1AXn, (n ¼ 1, 2, 3) where M is an early transition cooling, product dispersion in deionized water, ultrasonication, and

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Table 1
Electrochemical sensing platforms based on g-C3N4, Ti3C2Tx, h-BN materials.
Material Modified electrode Tech. L.R. Sens. Stability Target LOD Ref.

g-C3N4 g-C3N4/GCE SWASV – 22.668 μA/μM – Cd 2þ

3.97 nM [61]
g-C3N4/O-MWCNTs/SPE DPV 0.35–6.5 μg/L – – Pb2þ 0.008 μg/mL [71]
g-C3N4/GCE EIS 0.0025–1 μg/mL – – Pb2þ 0.001 μg/mL [55]
S-g-C3N4/GCE DPV 0.075–2.5 μM – – Pb2þ 3 pM [65]
Pd/g-C3N4/GCE DPV 0.01–15 μg/L – – Hg2þ 9 ng/L [57]
ACCG/Nafion/GCE DPV 0.1–50 μM 4.95 μA/μM – DA 0.1 μM [62]
g-C3N4/Fe3O4-CPE DPV 14–120 μM 0.16 μA/μM 96.8% (2 weeks) Tramadol 0.1 μM [63]
g-C3N4/GO/Fc-TED/GCE DPV 0.045–213 μM – 94.7% (30 days) metolcarb 8.3 nM [59]
Mpg-C3N4/β-CD/GCE LSV 1–100 μM 0.2 μA/μM – TNT 68 ppb [72]
CuFe2O4/g-C3N4/SPCE CV 0.03–697.175 μM 2.807 μA/μM.cm2 – Xanthine 13.2 nM [58]
TB/BSA/TBA/Ag-g-C3N4/GCE EIS 100 fM – 20 nM – 84% 11 days Thrombin 38 fM [56]
CdO/PANI/mpg-C3N4/GCE DPV 0.05–80 μM 0.0393 μA/μM 94.5% (30 days) Ep 0.011 μM [73]
TiO2-g-C3N4@AuNPs/GCE EIS 0.5–3 nM – 95.5% (20 days) AMX 0.2 nM [60]
Ti3C2Tx SPE/MXene/Au Pd/GA/AChE DPV 0.1–1000 μg/L – 95% 7 days POX 1.75 ng/L [51]
Ti3C2Tx/GCE Amp 0.015–10 mM – 90% (5 weeks) DA 3 nM [74]
Ti3C2Tx/GCE DPV 50 nM–100 μM 0.024 μA/μM – CBZm 10.3 nM [50]
H–C3N4/Ti3C2Tx/GCE DPV 0.5–1.5 μM 49.91 μA/μM 90.9% (15 days) Pb2þ 0.6 nM [53]
20% Pd@Ti3C2Tx/GCE Amp 0.5–10 μM 5.71 μA/μM.cm2 – L-Cys 0.14 μM [52]
AuNPs-Ti3C2-NTO-PEDOT/GCE DPV 0.0001–20 ng/mL – 84.23% (2 weeks) PSA 0.04 pg/mL [75]
h-BN D-h-BN/GCE DPV 0.01–30 μM 0.0848 μA/μM 96.55% (4 weeks) 4-AP 0.003 μM [68]
Nafion/Mb/BN/CILE CV 0.2–30 mM 6.340 μA/mM 94.5% (2 weeks) TCAA 0.05 mM [69]
h-BCN CV 10–500 μM 0.32 μA/μM – UA 2 μM [66]
PtNPs/POM/h-BN CV 0.1–300 μM – – NHS 60 nM [76]
h-BN/HNTs Amp 0.009–173 μM 0.459 μA/μM.cm2 – FZ 0.001 μM [67]
MIP/GQDs/2D-hBN/GCE EIS 1 pM–10 nM 30.014 μA/nM – SER 0.2 pM [70]

centrifugation. The chemical synthesis of g-C3N4 with reducing agents [69]. Moreover, h-BN combination with graphene quantum dots by
such as AgNO3 or NaBH4 provides a variety of nanohybrid electro- molecularly imprinted polymer enables trace level detection of serotonin
catalysts for sensing substrates like xanthine in biological fluids as potential neurotransmitters in human body (LOD ¼ 0.2 pM) [70].
(LOD ¼ 13.2 nM) or heavy metals [56–58] (Table 1).
Generally, there have been three consecutive processes to function- 2.4. Metal–organic frameworks (MOFs)
alize graphitic carbon nitride including (i) thermal condensation of
melamine or polymerization of urea, (ii) self-assembly, and (iii) elec- Metal organic frameworks (MOFs) are ultra-thin 2D nanosheets with
trodeposition [59,60]. Importantly, exfoliation and protonation with HCl large meso-macroporous structures [34,35]. The use of functional coor-
solution forms ultrathin g-C3N4 sensing interface for heavy metals [61]. dination polymers for MOFs synthesis uniformly disperse the transition
The combination of g-C3N4 with metal oxides gets bi-functional hybrid metal compounds on the surface of organic materials (Fig. 1 A, B) [77].
catalysts with high redox peak current using K3Fe(CN)6 solution medium MOFs sensing platforms are ultrathin and porous with controllable cavity
and also increases the effective surface area [62,63]. size and large surface areas. However, morphology of MOFs nano-
Investigation of interactions, morphology and charge distributions of composites is highly dependent on the growing time and pyrolysis
functionalized g-C3N4 is of crucial importance before experimental syn-
thesis and can be carried out using numerical tools such as Gaussian [64].
For instance, Zou et al., 2019 have calculated the difference of molecular
orbital energies between heavy metal ions and sulfur-doped graphitic
(S-g-C3N4) composite to demonstrate its selectivity towards lead ions
(Pbþ2) [65]. Another investigating method consists of using 3D response
surface diagram for the analysis of the interaction between g-C3N4
structure and different other parameters including even the effect of
biorecognition elements [60].
Graphitic carbon nitrides (g-C3N4) has a crystalline nanostructure
with high photocatalytic performance and large surface area. The elec-
trocatalyst properties of g-C3N4 depends on the nitrogen content which is
tunable by changing the volume ratio. The nitrogen doping improves
conductivity of g-C3N4 materials. Moreover, the use of ionic liquids are
promising precursors for constructing flexible nanostructure.

