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ChemElectroChem - 2020 - Hassanvand - Carbon Nanodots in Electrochemical Sensors and Biosensors A Review

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ChemElectroChem - 2020 - Hassanvand - Carbon Nanodots in Electrochemical Sensors and Biosensors A Review

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Reviews

ChemElectroChem doi.org/10.1002/celc.202001229

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3 Carbon Nanodots in Electrochemical Sensors and
4
5
Biosensors: A Review
6
7
Zahra Hassanvand,*[a] Fahimeh Jalali,[a] Maryam Nazari,[a] Fatemeh Parnianchi,[a] and
8 Carlo Santoro*[b]
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ChemElectroChem 2021, 8, 15 – 35 15 © 2020 Wiley-VCH GmbH

21960216, 2021, 1, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/celc.202001229 by University Of Waterloo, Wiley Online Library on [25/09/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Reviews
ChemElectroChem doi.org/10.1002/celc.202001229

1 This Review presents the latest advances in designing electro- their unique features such as quantum size, excellent biocom-
2 chemical sensors by using carbon nanodots (CNDs), carbon patibility, enzyme-like activity, high active area, and abundance
3 dots (CDs), and graphene quantum dots (GQDs), as a new class of hydrophilic groups, such as hydroxyl, carboxyl, or amine
4 of photoluminescent nanomaterials, which can be employed in functionalities. The applications of CDs and GQDs for the
5 a vast number applications, such as biomedicine, biosensing, electrochemical sensing of hydrogen peroxide, glucose, other
6 optical sensing, catalysis, solar cells, imaging, and electro- organic molecules, as well as metal ions are presented. The
7 chemical sensing. Recently, the application of CDs and GQDs in utilization of CDs and GQDs for immunosensing and aptasens-
8 electrochemical sensing has increased significantly because of ing is also reported.
9
10
1. Introduction in various applications.[7,12–16] Moreover, CDs and GQDs also
11
demonstrated promising electrocatalytic activity for excellent
12
Generally, semiconductor nanocrystals, having 1–10 nm diame- conductivity, water solubility and the further functionalization
13
ters and containing typically 103 to 104 atoms, are known as with various biological, organic, inorganic, or polymeric
14
quantum dots (QDs). Their charge carriers (electrons and holes) species.[17] One way for improving the electronic and electro-
15
show quantum confinement in all three spatial dimensions,[1] catalytic characteristics of CDs and GQDs is chemical doping
16
leading to discrete energy states. Light absorption and emission which also amends their electrical and thermal properties.[18]
17
are the excellent consequent of energy states-splitting. A Moreover, it is also feasible to combine other types of
18
significant number of researches about QDs is devoted to their nanomaterials with CDs and GQDs to form nanocomposites.
19
luminescence properties.[2] QDs are serious competitors for This leads to diverse properties and features in a single new
20
organic dyes in cellular labeling and tissue imaging areas[3,4] and material.[19] Electrochemiluminescence (ECL) applications of
21
in solar cells.[5] Carbon nanodots (CNDs), on the other hand, CNDs have been reviewed previously.[20,21] Herein, in this review
22
were initially discovered during the purification and separation work, the applications related to CDs and GQDs in electro-
23
of single-walled carbon nanotubes.[6] CNDs are found to be chemical sensors and biosensors are described and presented.
24
superior to other semiconductor QDs (e. g. CdTe, CdSe) due to This review presents the latest developments of electro-
25
low toxicity, high-biocompatibility, good chemical inertness and chemical sensors using carbon nanodots (CNDs), including
26
solubility.[7] CNDs could be categorized into two main groups: i) carbon dots (CDs), and graphene quantum dots (GQDs). In the
27
carbon-dots (CDs) and ii) graphene quantum dots (GQDs). The following parts, the application, and the synthesis methods of
28
former are typically quasi-spherical nanoparticles with sizes CDs and GQDs are described and electrochemical sensing of
29
lower than 10 nm and may be amorphous or nano-crystalline some significant analytes such as hydrogen peroxide, glucose,
30
with sp2/sp3 carbon clusters. Various particle sizes of CDs is metal ions, and organic molecules are reported. The utilization
31
obtainable under controlling reaction time, reaction temper- of CDs and GQDs for immunosensing and aptasensing is also
32
ature, and other synthesis factors.[8] They have exceptional considered. A full list of abbreviations used in this Review can
33
photochemical and physicochemical stability. Due to facile be found in the Supporting Information.
34
synthesis aqueous solubility, and their quantum yield, they are
35
superior to the other carbon nanoparticles with the property of
36
fluorescence.[8] However, GQDs resemble graphene nano-sheets
37 2. Electrochemical Carbon Nanodot-Based
with less than 100 nm lateral size (a few benzenic rings) as
38
studied by Ponomarenko et al. in 2008[9] and with the mixtures Sensors and Biosensors
39
of sp2 and sp3 carbons,[10] GQDs possess outstanding properties
40
including high surface area, large diameter, and having Among various nano-materials, CNDs have attracted great
41
conjugated π-π network for good surface grafting and the interest in electroanalytical investigations for their up-normal π-
42
other physical features.[11] The advantages of CDs and GQDs as π conjugation structure, inherent low toxicity, high solubility in
43
luminescent probes, such as, tunable emission wavelength, numerous solvents, high electrical conductivity, chemical and
44
high emission intensity, biocompatibility, and general excitation mechanical properties, quantum size, large active area, huge
45
source, made them excellent candidates as luminescent probes functional groups, abundant edge sites for functionalization,
46
intrinsic catalytic activities, and excellent biocompatibility.[22] In
47
the following sections, firstly differences between CNDs and
48 [a] Dr. Z. Hassanvand, Prof. F. Jalali, Dr. M. Nazari, F. Parnianchi
Faculty of Chemistry
carbon nanoparticles are exploited, secondly the synthesis
49
Razi University methods of CNDs are reported, thirdly the differences between
50 Kermanshah, Iran CDs and GQDs are described and fourthly, the immobilization
51 E-mail: [email protected]
[b] Dr. C. Santoro
of various molecules over CNDs is described. Moreover; the
52
Department of Chemical Engineering and Analytical Science sensing of: i) hydrogen peroxide and glucose; ii) various organic
53 The University of Manchester, The Mill Sackville Street molecules and iii) metal ion is presented. At last, the utilization
54 Manchester, M13PAL, UK
E-mail: [email protected]
of CNDs for immunosensing and aptasensing is also showed.
55
56 Supporting information for this article is available on the WWW under
https://doi.org/10.1002/celc.202001229
57

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 16 © 2020 Wiley-VCH GmbH

2.1. Differences between Carbon Nanodots and Carbon 2.2. Synthesis of Carbon Nanodots
1
Nanoparticles
2
CNDs synthesis techniques can be divided in two categories: i)
3
The difference of CNDs and other carbon nanomaterials are top-down and ii) bottom-up strategies. Top-down approaches
4
described below. Carbon materials, like graphite, graphene, focus on breaking down bigger carbon structures into nano-
5
carbon nanotubes, fullerene, and diamond have usually been scale structures using chemical, electrochemical,[26–28] or physical
6
widely used in the field of material science because they are methods such as arc discharge,[29] laser ablation (a simple
7
environmentally friendly, relatively easy to fabricate or synthe- approach to prepare carbon quantum dots focusing to laser
8
size and often largely commercially available. The macro-sized irradiation),[15,30] etc. On the contrary, bottom-up approaches
9
carbon material can difficultly serve as an ideal luminescent refer to the synthesis of CNDs from smaller carbon units (small
10
material due to lacking a suitable band gap.[23] CNDs are a organic molecules) mostly by using chemical synthesis, com-
11
greatly attractive alternative form of carbon for “older gener- prising template method,[31–33] microwave and hydrothermal
12
ation” of intensively considered carbon nanostructures. They synthesis.[34–37] In general, top-down strategies enable to obtain
13
are versatile nanocarbon materials and can also be well- CNDs with superior featured and therefore performance, but it
14
dispersed in water due to polar groups derived from starting also suffers from some disadvantages including lower
15
materials in their formation.[24] Compare to other nanoparticles, fluorescence quantum yield, difficult gathering, sophisticated
16
GQDs are widely employed in numerous areas of photocatalysis, procedures, and costly instruments. In the case of bottom-up
17
bioimaging applications, biosensing, optoelectronic tools, bio- strategies, the synthetic conditions are easier to be controlled,
18
logical, and environmental uses due to attractive advantage of more carbon sources are available and suitable for the synthesis
19
the electrochemical properties identical to graphene.[25] and the synthesized CNDs usually have higher fluorescence
20
quantum yield. The only disadvantage of this approach is that,
21
the following-up purification steps are more complicated and
22
23
24 Dr. Zahra Hassanvand received her Master’s Fatemeh Parnianchi is a PhD student at Razi
25 and PhD degrees in Analytical Chemistry from University, Kermanshah (Iran). She received
Razi University, Kermanshah (Iran) in 2013 and her Bachelor’s and Master’s degrees in 2010
26
2019, respectively. During her Master’s course, and 2014, respectively. She works in the field
27 her research focused on voltammetric deter- of sensors and biosensors and her PhD thesis
28 mination of gabapentin and amantadine is about bilirubin and lipophilic analytes
29 hydrochloride based on chemically modified sensors. She is interested in electrochemistry,
30 electrodes. Her PhD research activity con- biofuel cells, and drug delivery. She has also
31 cerned the fabrication of sensors for the expertise in molecular docking and Gaussian
determination of several pharmaceutical and software.
32 biological compounds. Her research interests
33 Dr. Carlo Santoro obtained his BSc (2006) and
lie under the umbrella of electrochemical
34 MSc (2008) in Environmental Engineering at
analysis.
the Politecnico di Milano (Italy). He then
35
Prof. Fahimeh Jalali received her PhD degree moved to the University of Connecticut (USA)
36 in Analytical Chemistry from Razi University, in 2009 obtaining his PhD in 2013 working on
37 Kermanshah (Iran), where she is currently a microbial fuel cell. He moved to the University
38 Professor of Chemistry. Her research is mainly of New Mexico (UNM, USA) in 2013 for his first
39 focused on electrochemical sensors and bio- post-doctorate developing hybrid microbial
sensors, surfactants, potentiometry, and spec- fuel cells with microbial anode and enzymatic
40
troscopy. cathode. As second post-doctoral experience,
41 he worked at Nanyang Technical University
42 (Singapore), developing biosensors to detect
43 volatile organic compounds. In 2015, he
44 Dr. Maryam Nazari received B.S., Master’s, and moved back to UNM working on low-cost
45 PhD degrees in Applied Chemistry from Razi platinum-free catalyst for oxygen reduction
University, Kermanshah (Iran) in 2011, 2013, reaction as well as supercapacitive bioelectro-
46
and 2019, respectively. During her Master’s chemical systems. From 2017 to 2020, he
47 course, her research focused on the fabrica- worked at University of the West of England,
48 tion of laccase biosensors for the detection of Bristol (UK). He is currently Lecturer at the
49 catechol. Her PhD research activity concerned University of Manchester (UK) in the Chemical
50 the fabrication of sensors and biosensors for Engineering and Analytical Science Depart-
51 phenolic compounds and the development of ment. His areas of expertise are on electro-
drug delivery carriers, under the supervision catalysis, carbonaceous materials, sensors and
52
of Prof. S. Kashanian. She has been an biosensors and electrochemical conversion
53 academic staff member at Razi University systems.
54 since 2020. Her main scientific interests are
55 sensors, biosensors, biofuel cells, and pharma-
56 ceutical formulations.
57

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 17 © 2020 Wiley-VCH GmbH

time consuming which leads to significant effect on the 2.4. Immobilization of Various Molecules on the Surface of
1
performance of CNDs. Bottom up technique is now the leading Electrodes through the Utilization of CNDs
2
tactics for synthesis.
3
CNDs usually contain functional groups (carboxyl, hydroxyl,
4
carbonyl, epoxide) at their edges that can act as reaction
5
2.3. Morphological Differences between Carbon Dots and sites.[43] Moreover, on these functional groups surface, varied
6
Graphene Quantum Dots organic/inorganic moieties and biomolecules (antibody, en-
7
zyme, protein, DNA, antigen, etc.) could be immobilized.
8
Carbon-based dots comprising CDs and GQDs are commonly Besides, because of supernormal π-π conjugation and electro-
9
defined as zero dimensional materials with bright fluorescent. static adsorption, organic conjugated molecules and materials
10
The former are typically fabricated by bottom-up synthetic with charged groups could be immobilized on their surface of
11
approaches and have spherical shape up to 10 nm,[38] although, them. For example, considerable progress was obtained by the
12
a few hollow-structured CDs have also been reported.[39,40] They work of Shao et al.[44] in which an electrochemical biosensor
13
can be amorphous or nanocrystalline with sp2 carbon clusters. based on CDs is employed to detect cerebral Cu2 + in rat brain
14
Some studies suggest the existence of diamond-like structure micro-dialysates, directly (Figure 1A). The highly selective ligand
15
formed by sp3 carbons.[30] In contrast, GQDs are usually derived towards Cu2 + was attached covalently to the large active area
16
from graphite/graphene or other graphitic 3D material by top- offered by CDs. Biocompatibility, and strong ability of CDs for
17
down synthetic methods. They generally exist in few-layer electron transfer, and high surface area (due to small size) were
18
structures, with lateral dimension up to 100 nm.[38,41] GQDs among the advantages of CDs which make them good
19
clearly possess a graphene structure inside the dots and characteristics and features for sensors and biosensors in order
20
commonly have higher crystallinity compare to CDs.[22] The to monitor physiological and pathological processes; hence CDs
21
shape of most synthesized GQDs is circular or elliptical, were applied for increasing of electrochemical recognition
22
although triangular, quadrate and hexagonal GQDs have been sensitivity. In this study, N-(2-aminoethyl)-N,N’,N’-tris-(pyridine-
23
synthesized as well.[42] 2-yl-methyl)ethane-1,2-diamine (AE-TPEA) was designed as a
24
specific molecule for improving of Cu2 + detection against other
25
metal ions with high selectivity. It was conjugated to COOH
26
and OH groups functionalized CDs through N-(3-(dimeth-
27
ylaminopropyl)-N’-ethylcarbodiimide hydrochloride (EDC), N
28
29
30
31
32
33
34
35
36
37
38
39
40
41
42
43
44
45
46
47
48
49
50
51
52
53
54
55 Figure 1. CD and GQDs based electrochemical assays. A) Illustration of an electrochemical method for monitoring Cu2 +. Adapted from Ref.[44] with permission;
Copyright (2012) American Chemical Society. B) The illustrative fabrication process of the pralidoxime (PAM)/GQDs/GCE for organophosphorus pesticides
56 sensing. Adapted from Ref.[45] with permission; Copyright (2015) Elsevier.
57