2.3. Hexagonal boron nitride (h-BN)

Hexagonal boron nitride (h-BN) has a similar structure of graphene

with high catalyst properties, especially with the presence of halloysite-
nanotube (HNTs) [66,67]. The use of melamine as precursor for h-BN
calcination gets defect structure which creates more catalytic sites
providing fast electron transfer [68]. A new method promoting fast Fig. 1. SEM images of MOF-818 (A) and MOF-818@rGo/MWCNTs (B).
electron transfer (ks ¼ 2.197 s1) consists of using ionic liquid-carbon Reproduced with permission from Refs. [77]. Ultrathin nanosheet Ni-MOF as-
paste electrode to immobilize h-BN with myoglobin (Mb) and nafion semblies (C, D). Reproduced with permission from Ref. [102].

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Table 2
Electrochemical sensing platforms based on MOF nanosheets.
Material Organic Growth T-time Morphology Aqueous medium Surface area Tech. Target Analytical performance Ref.
ligand (m2/g)

CuxCo3-xO4 urea 120  C for 8 h nano-needle DI water 22.244 EIS CV Glc L.R. ¼ Up to 1.4 [100]
Amp LOD ¼ 1.36 μM
Sens. ¼ 13291.7 μA/
mM.cm2
NiCo-MOF ATPA 120  C for 4 h Microneedles DMF & DI water – Amp Glc L.R. ¼ 1 μM–8 mM [79]
LOD ¼ 0.29 μM
Sens. ¼ 0.6844 μA/
mM.cm2
Ni3(PO4)2@ZIF-67/GCE ZIF-67 Rhombic dodecahedron DMF & DI water 354 Amp Glc L.R. ¼ 1–4 mM [111]
100  C for 5 h LOD ¼ 0.7 μM
Sens. ¼ 2783 μA/mM.cm2
Stability (%) ¼ 95% 3
weeks
ZnCo2O4/GCE PVP 160  C for 3 h microrice DMF & ethanol 25 CV Glc L.R. ¼ 0.01–0.55 mM [104]
LOD ¼ 5 μM
Sens. ¼ 436.1 μA/mM.cm2
Ni-BDC/GCE BDC 135  C for 24 h hierarchical DMF & 100 Amp.&CV Glc L.R. ¼ 0.01–0.8 mM [103]
multilayer acetonitrile & PVP LOD ¼ 6.68 μM
Sens. ¼ 636 μA/mM.cm2
Ni-MOF400 BTC uniform polyhedral DI Water & – Amp Glc L.R. ¼ 5 μM–4.1 mM [78]
room temperature ethanol LOD ¼ 0.92 μM
Sens. ¼ 2918.2 μA/
mM.cm2
BPNSs/TH/Cu-MOF/ TFA & PVP 3 h at 80  C DMF & ethanol 427.9 EIS & CV miR3123 L.R. ¼ 2 pM–2 μM [101]
GCE LOD ¼ 0.3 pM
CuTCPP/pOMC-3/GCE H2TCPP 80  C for 30 min DMF & ethanol 785.89 Amp. H3NO L.R. ¼ 5.8–733.8 μM [81]
LOD ¼ 0.8 μM
Sens. ¼ 10.18 μA/μM
COFETTA-TPAL- THF Nanospheres DMF 281.14 DPV H2O2 L.R. ¼ 1.1–500 μM [126]
Fc(COOH)2/GCE LOD ¼ 0.33 μM
Sens. ¼ 0.009 μA/μM
Stability ¼ 98.71% 5 days
Ni-MOF/GCE PTA 100  C for 4 h accordion- DMF þ NaOH – Amp N2H4 L.R. ¼ 0.5–8 mM [102]
like LOD ¼ 0.23 μM
Sens. ¼ 2412 μA/μM.cm2
MIP/pTH/Au@ZIF-67/ 2-MeIM rhombic dodecahedral Ethanol & 0.14 cm2a DPV Tyr L.R. ¼ 0.1 nM–4 μM [108]
GCE Methanol LOD ¼ 0.79 nM
BC/c-MWCNTs/ZIF- 2-MeIM Ultra-fine fiber – 240.66 CV BPA L.R. ¼ 0.01–0.4 mM [112]
8@LAC LOD ¼ 1.95 μM
Stability ¼ 80% 20 days
NiO/Fe2O3/NiCo2O4 2-MeIM 120  C for 1 h Nanocube Methanol – EIS Insulin L.R. ¼ 0.172 fM 1.72 nM [113]
shape LOD ¼ 0.16 fM
Ni-MOF/GO/GCE H3BTC regular columnar Ethanol þ DI – DPV 4-CP L.R. ¼ 0.10–300.0 μM [35]
water LOD ¼ 8 nM
Sens. ¼ 2.411 μA/μM
In2O3 NSAs/3D Gr ETG 200  C for 12 h 3D network DI water 77.5120 DPV DA L.R. ¼ 0–60 μM [127]
nanostructure LOD ¼ 0.1 μM
Sens. ¼ 2.69 μA/μM.cm2
Fe3þ@ε-MnO2 – hollow hydrangea-like – 54.01 EIS& CV DA L.R. ¼ 0.02–78 μM [128]
microspheres LOD ¼ 5 nM
Sens. ¼ 242.6 μA/mM.cm2
cs/α-MnO2/GCE – hollow urchin-like DI water 47.23 EIS & CV DA L.R. ¼ 0.05–88.8 μM [129]
microspheres LOD ¼ 12 nM
CoO–CoS/NF – sheet-like heterostructures – – Amp. H2O2 L.R. ¼ 2–954 μM [130]
LOD. ¼ 0.890 μM
Sens. ¼ 0.059 mA/μM.cm2
CoMoO4/MPC – Nanorods DI water 105 EIS & CV Glc L.R. ¼ 0.5 μM–0.108 mM [131]
LOD ¼ 0.13 μM
Cu/CuxO/NC/GCE NH2-BDC 100  C for 24 h DMF 34.09 CV & Amp Glc L.R. ¼ 0–5 mM [132]
Microflowers LOD ¼ 3.5 μM
Ni-MOF@CNTs/GCE 2-MeIM 3D heterostructures Methanol & PVP 64.5 DPV BPA L.R. ¼ 0.001 – 1 μM [133]
LOD ¼ 0.35 nM
Sens. ¼ 284.64 μA/
mM.cm2
Stability ¼ 96.0% 7 days
SnS@Co,N–C 30%/GCE 2-MeIM 3D Hierarchical Hollow DI water & PVP 0.326 cm2a DPV Ep L.R. ¼ 0.01–300 μM [134]
Microrod LOD ¼ 3.3 nM
MOF-818@RGO/ H2PyC Octahedral cubic TFA & DMF 176.30 DPV CA L.R. ¼ 0.2–7 μM and [77]
MWCNTs-3/GCE 7–50 μM
LOD ¼ 0.0052 μM
Sens. ¼ 12.89 μA/μM
Stability ¼ 95% one week

**electrochemical surface area (ECSA).

a
Electrode area (EA).

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A. Fethi
temperature [78–80] (Table 2). These physical characteristics of MOFs
allows selective determination of analytes with high sensitivity
(Sens. ¼ 10.18 μA/μM) [81].
2.5. Transition metal dichalcogenides (TMD)
As illustrated in Table 3, electrochemical sensors are now available
with variety of transition metal dichalcogenides (TMD) including,
tungsten disulfide (WS2) [82,83], nickel and titania dioxide [84], tin
oxide (SnO2) [85], antimony oxide (Sb2O3) [86], cerium oxide (CeO2)
[87], nickel(II) hydroxide Ni(OH)2 [88,89], platinum dichalcogenides
(PtS2, PtSe2, PtTe2) [90]. TMD sensing interfaces are favorable for
monitoring heavy metals due to their high electro-catalytic activity, fast
charge mobility and can easily attain the energy transition [91,92].
Siloxane nanosheets is also a wide energy band gap material with high
improvements in electrochemical oxidation of dopamine due to the hy-
droxyl groups-charged surface, for instance, charge transfer resistance
(Rct) decreases from 67.6 Ω (GCE) to 9.1 Ω (siloxene/GCE) [93].
3. Chemical synthesis of 2D nanomaterials
The synthesis of 2D nanomaterials is basically carried out by two main
methods, top-down and bottom-up strategies [94]. Designing 2D materials
by top-down approach is usually fulfilled by variety of exfoliation methods
[95], such as mechanical cleavage or ion intercalation method [96].
Whereas bottom-up strategies are based on chemical synthesis using suit-
able solvent and proper metal/organic ratio [97]. Among these methods,
chemical vapor deposition (CVD) and wet chemical synthesis (Hydro/-
Solvothermal) can produce ultrathin sensing platforms [98].
3.1. Non-toxic ligands
Chemical synthesis methods recently tend to use non-toxic ligands
avoiding the excessive need of aggressive etching agents [99]. Recent
studies are now starting to use eco-friendly acids such as ammonium
fluoride, trifluoroacetic acid (TFA) as fluorine source [100,101]
(Table 2). Ligands like TCPP considerably improve the catalytic proper-
ties of copper (II)-doped carbon nanocomposites with significant
decrease of charge transfer resistance (Rct) [81]. Hydrothermal reaction
of nickel(II) nitrate hexahydrate with p-benzenedicarboxylic acid in
presence of DMF and NaOH provides an accordion-like morphology
(Fig. 1 C, D). This ultrathin 2D MOF structure serves as sensing platform
to detect hydrazine [102].The use of polyvinylpyrrolidone (PVP) as
stabilizing agent with terephthalic acid and acetonitrile produces a
porous structure and forms with ZnCo2O4 material a conductive platform
(RCT ¼ 9.20 Ω) for monitoring glucose [103,104].
Imidazoles are potential ligands for the synthesis of 2D nanomaterials
since it can be prepared by facile methods with eco-friendly protocols
[105–107]. Zeolitic imidazolate framework (ZIF-67) is a 3D precursor
material with a rhombic dodecahedral architecture of mean size equal to
600 nm [108]. These ligands can prepare ultrathin MOF nanostructure
for sensing application by combination with acetonitrile and dime-
thylformamide (DMF) [109,110]. ZIF-67 composites are chemically sta-
ble but have a poor conductivity. Hence, applying ion exchange method
for growing ZIF-67 on the surface of Ni3(PO4)2 catalysts display an
excellent catalytic activity for glucose oxidation
(Sens. ¼ 2783 μA/mM.cm2) [111]. Similarly, ZIF-8 as encapsulation
agent can immobilize laccase on the surface of electrode and improves
the stability of bisphenol A biosensor (Stability ¼ 80% 20 days) [112].
Also, combination of ZIF with multifunctional groups design a novel
hetero-architecture material as aptamers support for detecting insulin at
ultra-low level (LOD ¼ 0.16 fM) [113].
3.2. Anti-aggregation surfactants
The use of surfactants reduce interfacial interactions and enhances
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Sensors International 1 (2020) 100035
the electrochemical activity of TMD sensing interfaces like molybdenum
disulfide (MoS2) (Table 3) [114–116]. However, the aggregation phe-