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 18 © 2020 Wiley-VCH GmbH

hydroxysuccinimide (NHS) chemistry. Moreover, GQDs were also GQDs-CS/MB casted over GCE. As another example, CDs nano-
1
used for modification of electrodes, and immobilization of hybrid in combination with silver nanoparticles (AgNPs/CDs)
2
ligands or electrochemical probes on electrodes surfaces. An casted on the GCE was successfully tested as an amperometric
3
oxime-based sensor through attaching pralidoxime (PAM) on H2O2 sensor. Interestingly, it was shown that Ag NPs and CDs
4
GQDs casted over glassy carbon electrode (GCE) was reported was able to mimic enzymatic activity and improve the detection
5
to detect the non-electroactive organophosphorus pesticides of the molecule of interest.[47] Moreover, a new electrochemical
6
(OPs) (Figure 1B). PAM was linked to GQDs through π-π platform fabricated by using reduced graphene oxide quantum
7
stacking interaction and electrostatic attraction with numerous dots (rGO QDs)/ZnO nanofibers (NFs) was studied and partic-
8
hydroxyl and carboxyl groups of GQDs. The introduction of ularly with the intention of measuring the intracellular H2O2
9
GQDs highly improved the electrode surface, and then extend released from cancerous and non-cancerous cells after anti-
10
the immobilization value of PAM. Therefore, the oxidation cancer drugs treatment. Enhanced catalytic activity was
11
current of PAM clearly raised and the oxidation current of PAM observed, which ascribed to the synergistic impact and to the
12
was decreased in the existence of fenthion.[45] large surface area between rGO QDs and ZnO nanofibers. It was
13
revealed that the proposed electrode shows high electro-
14
catalytic activity toward H2O2 released from prostate cancer cell
15
2.5. Use of CNDs for Electrochemical Sensing and Biosensing (PC-3) versus non-cancerous cell (BPH-1) therefore facilitating
16
the detectability of peroxide.[48] Furthermore, CDs/MWCNTs/GCE
17
CDs and GQDs have electrocatalytic activity for the reduction displayed a novel electrocatalytic activity towards H2O2
18
reaction of hydrogen peroxide (H2O2) and oxygen (O2). In reduction.[49]
19
parallel, CDs and GQDs showed activity towards the oxidation Also, blood glucose (GLC) has a significant impact for
20
of glucose mimicking glucose oxidase enzyme in the determi- human health. Numerous approaches including electrochemical
21
nation of glucose (GLC). CDs and GDQs are also reactive techniques are pursued to develop advanced GLC sensors. In
22
towards organic molecules, metal ions, and other relevant general, in electrochemical detection of GLC, glucose oxidase
23
substances, and therefore can be also applied for the sensing of enzyme (GOx) is used. The latter is able to catalyze GLC and
24
these molecules/ions/compounds. produce a current response that can be correlated positively
25
with the concentration of GLC.[22] Razmi et al. introduced high
26
performance GLC biosensor via GQD modified carbon ceramic
27
2.5.1. Hydrogen Peroxide (H2O2) and Glucose (GLC) Sensing electrode (CCE).[50] Because of the abundance of hydrophilic
28
edges and hydrophobic plane, large surface area, and high
29
H2O2 is a significant compound which is usually applied in porosity in GQD, the enzyme absorption on the electrode
30
industrial processes as oxidant.[17] However, high H2O2 concen- surface was improved. Li et al. synthesized the nanostructure
31
trations may be perilous for humans.[17] Hence, precise and electrocatalyst of CQDs/octahedral-cuprous oxide (Cu2O) to
32
accurate measurement of H2O2 is of vital importance. Different fabricate the non-enzymatic electrochemical sensors for the
33
procedures have been applied to determine H2O2. Among detection of GLC and H2O2.[51] CDs/octahedral Cu2O showed
34
which, it has been revealed that electrochemical sensors are a desirable electrocatalysis to the GLC oxidation and H2O2
35
promising method because of some useful features including reduction compared to octahedral Cu2O. Table 1 depicts a list of
36
being accurate, easy to handle and showing quick response. In electrochemical sensors for detecting H2O2 and GLC based on
37
general, related proteins or enzymes, like hemoglobin, myoglo- applications of CDs and GQDs
38
bin and horseradish peroxidase are used in the electrochemical
39
detecting for H2O2. Nevertheless, both proteins and enzymes
40
despite being very specific and sensitive to peroxide, they are 2.5.2. Organic Compound Detection
41
very costly, possess very finite lifetime and the operating
42
condition for the detection of H2O2 are quite problematic. The detection of organic molecules is highly important,
43
Recently, some inorganic nanomaterials such as metals, metal particularly those products with vital significance and ascorbic
44
oxides, and carbon nanomaterials have been made as acid (AA), biomolecules like dopamine (DA), uric acid (UA),
45
peroxidase biomimicking enzymes. These materials were used nicotinamide adenine dinucleotide (NADH) and so on. In fact,
46
in order to substitute enzymes (enzyme-less sensing) in the electrochemical sensors have achieved much more consider-
47
detection of H2O2. Related to this matter, CDs and GQDs ation and interests for various kind of organic molecules
48
showed the possibility of mimicking enzyme activity and they monitoring such as drugs, vitamins, chemicals pollutants,
49
have been reported as a non-enzymatic sensor for the detection explosives and amino acids because of low cost, simple
50
of H2O2.[46] Particularly, nanostructured GQDs-chitosan (GQDs- operation and high sensitivity. CNDs could be beneficial by
51
CS) was used for effective immobilization of methylene blue enhancing the electrochemical active surface area that is
52
(MB) via amino-hydroxyl reaction. Thus, the synergistic effect capable of interacting with some electroactive analytes, so
53
between MB and GQDs-CS leads to the resulting sensor to modification of electrode by CNDs can reinforce the rate of
54
exhibit appealing specific sensor activity. Potential interferents electrochemical reaction and therefore the signal output.
55
like dopamine, glucose, caffeine, uric and ascorbic acids and Several neurological illnesses can be connected to the
56
various inorganic salts hinder the electrochemical replication of abnormalities in dopamine (DA) concentrations. Thus, detection
57

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 19 © 2020 Wiley-VCH GmbH

1 Table 1. A list of applications of CDs and GQDs based electrochemical sensors for detection of H2O2 and GLC.
2 Modified electrode Target Method Linear range Detection Refs.
3 limit

4 CQDs/GCE H2O2 amperometry 100 nM–1 mM 300 nM [52]

[53]
5 NF/b-GQD/GCE H2O2 amperometry 1–10 mM 0.02 mM
[46]
GQDs-CS/MB/GCE H2O2 amperometry 1 μM–11.78 mM 0.7 μM
6
7 AgNPs/CDs/GCE H2O2 amperometry 0.2–27.0 μM 80 nM [47]
[54]
8 Ag/CNC/GCE H2O2 amperometry 5.00 μM–11.05 mM 0.51 μM
[48]
rGOQDs/ZnO NFs/ITO H2O2 amperometry 1–22.48 μM 0.025 μM
9
10 CDs/MWCNTs/GCE H2O2 amperometry 3.5 μM–30 mM 0.25 μM [49]
[55]
11 AuNPs-N-GQDs/GCE H2O2 amperometry 0.25 μM–13.327 mM 0.12 μM
[18]
Nitrogen doped carbon dots (NCDs)/(GCE) H2O2 DPV 0.05 μM–2.25 mM 41 nM
12 Ag/C/GCE H2O2 amperometry 4–25.5 mM 1.3 μM [56]

13 GQDs/AuNPs-PDA-GQD/ITO H2O2 amperometry 0.1–20000 μM 5.8 nM [57]

[58]
14 Pd Nanoparticles/N- GQDs @N-Carbon Hollow structured-Nanospheres (HNSs)/GCE H2O2 amperometry 250 nM–4 mM 20 nM
[51]
CQDs/Cu2O/NF/GCE H2O2 amperometry 5 μM–5.3 mM 2.8 μM
15 HRP/C-Dots/LDHs/GCE H2O2 amperometry 0.1–23.1 μM 0.04 μM [59]

16
[60]
17 GQDs/cysteamine/Au electrode H2O2 amperometry 0.002 to 8 mM 0.7 mM
[61]
CS-GODs/AgNCs/Au H2O2 CV 10 μM to 7.38 mM 0.15 μM
18 amperometry
19 Ternary GQD- PNF-GO/GCE H2O2 amperometry 0.01–7.2 mM 0.055 μM [62]
[63]
20 PtNPs-CDs/IL-GO H2O2 amperometry 1–900 μM 0.1 μM
[64]
PVA/GQD/GCE H2O2 amperometry 0.1–200 mM 0.53 μM
21
22 CuO@CQDs@CHNS H2O2 amperometry 0.1–1459 μM 2.4 nM [65]

23 /GCE
[17]
NF/HRP/NH2-CD/GCE H2O2 amperometry 5–590 nM 1.8 nM
24 AuPd-ANPs/GQDs/ACF microelectrode H2O2 amperometry 1.0 μM–18.44 mM 500 nM [66]

25 Cyt c/CD-MWCNTs/GCE H2O2 amperometry 2–30 μM 1.02 μM [67]

26 30–270 μM 2.59 μM
[68]
PEI-CDs/GCE H2O2 amperometry – –
27 And
28 CA-CDs/GCE
[69]
29 CDs-Pt nanocomposite/ITO electrodes H2O2 CV 2.5 μM–1 mM 0.8 μM
GLC – –
30 Hb-GQDs-CS/GCE H2O2 amperometry 1.5–195 μM 0.68 μM [70]

31 AuNPs@CDs/GCE H2O2 amperometry – – [71]

32 CV
[72]
NF/Hb/B-GQDs/CILE H2O2 DPV 5-26 mM 0.04 mM
33 TCA 0.1–300 mM 0.053 mM
34 NaNO2 0.1–100 mM 0.03 mM
[73]
35 GQDs/modified Pt disk OH CV 3M –
*
[74]
SOD-GNPs-CS-IL)/GCE (O2 ) CV 5.6–2700 nM 1.7 nM
36 amperometry
37 GOx-GQD/CCE GLC amperometry 5–1270 μM 1.73 μM [50]

38 [75]
NiO@NCDs/Ni foam electrodes GLC amperometry 5 μM to 12 mM 0.01 μM
39 GOD-CNDs-rGO/GCE GLC CV 40 μM–20 mM 40 μM [76]

40 GQDs/CoNiAl-LDH/CPE GLC amperometry 0.01–14.0 mM 6 μM [77]

[78]
41 N-doped CDs/CS/GOx/GCE GLC CV 1–12 mM 0.25 mM
[79]
CQDs/Cu2O/GCE GLC amperometry 6 μM–6 mM 6 μM
42 MIP/CDs-CS/GCE GLC DPV 0.5–600 μM 0.09 μM [80]

43 CQDs/AuNPs-GOx/Au GLC amperometry 0.05–2.85 mM 17 μM [81]

[82]
44 GOx-GQD/GCE GLC amperometry 10 μM–3 mM 1.35 μM
[83]
CQDs/AuNPs-GOx/GDAE GLC amperometry 0.16–4.32 mM 13.6 μM
45
46
47
48
and measurement of DA is essential in the clinical medical of the electrode and CDs were able to interact with DA through
49
practice.[84] For this purpose, Jiang et al. loaded the N-doped amine functional groups, as well as CDs was able to reduce
50
carbon quantum dots (NCQDs) on the bare GCE by Nafion(TM) copper hydroxide directly. Additionally, the presence of AA and
51
(NF) solution to form NCQDs/GCE. The proposed electrode was UA had no interference in the measurement of DA, since the
52
utilized for DA detection with broad linear range and low sulfonic groups in NF inhibit anionic AA and UA from accessing
53
detection limit.[85] the electrode surface.[86]
54
In parallel, a cuprous oxide-carbon dots/Nafion (Cu2O-CDs/ Also, layers of the N-CDs and ferrocene@β-cyclodextrin
55
NF) composite film was fabricated for the determination of DA. (Fc@β-CD) were deposited on a GCE. This material showed
56
The Cu2O nanoparticle were able to enhance the conductivity higher catalytic activity towards UA oxidation in comparison
57

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 20 © 2020 Wiley-VCH GmbH

with the unmodified electrode (N-CD and Fc@β-CD,

1
respectively).[87] Furthermore, L-ascorbic acid (L-AA) imprinted
2
polymer film was fabricated on pencil graphite electrodes (PGE)
3
modified with carbon dots (CDs), polyaniline ferrocene-
4
sulfonic acid (PANI-FSA) for separation and measurement of D-
5
ascorbic acid (D-AA) and L-ascorbic acid (L-AA) formed in
6
aqueous and biological samples as reported in Figure 2.[88]
7
Carbon screen printed electrode modified with magnetic
8
nanoparticles and CDs (SPE/MagNP/CDs) has been applied
9
towards determination of NADH as shown in Figure 3.[89] The
10
presented technique introduced a helpful methodology for
11
assembling dynamic modifier agent and the elimination of the
12
magnet leads to effective release of nanoparticles. A broad
13
range of electrochemical sensors for detection of organic redox
14
reaction consisting of DA, UA, AA, EP, and vitamins, utilizing
15
CNDs is listed in Table 2.
16 Figure 3. A picture of carbon screen-printed electrode (SPE) containing a
As mentioned above, CNDs can also improve performance
17 tiny magnet. Adapted from Ref.[89] with permission; Copyright (2017) Wiley-
in drugs investigation due to their excellent characteristics and VCH GmbH.
18
properties such as high surface area, and high electrical
19
conductivity. For example, a novel electrochemical sensor was
20
prepared for doxorubicin hydrochloride (DOX) detection.
21
AgNPs, CDs and rGO were deposited on GCE electrode by a hydroxy-benzene isomers, hydroquinone (HQ), catechol (CC)
22
one-step electrodeposition method as shown in Figure 4.[155] Ag and resorcinol (RS), simultaneously.[157] In parallel, it was also
23
(NH3)2OH concentration affected electrocatalytic activities sig- shown the possibility of using electrostatic assembly strategy in
24
nificantly. It was revealed that when the volume ratio of CDs- order to bind GQDs to the surface of a GCE.[158] As result, the
25
GO (3 : 1, v/v) to Ag (NH3)2OH was fixed to 1 : 1, the best current electrode was applied for concurrent electrochemical
26
electrocatalytic activities were attainable. determination of CC and HQ.
27
Moreover, Zhou et al. introduced gold nanoparticles/amino One of the most environmentally perilous chemicals is
28
acid-functionalized GQDs, (GNs/amino acid-GQD) and its appli- explosive nitro-aromatic compound 2, 4, 6-trinitrotoluene (TNT).
29
cation for electrochemical sensing of p-acetamidophenol Exposure to TNT could lead to pancytopenia, a disorder of the
30
(APAP).[156] They provided twenty kinds of amino acid-GQDs by blood- forming tissues in humans and other mammals.[159,160]
31
one-step simple pyrolysis of citric acid and amino acid which Therefore, a sensitive and selective analytical platform to
32
directly reacted with HAuCl4 to form GNs/amino acid-GQD. detection of TNT is required. It was shown that the best and
33
Also, an electrochemical sensor obtained by using Nafion/ more appropriate electrode material for catalyzing TNT reduc-
34
multi-walled carbon nanotubes/carbon dots/multi-walled car- tion and therefore being able to its detection, is a material that
35
bon nanotubes electrode (NF/MWCNTs/CDs/MWCNTs) with can adsorb TNT on its surface. Zhang et al.[161] prepared an
36
layer by layer (LBL) techniques was built for detecting di- electrochemical sensor for TNT determination based upon
37
38
39
40
41
42
43
44
45
46
47
48
49
50
51
52
53
54
55
56 Figure 2. Creation of L-AA imprinted polymer film on the CDs modified PGE. Adapted from Ref.[88] with permission; Copyright (2015) Elsevier.
57

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 21 © 2020 Wiley-VCH GmbH

1 Table 2. Electrocatalysis of organic redox reaction consists of DA, UA, AA, EP, and vitamins, etc.
2 Modified electrode Target Method Linear range Detection limit Refs.
3
4 CS/N-GQDs@SPCE DA DPV 1–200 μM 0.145 μM [90]
[91]
5 CQDs/MoS2/Mo foil DA CV 0.01–5 μM 0.0090 μM
[85]
NF/NCQDs/GCE DA DPV 0–1 mM 1.0 nM
6 GQDs/NF/GCE DA DPV 5 nM–100 μM 0.45 nM [92]

7 NCDs/GCE DA DPV 50 nM-8 μM 1.2 nM [93]

[94]
8 CDs-CS/GCE DA DPV 0.1–30.0 μM 11.2 nM
[95]
(GQDs-NHCH2CH2NH) DA DPV 1–150 μM 0.115 μM
9 /GCE
10 Au @ CDs-CS/GCE DA DPV 0.01–100.0 μM 0.001 μM [96]
[86]
11 Cu2O-CDs/NF DA DPV 0.05–45.0 μM 1.1 nM
12 NF/rGO-CDs/GCE DA DPV 0.01–450.0 μM 1.5 nM [84]

13 CDs/GCE DA DPV 0.05–2.0 μM 4.6 nM [97]

[98]
14 Bi@C-PTCA/GCE DA DPV 0.2–87.2 μM 0.06 μM
[99]
CD/ERGO/CF microelectrode DA DPV 0.1–100 μM 0.02 μM
15 His-GQD-GMA DA DPV 1.0 nM–80 μM 0.29 nM [100]

16 CDs/GCE DA DPV 0.15 μM–0.15 mM 26 nM [101]

[102]
17 Au NPs-GQDs-NF/GCE DA DPV 2–50 μM 0.84 μM
[103]
GQDs/GCE DA DPV 0.4–100 μM 50 nM
18
19 CDs/IL-graphene/GCE DA DPV 0.1–600 μM 30 nM [104]
[105]
20 SPCE/CQD DA CV 1–7 μM 0.099 μM
[106]
SnO2/PANI/N-GQD/GCE DA DPV 0.5–200 μM 0.42 μM
21 Au-GQDs-NF/GCE DA DPV 2–50 μM 0.84 μM [107]

22 AuNPs-CPE DA DPV 10–600 μM 0.7 μM [108]

[109]
23 OH-GQD@VMSF/Au DA DPV 200 nM–100 μM 120 nM
[110]
TC-GQD/GCE DA DPV 1–500 μM 0.22 μM
24 GQD/SPE DA DPV 0.1–1000.0 μM 0.05 μM [111]

25 Tyr – –
26 [112]
Au-Cu2O/rGO DA DPV 10–90 μM 3.9 μM
27 UA 100–900 μM 6.5 μM
28
[113]
29 CNDs-rGO/GCE DA amperometry 0.08–227 μM 0.03 μM
UA 0.08–328 μM 0.05 μM
30
31 CQDs/GCE DA LSV 0.19–11.81 μM 2.7 μM [114]