nomenon and the lack of electronic conductivity of MoS2 nanosheets
limit their performance in sensing platforms. Recent report demonstrates
that the use of riboflavin 50 -monophosphate sodium salt (FMNs) under
ultrasonication effect provides uniform dispersion of MoS2 and prevent
re-aggregation [114,117]. Other surfactants and metal intercalation
agents show the similar effect such as, thioglycolic acid (TA) [118],
N-methyl-2-pyrrolidone (NMP), sodium cholate (SC) [119,120]. Inter-
estingly, loading gold nanoparticles on exfoliated MoS2 nanosheets with
polyacrylic acid (PAA) improves considerably the sensitivity of apta-
sensor for monitoring endotoxins (LOD ¼ 29 ag/mL) [121]. Similarly,
self-assembling gold nanoparticles on the surface of MoS2 nanoflakes
using hydrazine hydrate as reducing agent provides high catalytic plat-
form for detecting uric acid in real urine sample (Sens. ¼ 4.5464 μA/μM)
[122]. Also, the use of ionic liquids and 5-sulfosalicylic acid (SSA) for
functionalizing MoS2 with carbon materials can minimize the aggrega-
tion phenomenon and reduces charge diffusion resistance [123–125].
4. 2D Morphology-performance strategies
The morphology of sensing interfaces changes continually during
chemical synthesis affecting on catalytic sites of electrochemical sensor.
Recent efforts trying to apply advanced methods for producing uniform
and porous structure as catalysts [135–138]. Growing metal oxides on
three-dimensional carbon materials by calcination is a technique
providing a large surface area. Similarly, coating conductive polymers at
2D material sensing layers promotes an efficient electronic transport of
electrochemical species [139]. Also, incorporation of
conjugated-polymers to carbon materials nanostructure avoid aggrega-
tion although some of polymers have low coating density due to their
weak interactions.
4.1. Technologies for uniform interfaces
The synthesis of 2D MOFs with ionic surfactant-assisted dispersion
method easily provides ultrathin layers with uniform interface using
chitosan and (4-carboxy-phenyl) porphyrin (TCPP) [140]. The TCPP as
catalyst precursor highly improves the electron mobility due to the
conjugated π-electron system [81,140]. The condensation reaction be-
tween ETTA and TPAL in presence of ferrocene is also a simple method
for preparing uniform nanospheres (200 nm in diameter) ordered
dispersed layer with surface area of 281.14 m2/g [126] (Fig. 2). Recent
approaches show good applicability to form controlled porous structures
such as, the use of amphiphilic copolymers or metal-organic gels as
surfactants, or furthermore, hybridization of metal oxide coated-polymer
with carbon materials [46,141,142].
4.2. Porous structure methods
The decrease of the charge-transfer resistance (Rc) of 2D nano-
composites after functionalization confirms the porous nanostructure
and thus indicates fast diffusion of electroactive species allowing high
redox conductivity. Wet chemical synthesis is an efficient strategy to
improve the porosity of electrocatalysts [143]. For instance, graphitic
carbon nitride (g-C3N4) doped with MWCNTs by chemical oxidation
method displays a three-dimensional porous structure [71]. Also, the
electrodeposition of polyaniline and cadmium oxide nanoparticles on
g-C3N4 nanosheets provides mesopores structure with sizes smaller than
15 nm [73]. To prepare mesoporous platform by facile strategy, the
conical-cylindrical cavity structure of cyclodextrins (β-CD) is compatible
with graphitic-carbon nitride [72]. Especially, with nitrogen doping and
calcination to increase the average pore diameter [134,144]. This pro-
cedure provides crystalline carbon structure with uniform charge distri-
bution due to the strong electronegativity of nitrogen element [145]. In
addition, the consecutive application of coprecipitation method and
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Table 3
Electrochemical sensing platforms based on TMD materials.
TMD material Sensing platform Tech. Target Performance Real sample Ref.
Recovery (%)

MoWS2 Mo0.75W0.25S2/GCE Amp. H2O2 L.R. ¼ 0.4–10000 μM – [115]

LOD ¼ 0.3 μM
Sens. ¼ 1290 μA/mM.cm2
MoS2 AuNPs/MoS2/rGO/GCE DPV NCL L.R. ¼ 0.5 nM–1.0 μM human serum (98.3%–104.9%) [123]
LOD ¼ 0.16 nM
MoS2 SSA/MoS2/o-MWCNTs/GCE DPV Cu2þ L.R. ¼ 0.1–11 μM Milk (105 %–112.67%) [124]
LOD ¼ 0.057 μM
MoS2 FMNs/MoS2/GCE DPV DNA L.R. ¼ 0.1 fM – 0.1 nM serum (97.0%–101.5%) [117]
LOD ¼ 0.12 aM
MoS2 LBA/Au/MoS2-PAA/GCE DPV LPS L.R. ¼ 100 ag 100 pg/mL clinical insulin (98.2%–101.25%) [121]
LOD ¼ 29 ag/mL
MoS2 Co@MoS2/rGO/SPE CV Glc L.R. ¼ 0–1.2 mM – [125]
LOD ¼ 30 nM
Sens. ¼ 0.945 μA/mM
MoS2 MoS2-AuBSPE CV Tyr L.R. ¼ 0–200 μM Food integrator (98.2 %–104.4%) [119]
LOD ¼ 0.5 μM
Sens. ¼ 1580 μA/mM.cm2
MoS2 MoS2/rGO-GCE CV Pb2þ LOD ¼ 0.005 μM Tap water (99.10%–101.80%) [114]
Sens. ¼ 50.80 μA/μM
MoS2 CuO/MoS2 CV Amp Glc L.R. ¼ 0.1–1 mM – [118]
LOD ¼ 0.017 μM
Sens. ¼ 1055 μA/mM.cm2
Stab. ¼ 85% 30 days
MoS2 MoS2/ANC/GCE CV TF L.R. ¼ 1 nM–1 μM Fructus polygoni orientalis (98.9%100.5%) [144]
LOD ¼ 0.3 nM
Stab. ¼ 94.6% (1week)
MoS2 Au–MoS2/GCE CV UA L.R. ¼ 0.033–10.0 μM Urine (92.0 %–105.6%) [122]
LOD ¼ 0.0182 μM
Sens. ¼ 4.5464 μA/μM
Stab. ¼ 90.7% 4 weeks
MoS2 MoS2/CuS–Au/GCE Amp CEA L.R. ¼ 50 fg/mL–100 ng/mL Human serum (96.9%–104.3%) [151]
LOD ¼ 16.7 fg/mL
MoS2 AuNRDs/1T-MoS2/SPE DPV DOX L.R. ¼ 0.01–9.50 μM Human blood serum (99.2%–100.8%) [120]
LOD ¼ 2.5 nM
Sens. ¼ 7.13 μA/μM.cm2
WS2 BN-IL-WS2/GCE DPV 4-AP L.R. ¼ 0.01–50 μМ Seawater (101.4%) [83]
LOD ¼ 3 nM
WS2 WS2/GCE DPV UA L.R. ¼ 5 μM–1 mM Blood serum (96%–106.7%) [82]
LOD ¼ 1.2 μM
Sens. ¼ 312 nA/μM.cm2
TiO2 Ni/TiO2 SCNWA Amp. Glc L.R. ¼ 0.2–2 mM Human serum (100.3%–111.5%) [84]
LOD ¼ 10 μM
Sens. ¼ 1472 μA/μM.cm2
SnS2 SnS2/GR-β-CD/GCE DPV DA L.R. ¼ 0.01–150.76 μM Human serum (99.3%) [91]
LOD ¼ 4 nM
Sens. ¼ 2.49 μA/μM.cm2
VS2QDs VS2QDs-GNP/CMWCNTs/DZBA/BSA EIS DZN L.R. ¼ 10 fM – 10 nM River water (107%) [43]
LOD ¼ 2 fM
Bi2O3 SnS–Bi2O3/GCE SWASV Cd L.R. ¼ 0.10–1.00 μM Tap water (97%) [92]
(II) LOD ¼ 1.50 nM
Sens. ¼ 131.5 μA/μM
SnO2 SnO2 nws DPV RF L.R. ¼ 0–13 μM Pharmaceutical sample (98%) [85]
LOD ¼ 0.6 μM
Sens. ¼ 0.035 mA/μM
Si6H3(OH)3 Siloxene/GCE DPV DA L.R. ¼ 10–1100 μM – [93]
LOD ¼ 0.327 μM
Sens. ¼ 0.0728 μA/μM.cm2
Sb2O3 Sb2O3/MWCNTs CV Cd2þ L.R. ¼ 80–150 ppb [86]
LOD ¼ 16.77 ppb –
Sens. ¼ 1.932 μA L/μg
CuO CuO-NPs/GCE CV Glc L.R. ¼ 5–600 μM Serum (96–107%) [141]
LOD ¼ 0.59 μM
Sens. ¼ 1098.37 μA/mM.cm2
CuO Ag–CuO Amp. Glc L.R. ¼ 5 μM–30 mM Urine (105.4%) [147]
LOD ¼ 5 μM
Sens. ¼ 150.17 μA/mM.cm2
CoS2 CoS2@C-HRP Amp. CEA L.R. ¼ 0.001–80 ng/mL Serum (94.7%–105.6%) [152]
LOD ¼ 0.33 pg/mL
Co3O4 Co3O4/N-DC/GCE Amp. N2H4 L.R. ¼ 0.50–977.40 μM River wate (94.80%–101.1%) [146]
LOD ¼ 0.11 μM
Sens. ¼ 56.63 mA/mM
(continued on next page)

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Table 3 (continued )
TMD material Sensing platform Tech. Target Performance Real sample Ref.
Recovery (%)