32 UA 0.21–13.39 μM 1.3 μM
33 Ru @Au NPs/ PEA DPV 1 pM–1 nM 0.2 pM [115]

34 (C3N4 NTs)-GQDs/(MIP)/GCE
[116]
35 rAu-PtNPs/GQDs/GCE AA SWV 1–100 nM 0.3 nM
DA 1–100 nM 0.3 nM
36 UA 1–100 nM 0.3 nM
37 Trp – –
38 [117]
GQDs or CQDs/BPPGE UA CV – –
39 AA
40 β-CD/CQDs/GCE DA DPV 4–220 μM 0.14 μM [118]

41 UA 0.3–200 μM 0.01 μM
Trp – –
42
43 N-CDs/GCE UA amperometry 20–260 nM 1.3 nM [119]

44 [120]
GQDs/2D-hBN/GCE SER DPV 1 pM–10 nM 0.2 pM
45 NiAl-LDH/CD/GCE ACh amperometry 5–6885 μM 1.7 μM [121]

46 GQDs/GCE HSA CV 0–80 nM – [122]

47 EIS
[89]
MagNP/CQDs/SPE NADH DPV 0.2–5 μM 20 nM
48 MI-PANI-FSA-CDs/PGE L-AA DPV 6.0–165.0 nM 0.001 nM [88]

49 D-AA DPV 6.0–155.0 nM 0.002 nM

[123]
50 MI-PANI-FSA-CDs/PGE D-AA EIS 0.020–0.187 nM 0.00073 nM
L-AA 0.003–0.232 nM 0.00016 nM
51 GQD/AuNP/GCE Que DPV 0.01–6.0 μM 2.0 nM [124]

52 MoS2-CNTs Que DPV 0.002–1.6 μM 0.82 nM [125]

53 @GONRs/HS-CD/N-GQDs/GCE
[126]
MIPs/RGO-CDs/GCE Rutoside DPV 0.01–6.5 μM 3 nM
54 Polyaniline functionalized GQDs/GCE Calycosin DPV 11–352 μM 9.8 μM [127]

55
56
57

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 22 © 2020 Wiley-VCH GmbH

1 Table 2. continued
2 Modified electrode Target Method Linear range Detection limit Refs.
3
[128]
4 TvL/MoS2/GQDs/CSPEs Caffeic acid – 0.38–100 μM 0.32 μM
5 Chlorogenic acid 8.26–100.00 μM 0.19 μM
Epicatechin 2.86–100.00 μM 2.04 μM
6
[129]
7 N-CQD/HPCu2O/ CAF DPV 0.05–43 μM 0.004 μM
8 MWCNT/GCE
[130]
(GQDs/Au)n/GCE MG DPV 0.4–10 μM 0.1 μM
9
[131]
10 AuNPs/GQDs-WS2/GCE MG DPV 0.01–10 μM 3.38 nM
[132]
11 GQD@ NF/AuNP-SPCE Vanillin LSV 13–660 μM 3.9 μM
DPV 0.66–33 μM 0.32 μM
12 GQDs/GNPs/GCE Luteolin DPV 0.01–10 μM 1.0 nM [133]

[134]
13 β-CD-GQD/GCE AA SWV 0.01–170 μM 0.49 μM
14 [135]
GQD-CS/GCE AA SWV 0.7 μM–0.01 mM –
15
[136]
16 Fe3O4 MNPs-GQDs/GCE AA CV 0.1–9 mM –
[137]
17 PPy-BPQDs-MIPs/PEDOTNRs AA DPV 0.01–4 mM 0.0033 mM
/GCE
18 GQD/GCE AC DPV – – [138]

19 AA 25-1350 μM 10 μM
20 [139]
Poly aspartic acid-GQDs/GCE Vitamin B2 DPV – 0.22 μM
21 Vitamin B9 0.1 μM
22 AA 0.1 μM
23 [140]
N-CQD/SnO2/SPCE Vitamin B2 DPV 0.05–306 μM 8 μM
24
[141]
25 Fc-S-Au/C NC/graphene/GCE AA 1.00 μM
26 UA 0.05 μM
DA 0.12 μM
27 AC –
28
[87]
29 Fc@β-CD/N-CD/GCE UA DPV 5–120 μM 0.08 μM
30 UOx-GQDs/GCE UA DPV 1–800 μM 0.3 μM [142]

[143]
31 C-dots engulfed Fe3O4 hybrid UA amperometry 0.01–0.145 μM 0.006 μM
32 nanocomposite/GCE
[144]
RGOQDs/GCE UA DPV 0.024-12.5 μM 0.024 μM
33 X – –
34 G – –
35 [145]
GQDs/Lac/GCE EP CV 1–120 μM 83 nM
36 MIP/g- EP DPV 1 pM–1 nM 0.3 pM [146]

37 C3N4/NCDS(8.0 %)/GCE
[147]
38 GQD-CS/CPE EP SWV 0.36–380 μM 0.3 nM
[148]
CQDs/CPE EP CA 0.02–0.8 and 0.8–20 0.006 μM
39 GCE/GQDs/Lac EP CV 1–120 μM 83 nM [149]

[150]
40 GCE/GQDs/AuNPs NE SWSV 0.5–7.5 μM 0.15 μM
[151]
41 β-CD@N-GQD/FC/GCE Cholesterol DPV 0.5–100 μM 0.08 μM
[152]
PARG-GQDs/GCE MDA DPV 0.06–0.2 μM 0.329 nM
42 PARG-GQDs-CS/GCE MDA DPV – 5.94 nM [153]
[154]
43 L-CQDs or D-CQDs/CPE L-TA LSV – –
44 EIS
D-TA
45
46
47
48
aqueous N-rich carbon dots (CDs). The interaction between CDs Au nano-hybrids. The modified GCE showed desirable electro-
49
and the molecule of interest occurred through an acid-base catalytic activity with significant negative shift in over potential
50
pairing interaction between the electron-rich amino groups of for nitrite oxidation. This occurred because of the synergistic
51
N-rich carbon dots and electron-deficient nitro-aromatic rings effects between carbon dots and AuNPs.[162] The current sensor
52
of TNT. This led to the formation of some TNT-amine complexes was applicable for nitrite sensing in real lake water sample with
53
through the charge transfer. excellent and promising results. A broad range of electro-
54
Zhuang et al. deposited CDs and gold nanoparticles (CD/Au) chemical sensors using CNDs for the detection of small organic
55
nano-hybrids on a GCE and then a Nafion solution was casted molecules consisting in pharmaceuticals and drugs is reported
56
on the top of on the surface of electrode in order to fix the CD/ in Table 3. CNDs containing materials for the electrochemical
57

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 23 © 2020 Wiley-VCH GmbH

Importantly, Ou et al. proposed a platform for electro-

1
chemical enantio-recognition of tryptophan (TRP) isomer via
2
GQDs incorporated into β-cyclodextrin (GQDs/β-CD) film using
3
H-bonds between the oxygen-containing groups on GQDs and
4
the hydroxyl groups on β-CD. The GQDs/β-CD nanocomposites
5
combined the advantages of both GQDs (highly negatively
6
charged from ionization of carboxyl groups of GQDs) and β-CD
7
(chiral microenvironment).[237] The GQDs/β-CD nanocomposites
8
revealed different binding constants for tryptophan enantiom-
9
ers and specifically bonded with L-TRP and constructed
10
inclusion complexes. In this way, this methodology could be
11
used for separation and measurement of tryptophan enantiom-
12
ers (Figure 5).
13
Another application of CDs and GQDs is for the sensing of
14
important bases of DNA and RNA. For instance, an electro-
15
chemical device based on the AgNPs and GQD was used for the
16
determination of guanine (G) and adenine (A).[238] G and A as
17
DNA/RNA bases have an important role in protein biosynthesis
18
and the storage of genetic information.[239] A broad range of
19
Figure 4. The preparation and application of AgNPs-CDs-rGO/GCE sensing electrochemical sensors using CNDs for electrocatalysis of
20
system. Adapted from Ref.[155] with permission; Copyright (2017) Elsevier. amino acids and important bases found in DNA and RNA is
21
listed in Table 5.
22
23
sensing of chemical pollutants, organophosphate insecticide,
24
explosive material and inorganic compound are listed in 2.5.3. Metal Ion Sensing
25
Table 4.
26
L-cysteine (L-Cys) is a hydrophilic non-essential amino acid The sensing of heavy metal ions and other relevant compounds
27
that plays crucial roles like cancer indicator, antioxidant and sensing is essential in order to have a detection tool which is
28
antitoxin in biological systems. One of the most preferred fast, possibly online and certainly low cost and therefore
29
techniques for detection of amino acid, like L-Cys, is the affordable. According to the properties of CDs and GQDs
30
electrochemical methods.[235] Wang et al. modified graphite felt (described above), they have been extensively utilized for the
31
substrate with polypyrrole (PPy) and GQDs@ Prussian blue design of electrochemical sensors to the heavy metal ions
32
nanocomposite (PPy/GQDs@PB/GF) for electrochemical sensing detection. For instance, many oxygen-containing groups on
33
of L–Cys.[236] Firstly, GQDs was adsorbed on GF surface ultrasoni- their surfaces, enhanced opportunities for heavy metal ions
34
cally, then PB nanocomposite hybrid film electro-polymerized deletion. These particular features also have a significant effect
35
on a GQDs modified GF electrode. The reaction rate of the PB on re-oxidizing metals to ions for the stripping analysis.
36
formation was clearly enhanced by the existence of GQDs. Punrat et al. reported[262] polyaniline/graphene quantum
37
Finally, at last, a PPy-film was electrodeposited on the electrode dots (PANI/GQDs) modified screen-printed carbon electrode
38
surface in order to enhance the stability of the device. (SPCE) for Cr (VI) ion determination. Initially, GQDs were
39
40
41
42
43
44
45
46
47
48
49
50
51
52
53
54
55
Figure 5. Preparation of GQDs/β-CD and the separation of TRP isomers using nano-composites. Adapted from Ref.[237] with permission; Copyright (2015)
56 Elsevier.
57