Co3(PO4)2 net-Co3(PO4)2/NG/GCE Amp. Glc L.R. ¼ 0.005–0.1 mM serum (94% 103%) [145]
LOD ¼ 1 μM
Sens. ¼ 2307 μA/mM.cm2
Stab. ¼ 95% 3 weeks
NiO CFL-Hoþ
3 /NiO NSs DPV & CV CBZ L.R. ¼ 0.001–310.0 μM Urine (101.6%) [153]
LOD ¼ 4.5 nM
CeO2 CeO2/GNP/GCE DPV TBBPA L.R. ¼ 0.005–1 μM Lake water (98.7%–101.2%) [87]
LOD ¼ 1.8 nM
NiCo2O4 NiCo2O4RMNs@PEDOT/rGO Amp. H2O2 L.R. ¼ 0.388–140 mM H2O2 disinfectant (103.3%) [142]
LOD ¼ 0.031 μM
Sens. ¼ 678.93 μA/mM.cm2
Stab. ¼ 85.4% 81 days
Ni–Co Ni–Co Phosphate CV & Amp. Glc L.R. ¼ 2–4470 μM Human serum (98.3%–101.6%) [34]
LOD ¼ 0.4 μM
Sens. ¼ 302.99 μA/mM.cm2
PtCoNi dPtCoNi@Pt-skin NP LSV CPK-MB L.R. ¼ 0.001–2500 ng/mL Human serum (99.2%–101.0%) [46]
LOD ¼ 0.62 pg/mL
Stab. ¼ 95.2% 28 days
ZnO ZnONSt@GO DPV MP L.R. ¼ 0.03–670 μM Vegetables (98%) [149]
LOD ¼ 1.2 nM
Sens. ¼ 16.5 μA/μM.cm2
PtTe2 GCE/PtTe2 Amp H2O2 L.R. ¼ 3–300 μM Human serum [90]
LOD ¼ 1.2 μM
Sens. ¼ 10.9 μA/mM
Stab. ¼ 80% 6 days
Ni(OH)2@MnO2 Ni(OH)2 NCs@MnO2 NSs CSA/GCE CV DA L.R. ¼ 18.30–118.58 μM Injection purchased sample (92%–101.7%) [89]
EIS LOD ¼ 1.75 nM
Sens. ¼ 1249.9 μA/mM.cm2
Ni(OH)2 AuNPs/Ni(OH)2 NS/GCE Amp Glc L.R. ¼ 0.002–6.0 mM Food samples (96%103.7%) [88]
LOD ¼ 0.66 μM
Sens. ¼ 82.71 μA/mM.cm2

calcination treatment creates more catalytic sites for the oxidation of
electroactive species [146,147]. Hydrothermal approach is also appli-
cable to get 3D porous structure with silver(I) nanoparticles under 120  C
for around 6 h. These conditions allow synthesizing hollow urchin-like
α-MnO2 material with aligned nanowires of large cavities (47.23 m2/g)
(Fig. 3 A, B) [129].
4.3. Designing 3D sensing platforms
Porous sensing platforms considerably perform the sensor sensitivity,
especially, using 3D structure with high specific surface area (SSA). To
determine SAA parameter, Cottrell theory estimates the adsorbed
amount of the electrochemical active species and then provides the dif-
ference between faradaic charge indicating morphology change (Table 2)
[133]. Growing metal oxides is a fast strategy producing porous structure
such as incorporation of ferric ion (Fe3þ) into MnO2 framework forming
hydrangea-like morphology with large electroactive surface area of
(54.01 m2/g) (Fig. 3 C, D) [128]. Similar recent approaches like depo-
sition of conducting polymer or metal oxides (In2O3 or ZnO) on the
surface of three-dimensional carbon materials enlarges the specific sur-
face area (77.5120 m2/g) [127,148,149]. Moreover, calcination of ZnO
and carbon materials functionalized with amine groups improves the
formation of the porous structure while keeping the ZnO rose flower-like
morphology (Fig. 3 E, F) [150]. Similarly, loading CoMoO4 nanorods on
the surface of 3D macroporous carbon considerably increases the surface
area from 22.24 m2/g (CoMoO4) to 105 m2/g (CoMoO4/3DMC) [131].
Also, hydrothermal synthesis and carbonization of copper (Cu) under
argon atmosphere provides 3-D flower-like structure with increasing the
value of the surface specific area from 15.04 m2/g (Cu-MOF) to
34.09 m2/g (Cu/CuxO/NC) [132].
As can be seen in Fig. 3, metal oxides synthesized by hydrothermal
method provide a three-dimensional morphology with high specific
surface area. The mechanical properties of sensing platforms can be
performed by combination of conducting polymers to offer more
robustness and high surface roughness. The three-dimensional structure
is depending on the working temperature of hydrothermal synthesis. The
main shortcoming is the long synthesis reaction time and high working
temperature. In the other hand, 3D-printing of carbon materials in flex-
ible polymers provides ready-to-use sensing platforms for miniaturiza-
tion in electrochemical sensing applications which is the main challenge
in constructing miniaturized sensors for healthcare applications.

5. Progress and future directions

Recent methods efficiently improve the performance of catalytic

Fig. 2. HRTEM image of COFETTA-TPAL into COFETTA-TPAL-Fc(COOH)2 nano-
spheres. (A), partial enlarged TEM image (B). Reproduced with permission
from Ref. [126].
sensing interfaces using multifunction groups and the significant prog-
ress in preparing 2D nanocomposites provides a comprehensive evalua-
tion of the advanced sensor technology [154,155]. However, recent
requirements for continuous control of chronic diseases and human body
activities are not sufficiently fulfilled because of the limited application

7
A. Fethi
Fig. 3. Morphological SEM images of nanocomposites synthesized at 120  C for
6 h based on urchin-like α-MnO2 (A–B). Reproduced with permission from
Ref. [129]. SEM images of Fe3þ@ε-MnO2 (C–D). Reproduced with permission
from Ref. [128]. SEM images of rose flower-like ZnO before calcination (E) and
after calcination (F). Reproduced with permission from Ref. [150].
of flexible smart biosensors [156]. Although the several recent efforts
trying to develop new features for controlling human health risks by
wearable sensors [157–160].
5.1. Cancer biosensors
Ultra-high sensitive detection of cancer biomarkers promotes early
diagnosis which prevents mitigation of cancer metastasis and, therefore,
therapy becomes possible providing a definitive recovery [21]. Dual
signal amplification is a strategy detects different types of cancer by
sandwiching the cancer antigen between the immuno-platform with
surface-end secondary antibody (Ab2) and substrate material contains
primary antibody (Ab1). Hence, the sensitivity of sandwich-type bio-
sensors is highly dependent on the material nanocomposites [161].
Intense efforts now underway to enhance their electrocatalytic ability to
react with signal probes (H2O2, ferrocene) [153]. Ma et al., 2019 have
prepared a 3-dimensional sensing platform for the detection of carci-
noembryonic antigen (CEA) with hollow nanotubes morphology by
high-temperature calcination after hybridization of CoS2 nanoparticles
with carbon (Fig. 4A-B) [152]. Recently, porous sensing platform
mulberry-shaped based on trimetallic component (Au@PtPd) as a signal
amplifier allowing high catalytic reduction of H2O2 with ultra-low
detection limit of cancer biomarkers (LOD ¼ 16.7 fg/mL) (Fig. 4C, D)
[151]. Also, the combination of Ti3C2Tx with gold nanoparticles and
conducting polymer show an excellent analytical performance for the
determination of prostate-specific antigen (LOD ¼ 0.04 pg/mL) [75].
5.2. Wearable flexible sensors
Biocompatibility and biodegradability of 2D nanomaterials are
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Sensors International 1 (2020) 100035
Fig. 4. SEM images of calcined CoS2@C nanocomposite (A) and CoS2@C hol-
low nanotubes (B). Reproduced with permission from Ref. [152]. SEM images of
MoS2/CuS nanocomposites (C) TEM image of Au@PtPd MPs (D) Reproduced
with permission from Ref. [151].
promising characteristics led to design implantable and wearable flexible
sensors [162–167]. These tools have tunable nanostructure allowing
continuous control of chemical and physical human activities [168–171].
However, flexible sensors are still not largely commercialized because of
the high-cost instruments for printing devices. Thus, there is a need for
fast printing strategies using stretchable conductive polymers (Fig. 5.)
[172–174]. Recently, novel synthetic technique of printable inks using
MXene derived quantum dots construct wearable biosensor for in vitro
perspiration analysis (Fig. 6. A) [54]. Also, PEDOT:PSS solution is the
most favorable polymer ink since it forms a transparent film with an
excellent conductance and high thermal stability [175,176] (Fig. 6B).
The incorporation of carbon materials in polymeric matrix is a
cost-effective method to get flexible nanostructure with satisfactory
properties [177,178]. Especially, carbon materials spin-coated elastic
polymeric substrates such as, polyethylene terephthalate (PETE), poly-
dimethylsiloxane (PDMS) [172], styrene ethylene butylene styrene
(SEBS). Polyimide is also a flexible and printable material with good
mechanical, and thermophysical characteristics [179], its combination
with molybdenum disulfide (MoS2) using plasma enhanced-chemical
vapor deposition (PE-CVD) constructs flexible biosensor for endocrine
hormones quantification (Fig. 6C) [180]. However, coffee ring effect is a
frequent drawback during spin-coting process. Efficient methods can
perform the inkjet process by controlling the evaporation or by incor-
poration of hydrogel in carbon nanocomposite or with plasticizing film
polymer with ionic liquids [176,181–183].
5.3. Nanozymes in biomedical and environmental applications
The eco-friendly synthesis methods of novel materials with controlled
size and morphology gain much interest in constructing sensing plat-
forms and several recent papers review their application in biomedical
field [184,185]. Accordingly, recent application of hybrid nano-
structured materials in healthcare area enables their utilization as
sensing biointerfaces for monitoring small molecules [186–189]. The use
of nanomaterials with enzyme-like properties overcomes the limitations
related to the use of biological elements such as loss of activity and
enzyme denaturation which causes low stability in sensor response [190,
191]. Nanozymes are now successfully applied for cancer immuno-
therapy and for monitoring human activities like respiration control
[192–194]. For instance, new sensors based on stabilized zirconia solid
electrolyte can measure the exhaled breath of diabetic people and can
A. Fethi
Fig. 5. Schematic illustration of fabrication sequence for PEDOT:PSS conductive polymer film. Reproduced with permission from Ref. [172].
control iso-propanol (IPA) in the breath of patients [195,196]. Also,
sensor-based on Zn2SnO4 film synthesized by spray pyrolysis method can
detect NO2 at low concentration (8 ppm) under an operating temperature
of 200  C without using any additional catalyst [197]. Recently, new
sensors based on functionalized TiO2 nanoparticles with silver and gra-
phene oxide offer nano-level detection of drugs like furantril, nimesulide
(LOD ¼ 1.44 nM) and ambroxol (1.05 nM) in human urine and pharma-
ceutical samples [198–200].
The use of chitosan thin films promotes fast diffusion of the inter-
esting target molecule since this polymer is reusable with good catalytic
properties and can serve as support for the degradation of environmental
pollutants [201–203]. Thus, the irradiation method provides a homo-
geneous distribution of small size nanoparticles on carbon nanosheets
and can decorate multi-wall carbon nanotubes (MWCNTs) with variety of
metal oxide nanoparticles such as iron oxide or bismuth nanoparticles
[204]. Bhakta A.K. et al. (2020) have decorated multi-wall carbon
nanotubes with lanthanum hydroxide nanoparticles using diazonium to
construct sensors for environmental applications [205]. Similarly, in