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 24 © 2020 Wiley-VCH GmbH

1 Table 3. . Some applications of CNDs for the determination of small organic molecule such as drugs.
2 Modified electrode Target Method Linear range Detection limit Refs.
3
4 AgNPs-CDs-rGO/GCE DOX CV 10 nM–2.5 μM 2 nM [155]

5
DPV
6 GQD/GCE DOX DPV 0.018–3.60 μM 0.016 μM [163]

7
[164]
8 GQD/GCE DOX DPV 0.018–3.6 μM 0.016 μM
9 PARG-GCE DOX DPV 0.069–1.08 μM 69 nM [165]

10
[166]
11 GQDs-PANI/ZnO-NCs/GCE CPT-11 DPV 0.1–25.0 μM 0.011 μM
5-FU 0.1–50.0 μM 0.023 μM
12 GCE (Fe3O4@GQDs/f-MWCNTs/GCE) L-DOPA DPV 3.0–400 μM 14.3 nM [167]

13
[168]
14 RTIL-GQDs/CPE L-DOPA SWV 0.05–250.0 μM 10.0 nM
[169]
GQDs-IL–CPE MD SWV 0.04–750 μM 0.01 μM
15
16 Apt/AuNPs/GQD-SH/GCE STR EIS 0.1–700 pg/ml 0.033 pg/ml [170]
[171]
17 N-CQD/Cu2O/GCE ASA – 1–907 μM 2 nM
[172]
N-CNDs/CoTAPhPcNPs)/GCE ASA DPV – 0.966 μM
18 IBU 0.419 μM
19 INDO 0.72 μM
20 [173]
GA@O-CQDs/GCE AC DPV 0.001–10 μM 0.38 nM
21
22 GQD/GCE AC DPV 5–80 μM 0.15 μM [138]

23 AA 25–1350 μM 10 μM
24 Fc-S-Au/C NC/graphene/GCE AA – [141]

25 UA –
26 DA –
AC 0.10 μM
27
28 GQD@NF/GCE SMT DPV – 74.8 μg L 1 [174]
[175]
29 GQD-GCE CPFX DPV – 0.1 μM
[176]
PoAP/GQD/GCE LV DPV 0.05–100 μM 10 nM
30 C-dots@CuFe2O4/CPE RIF SWV 0.07–8.0 μM 0.022 μM [177]

31 INZ 0.1–14.0 μM 0.041 μM

[178]
32 NiO/GQD/GCE CLZ DPV 3 nM–1 μM 0.55 nM
[179]
GQDs/NiMnO3/CPE DB DPV 0.08–40.0 μM 0.02 μM
33 GQDs/SPE IPR DPV 1.0–900.0 μM 0.6 μM [180]

34
[181]
35 m-GQDs-MIP@SPCE IFO DPASV 0.25–121.35 ng/mL 0.177 ng/mL
36 CQDs/GCE ETO DPV 0.02–10 μM 5 nM [182]

37
[183]
38 GQD/SPE THEO CV 1.0–700.0 μM 0.2 μM
DPV
39 amperometry
40 ZnO@GQD/PGE 6-MP DPV 0.01–700 μM 5.72 nM [184]
[185]
41 CQDs/NH2 fMWCNT/AgNPs/GCE RIL AdSDPV – –
[186]
DMCCE/GQDs Zlp DPV 0.1–10 μM 0.06 μM
42 MIP/AuNPs/GQD-SH/SPCE SOT DPV 0.1–250 μM 0.035 μM [187]

43 NH2fMWCNT/ZnO/GQDs/GCE PZ DPV 0.063 nM- 0.12 μM 0.01 nM [188]

[189]
44 ds-DANN-IL/GQDs/CPE Topotecan DPV 0.35–100 μM 0.1 μM
[190]
C-dots@MOF/CuF D-PA CV 100–600 μM –
45 L-PA CV 100–600 μM –
46
[191]
47 Au/AgNRs@N-GQDs-MIP/SPCEs HU DPASV 0.55–108.44 ng/mL 0.05 ng/mL
[192]
GQDs-thio/npGCE Cisplatin DPASV 0.2–110 μM 0.09 μM
48 CS/CDs-CTAB/GCE Mesalazine amperometry 0.1–10 μM 0.05 μM [193]

49
50
51
obtained in a bottom-up method from citric acid. Then, in an Moreover, Shao et al. created an electrochemical platform
52
optimized ratio GQDs were mixed with aniline monomer and by CQDs in order to determining Cu2 + in rat brain micro-
53
was added to an electrochemical flow cell for electro-polymer- dialysates directly.[44] In another investigation, an electrochem-
54
ization of the aniline monomer. The PANI/GQDs/SPCE was ical approach was developed using graphene quantum dot-
55
utilized to the determination of Cr (VI) concentration in real modified pencil graphite electrode (GQD/PGE) for copper (II)
56
samples. ions sensing.[263]
57

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 25 © 2020 Wiley-VCH GmbH

1 Table 4. Some application of CNDs for the determination of organic molecules including pollutant, organophosphate insecticide, explosive material, and
inorganic compound.
2
3 Modified electrode Target Method Linear range Detection limit Refs.

4
[157]
5 NF/MWCNTs/CDs/MWCNTs HQ DPV 1–200 μM 0.07 μM
CC 4–200 μM 0.06 μM
6 RS 1–400 μM 0.15 μM
7
[194]
8 CDs-ZnO/MWCNTs HQ DPV 5.0–200 μM 0.02 μM
CC 5.0–200 μM 0.04 μM
9
10 Co3O4-His-GQD/GCE HQ DPV 2 nM–0.8 mM 0.82 nM [195]

11 [196]
CuO-His-GQD/GCE HQ DPV 0.001–40 μM 0.00031 μM
12 Au-GQDs/GCE CC DPV 2–50 μM 0.869 μM [197]

13
[198]
14 Lac-F,N-CDs/GCE CC amperometry 12–450 μM 14.0 nM
15 GQDs/GCE HQ DPV 4.0–600 μM 0.40 μM [158]

16 CC 6.0–400 μM 0.75 μM
17 [199]
CNDs-CS/GCE TCS LSV 10 nM–1.0 mM 9.2 nM
18 MIP-Au/CS-CDS/GCE PAT DPV 1 pM–1 nM 0.75 pM [200]

19 GQDs/AgNP/GCE TBHQ DPV 0.15–300 μM 0.07 μM [201]

[161]
20 CQDs/GCE TNT DPV 5 nM–30 μM 1 nM
[202]
N-GQDs/GCE TNT LSV 1–400 ppb 0.2 ppb
21 (WP6s) and (N-CQDs)/GCE TNT DPV 0.001–20.0 μM 0.95 nM [203]

22
[204]
23 Apt/AgNPs/thiol- TNT DPV 0.001–0.300 pM 0.33 fM
GQD/GCE
24 N-GQD/GCE TNP DPV 1 nM–100 μM 1 nM [205]

25 RF/GQDs/GCE S2O82 amperometry 1.0 μM–1 mM 0.2 μM [206]

[162]
26 NF/CD/AuNPs/GCE NO2 amperometry 0.1 μM–2 mM 0.06 μM
[54]
Ag/C NC/ NO2 DPV 4.00 μM–2.00 mM 0.48 μM
27 PEDOT-CQDs/GCE NO2 amperometry 0.5–1110 μM 88 nM [207]