order to enhance the surface area of the carbon paste electrode, bismuth
was used to decorate multi-walled carbon nanotubes by drop-casting
method with cetyltrimethylammonium bromide [206].
6. Current issues in electrochemical miniaturized sensors
There has been still challenging issues and future directions in
nanomaterials synthesis to further improve the performance of sensing
platforms. Several current efforts now interest in constructing flexible
structures with 2D materials such as MXene as a pressure sensor for the
detection of gases [207–209]. However, the aggregation of MXene is still
a limitation in constructing sensors and often resulted in using carbon
materials that serve as interlayer spacers such as amino-functionalized
carbon nanotubes [210,211]. Also, the use of NH4 ions during the
MXene coagulation promotes large dispersion and can assemble sheets
into flexible fiber morphology using wet-spinning method [212]. Recent
strategy constructs wearable sensor using liquid nitrogen frozening and
vacuum drying after annealing process to form a 3D macrostructure of
the Mxene/Go aerogel nanocomposite [213]. Interestingly, recent report
shows that the addition of sugar and sucrose monopalmitate as a sur-
factant for the stabilization of gold nanoparticles promotes large
dispersion and can avoid aggregation [214].
MOFs nanoplatforms have high adsorption capacity and mesoporous
structure with fast functionalization and good biocompatibility [215].
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Sensors International 1 (2020) 100035
However, MOFs still suffer from stability issues which is closely related to
their structures, and several new approaches were applied to overcome
this limitation [216,217]. Also, the use of concentrated salts with high
rate of ion association is the main shortcoming in the synthesis of plat-
forms because it increases the bulk electrolyte resistance [218]. The
addition of functional groups for MOFs synthesis such as carboxylates
and phosphates decrease the pka value of imidazolate ligands providing
more acid stability and good dispersibility of zeolitic imidazolate
frameworks (ZIFs) [219].
3D-printed carbon electrodes are promising catalysts for sensing
applications due to their surface roughness with more catalytic sites.
These electrodes were made by three-principle printing strategies, the
selective laser melting (SLM) [220,221], fused deposition modeling
(FDM), and the direct ink writing [222–224]. This last suffers from
changes in filament microstructures during the direct ink writing while
FDM strategy is the most used to construct sensing platforms, however,
high working temperature is its main shortcoming [225,226]. Inter-
estingly, printing pharmaceuticals like thermolabile drugs with low
FDM printing temperature is now possible [227]. On the other hand,
printing strategies have many advantages such as one-step processing
and can produce uniform porosity provided that some parameters are
adequately optimized like rheological properties of printable polymers
and the printing speed since it affects the morphology and mechanical
properties of printed platforms [228,229]. To perform more these
sensing platforms, several other parameters should be taken into ac-
count during the synthesis process including pore structure, specific
surface area, electrical conductivity, mechanical properties (flexi-
bility), and material density [230,231]. Another main advantage of
these strategies is the use of eco-friendly materials and biodegradable
printable polymers with high conductivity which leads to quantify
pollutants and heavy metals in real samples [232–234]. For instance, V.
Katseli et al., 2020 have prepared 3D-printed electrodes as miniatur-
ized sensor for the detection of Hg(II) in bottled water and fish oil
samples using polylactic acid (PLA) [235,236]. This thermoplastic
polymer is intensely used to prepare 3D-Printed nanocomposites due to
its fast incorporation with various organic and inorganic colloids and
low printing energy [237–239]. Sensing platforms based on PLA
polymer are assemblable in a portable system and disposable sensors
for glucose monitoring in biological fluids [240]. However, the limit of
detection is still in micro-level, this may be due to the absence of
porosity of PLA polymer which the use of epoxy chain extension reac-
tion can improve their pore properties [222].
A. Fethi
7. Conclusion
In this paper, recent advances in design strategies of 2D nano-
materials for sensing applications are addressed in detail. Synthesis
methods for regulate structures with morphology control and uniform
size distribution are comprehensively reviewed. As shown, significant
progress has been made to best explore the electrochemical properties of
nanomaterials with a 3D sensing interface. A variety of sensing tools for
the determination of a wide range of hazardous materials and chemical
compounds including even cancer biomarkers are now available with
new design and more unique properties.
However, there are still several drawbacks in the synthesis and design
of nanomaterials including aggregation phenomenon, strong interfacial
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Sensors International 1 (2020) 100035
Fig. 6. Schematic of the MXene-Based
wearable biosensor with an optical image of
the sensor wristband laminated on human
skin (A). Reproduced with permission from
Ref. [54]. Schematic of 3D printing of con-
ducting PEDOT: PSS polymer on poly-
ethylene terephthalate (PETE) substrate (B).
Reproduced with permission from
Ref. [175]. Schematic of the process for the
synthesis of MoS2 on a flexible Au-PI elec-
trode (MoS2–Au-Polyimide flexible sensor)
using PE-CVD at 150  C (C). Reproduced
with permission from Ref. [180].
interactions, concentrated etching agents, morphology-dependent
growth time, and high-temperature working range. Thus, future chal-
lenges required for more useful strategies to synthesis novel nano-
composites in sensing applications. Actually, there has been an urgent
need to develop fast printing strategies in constructing flexible platforms
for the miniaturization of wearable biosensors owing to their ability to
real-time controlling of human chronic diseases.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
A. Fethi Sensors International 1 (2020) 100035

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