28 NGQDs @ NCNFs/GCE NO2 DPV 5–3000 μM 3 μM [208]

[209]
29 N-CDs1/GCE NO2 DPV 0.7–6000 μM 0.23 μM
N-CDs2/GCE DPV 0.7–8000 μM 0.23 μM
30 N-CDs3/GCE DPV 0.7–2000 μM 0.23 μM
31 CDs/Fe3O4@g-C3N4/GCE Thiocyanate DPV 0.001–0.900 μM 140 pM [210]

32 (SCN )
[211]
MIPPy/GQDs/GCE BPA DPV 0.1–50 μM 0.04 μM
33 NF/N-CDs/GCE BPA amperometry 0.01–0.21 μM 1.3 nM [212]

34 GQDs-hNiNS/MIECS/GCE BPS DPV 0.1–50 μM 0.03 μM [213]

[156]
35 GNs/Pro-GQD/GCE APAP DPV 0.08–100 μM 0.02 μM
[214]
Pt/carbon black (Vulcan XC-72)-CQDs/NF/GCE CH3OH CV – –
36 amperometry
37 PtCo/GCG/GCE CH3OH CV – – [215]
[216]
38 Au@N-CQDs@Pt/GCE CH3OH CV – –
[217]
Pt nanoflowers decorated -CQD composite CH3OH CV – –
39 Pt/NCQDs-MWCNT/GCE CH3OH CV – – [218]

40 Pt/NCQDs-MWCNT/GCE CH3OH CV – – [219]

[220]
41 GQDs-CS-GCE CH3OH CV – –
β-CD-GQDs-GCE
42 Pt/Lg-CDs/GCE CH3OH CV – – [221]

43
[222]
44 Pd-NPs/RCQDs/GCE CH3OH LSV – –
[223]
GQDs/α-CD/AgNPs/GCE AFM1 LSV 0.015–25 mM 2 μM
45 2-aminobenzyl amine/GQD/SPE Parathion EIS 0.01–106 ng/L 46 pg/L [224]

46 Apt/GA/Glu-GQD/Au/GCE Acetamiprid DPV 1.0 fM–105 fM 0.37 fM [225]

[226]
47 GQD/GCE MY DPV 0.06–50 μM 0.03 μM
CU 0.4–10 μM 0.1 μM
48
49 MIP/PdNPs/BZ/GQDs/ CIT DPV 1–5 nM 0.2 nM [227]

50 GCE
[228]
CDs/GCE Carbendazim DPV 0.1–10 μM 10 nM
51 PAM/GQDs/GCE OPs DPV 10 pM–0.5 μM 6.8 pM [45]

52 C3N4 NTs@ GQDs/(MIP)/GCE CHL SWV 0.01 nM–1 nM 2 pM [229]

[230]
53 CDs/CTAB/CS/GCE 2,4-DCP DPV 0.04–8.0 μM 0.01 μM
[231]
rGQDs/CoPc/GCE N2H4 amperometry 4.4 μM
54 NH2GQDs/CoPc/GCE 8.6 μM
55
[232]
56 PPy/CDs/PB/SAuNPE N2H4 amperometry 0.5–80 μM 0.18 μM
57

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 26 © 2020 Wiley-VCH GmbH

1 Table 4. continued
2 Modified electrode Target Method Linear range Detection limit Refs.
3
[233]
4 GQDs/cobalt mono-carboxy-phenoxy phthalocyanine (complex 1@GQDs)/GCE N2H4 CV 10 μM
5 GQDs/cobalt tetra-carboxy-phenoxy-phthalocyanine 8 μM
(complex 2@GQDs)/GCE 43 μM
6 GQDs/cobalt tetra amino-phenoxy
7 phthalocyanine (complex 3@GQDs)/GCE
[234]
8 AA/CNDs/AuSPE N2H4 CV - -

9
10
11
Lead ion (Pb2 +) and cadmium ion (Cd2 +) are generally wide for is absent for Hg2 +. This result confirmed the synergistic
12
circulatory and spread in groundwater and soil due to the fast integration between AuNPs and GQDs that is significant for
13
development of industries. Li et al., developed an electro- Hg2 + system detection. This sensor was also utilized for Cu2 +
14
chemical sensor for the simultaneous detection of Pb2 + and ions detection through the same procedure done for Hg2 +.
15
Cd2 + by anodic stripping voltammetry; this sensor was con- A list of applications of CNDs based electrochemical sensors
16
formed from the hybrid of N-doped carbon quantum dots- for heavy metal ion sensing is summarized and shown in
17
graphene oxide (NCQDs-GO).[264] Mixing of GO and NCQDs Table 6.
18
achieved the NCQDs-GO hybrid. Then, the synthetized hybrid
19
mixture was dropped onto GCE. Nafion film was used for hybrid
20
stabilization and electrode reproducibility improvement. Abun- 2.5.4. Immunosensing and Aptasensing
21
dant oxygen-containing functional groups and large electro-
22
active surface areas were the properties of both NCQDs and GO Effective and sensitive detection of specific biomolecules like
23
that act as active sites for the heavy metal ions adsorption DNA and protein is significant and extremely important in
24
through electrostatic interaction and affect the sensor sensitiv- clinical analysis. GQDs and CDs represents attractive features to
25
ity. For stripping analysis, homogeneously distribution of recent electrochemical biosensing because of their unique
26
NCQDs onto GO surface played a significant role in re-oxidizing properties, which could increase the electrocatalytic activity and
27
metals into ions. Upon these great results, superior analysis therefore sensing of the immunosensors and aptasensors.[278]
28
performance were obtained for electrochemical detection of Wang and coworkers developed[279] ultrasensitive electro-
29
Pb2 + and Cd2 + utilizing a NCQDs-GO/GCE compared to those chemical immunosensor for Avian leucosis viruses (ALVs-J), a
30
systems applied only GO (GO/GCE) and only NCQDs (NCQDs/ well-known kind of avian retroviruses associated with neoplastic
31
GCE). diseases,[280] by combining GQDs, Fe3O4 nano-spheres and
32
Several dangerous issues including neural and renal prob- apoferritin-encapsulated Cu (Cu-apoferritin) nanoparticles (Fig-
33
lems can be created by mercury ions (Hg2 +) accumulation.[265] ure 6). First, Cu-apoferritin nanoparticles as electroactive probes
34
Hence, detection of such trace amount is of a great challenge. were fixed on Fe3O4@GQDs hybrid, after the sandwich-type
35
Ting et al., synthesized a conjugation of gold nanoparticles assembly between antibody 1 (Ab1) and antigen (ALVs-J), Cu
36
(AuNPs) and GQDs and utilized it through anodic stripping was released from the apoferritin cavity and determined by
37
voltammetry (ASV) method for sensitive electrochemical heavy DPV. In fact, GQDs led to the expansion of electrode surface,
38
metal ions determination (Cu2 + and Hg2 +).[266] Firstly, they used thus more Cu-apoferritin nanoparticles were loaded on the
39
the chemical reduction of gold chloride solution for cyste- surface as electroactive probes. As a result, electrochemical
40
amine-capped AuNPs synthesis.[267] Then, GQD solution was signal was enhanced importantly.
41
added to the result cysteamine-AuNPs, followed by the addition Importantly, a novel immunosensor based on poly L-
42
of EDC. After that, the sediment was obtained by solution cysteine (P-Cys) as conductive matrix and GQDs/gold nano-
43
centrifugation; to completely remove the excess GQDs, this step particles (GNPs) as dual amplification elements was designed
44
was repeated for 5 times and then deionized water was used for highly sensitive determination of tumor suppressor protein
45
for re-dispersing. The obtained GQD-AuNPs was drop onto the p53 antigen.[281] In this immunosensor, electrochemical techni-
46
surface of electrode followed by dropping of Nafion solution ques were utilized to immobilized P-Cys-GQDs/GNPs nano-
47
onto the modified electrode for layer protection and proton composite onto a gold electrode surface. Particularly, cyclic
48
exchange membrane. The negatively charged hydroxyl and voltammetry technique was used for the electropolymerization
49
carboxyl groups of GQDs and the initially applied negative of L-Cys and then electrodeposition of GQDs onto Au electrode
50
voltage ( 0.2 V for 120 s) caused to pre-concentration Hg2 + modified with P-Cys. Prepared transducer gave an extensive
51
ions onto the electrode surface.[268] It was suggested that Hg2 + surface area to fix a huge number of the anti-p53. So, the
52
and carboxyl groups could interact together in R-COO-(Hg2 +)- sensitivity of the sensor was improved using the proposed
53
OOC-R form.[269] Furthermore, AuNPs shown great affinity to Hg2 modifier.
54 + [270]
and electrode modified with AuNPs gives a much weaker Synthesized CDs are extremely effective for immobilization
55
oxidation peak compared to electrode modified with GQD- of unmodified oligonucleotides in electrochemical DNA sensor
56
AuNPs, whereas GCE did not demonstrate any oxidation peak
57

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 27 © 2020 Wiley-VCH GmbH

1 Table 5. A list of applications of CNDs based electrochemical sensors for amino acids sensing and important DNA/RNA bases.
2 Modified electrode Target Method Linear range Detection limit Refs.
3
4 MIB/Au/ERGQD/GCE GSH DPV 0.03–1300.0 μM 9 nM [240]
[241]
5 CTAB-AuNRs-GQDs/GCE GSH amperometry 0.5–7 μM 0.23 μM
6 GQDs/β-CD/GCE TRP isomers DPV – – [237]

7
[242]
8 N-CDs/β-CD/GCE TRP isomers DPV
9 Fe3O4 MNP-GQDs/GCE L-Cys DPV 0.01–100 μM – [243]

10 L-Tyr 0.09–230 μM
11 L-Asp 1–50 μM
L-Phe 0.5–650 μM
12 FF/GQDs)/CS/CTAB TRP DPV – – [244]

13 enantiomers
[245]
14 GQDs-CS/GCE TRP enantiomers DPV – -
15 GQDs- TA/GCE TRP enantiomers DPV – – [246]

16 NH2-GQDs/β-CD/GCE TRP enantiomers DPV 1.0–30.0 μM 0.65 μM [247]

[248]
17 Fe3O4 MNP-GQDs/GCE L-TRP DPV 0.08–150 μM 0.08 μM
[249]
CS-CNDs/GCE TRP DPV up to 90 μM 90 nM
18 β-CD/CQDs/GCE DA DPV – – [118]

19 UA – –
20 TRP 5–270 μM 0.16 μM
21 rAu-PtNPs/GQDs/GCE AA SWV – – [116]

22 DA – –
23 UA – –
TRP 1–100 nM 0.3 nM
24
25 GQDs/β-CDs/GCE L-Tyr CV 6–100 μM 6.07 nM [250]

26 D-Tyr 0.1–1.0 mM 0.103 μM

[251]
Β-CD-GQD/GCE L-Tyr DPV 0.1–1.5 μM 100 nM
27 GQD-RuCl3/CCE L-Tyr amperometry 1–937 μM 0.23 μM [252]

28 GQD/SPE DA DPV – – [111]

29 Tyr 1.0–900.0 μM 0.5 μM

[253]
CS-GQD-GCE L-Cys CV – –
30 DA
31 UA
32 L-Tyr
L-Phe
33 AA
34 Poly (alizarin yellow R)/CQD/GCE L-Cys CV 0.3–7.2 μM 90 nM [254]

35 amperometry
[255]
β-CD-GQD/GCE L-Cys DPV 0.01–2 mM –
36 PPy/GQDs@PB/GF L-Cys amperometry 0.2–1000 μM 0.15 μM [236]

37 rCDs-CS/PB/ITO L-Cys amperometry – – [256]

[257]
38 Poly-L-cysteine/GQD/GNPs/GCE L-P DPV 0.5 nM–10 mM 0.1 nM
[258]
Poly(aspartic acid)-GQDs/GCE Taurine DPV – 0.001 mM
39 AgNPs/GQD/GCE G DPV 0.015-430 μM 0.01 μM [238]

40 A 0.015–390 μM 0.012 μM
[259]
41 CQDs/PAPox/GCE G CV 1.0–65 μM 0.51 μM
A DPV 2.0 to 70 μM 0.39 μM
42 PBG/CQDs/GCE G CV 0.50–142 μM 0.016 μM [260]

43 A DPV 0.30 ~ 130 μM 0.026 μM

[144]
44 RGOQDs/GCE UA DPV 0.024–12.5 μM 0.024 μM
X – –
45 G – –
46 GOQDs/f-MWCNTs/PGE G LSV 0.2–180.0 μM – [261]

47 X 0.2–150.0 μM
A 0.5 to 200.0 μM
48 HPX 0.5–180.0 μM
49
50
51
52
immobilization, in contrast to carbon nanotubes that required Through hydrogen bonding and π-π stacking interactions of
53
chemically modified oligonucleotides. the DNA bases, HP1 could be straightly adsorbed onto the CDs/
54
García-Mendiola et al.[282] proposed a biosensing platform AuSPE modified electrode.[283] Finally, HP1/CDs/AuSPE electro-
55
for gene mutation detection based on CDs/AuSPEs modified by chemical DNA biosensors were utilized for accurate and
56
25-mer sequence of helicobacter pylori bacterium (HP1). selective hybridization monitoring. Safranine (SAF) was used as
57

1 Table 6. A list of applications of CNDs based electrochemical sensors for heavy metal ion and related component sensing.
2 Modified electrode Target Method Linear range Detection limit Refs.
3
4 PANI/GQDs/SPCE Cr4(VI) LSV 0.1–10 mg L 1
0.097 mg L 1 [262]

5 [44]
AE-TPEA/CDs/APTMS/GCE Cu (Π) DPASV 1–60 μM 100 nM
6 GQDs/GCE Cu (Π) DPASV – 0.3 nM [271]

7
[264]
8 NCQDs-GO/GCE Cd(Π) ASV 11.24—11241 μg/L 7.45 μg/L
Pb(Π) 20.72–10360 μg/L 1.17 μg/L
9 GQDs/AuNPs/GCE Hg(Π) ASV – 0.02 nM [266]

10 Cu (Π) 0.05 nM
[109]
11 OH-GQD@VMSF/ITO Hg(Π) DPASV 1.0 nM-0.5 μM 9.8 pM
OH-GQD@VMSF/ITO Cu (Π) 1.0 nM-1.5 μM 8.3 pM
12 NH2-GQD@VMSF/ITO Cd(Π) 1.0 μM-20.0 μM 4.3 nM
13 CS/GQDs/GCE Zn(Π) SWASV 50–450 μg/l 8.84 μg/L [272]

14 Cd(Π) 1.9 μg/L

Pb(Π) 3.10 μg/L
15 GQDs/GCE Pb(Π) DPASV 0.8–10 μM 7 nM [273]

16
[263]
17 GQD/PGE Cu (Π) SWASV 0.05–4 nM 0.012 nM
[274]
GQDs/graphene/GCE Cu (Π) DPASV 0.015–8.775 μM 1.34 nM
18 GNPs/SPGE Pb(Π) SWASV 20–200 ppb 2.2 ppb [275]

19 Cu (Π) 20–300 ppb 1.6 ppb

[276]
20 CS-CNDs-E. coli@TH/GCE Cd(Π) amperometry – –
Cu(Π)
21 Pb(Π)
22 Zn(Π)
[277]
23 ERGQDs/GE U SWV 23.4–345.8 ppb 2 ppb
24
25
26
an electrochemical redox probe in order to bind to double biosensors. However, despite an increasing number of pub-
27
stranded DNA (dsDNA) specifically.[284] lished studies, the application of the mentioned nanoparticles,
28
In another example, an aptasensor is designed for hepatitis is still at the initial stage and further improvements need to be
29
C virus (HCV) core antigen measurement. For this purpose, the pursued in order to finally reach large scale utilization and
30
aptamer was fixed onto the GQDs through non-covalent commercialization. One way for improving the electronic and
31
interactions.[285] Moreover, proposed aptasensor was also used electrocatalytic characteristics of CDs and GQDs is chemical
32
for HCV core antigen sensing in human serum as real sample doping which also amends their electrical and thermal proper-
33
with good precision and accuracy. ties. Moreover, it is also feasible and envisioned to combine
34
As mentioned above, CDs can be utilized for reducing Au +, other types of nanomaterials with them to form nano-
35
Ag , Cu2 + or graphene oxide to Au,[286] Ag,[287] Cu2O[86] and
+
composites. This leads to diverse properties and features in a
36
reduced graphene oxide,[288] respectively. According to this single novel material.
37
mentioned property, CDs can be utilized to synthesize Pd- CNDs have attracted considerable interest in electrochem-
38
Au@CDs nanocomposite. Firstly, Pd-Au@CDs nanocomposite ical analysis because of the significant electron transfer,
39
solution was dropped on the GCE with the intention of chemical stability, low toxicity, biocompatibility, and large
40
preparing Pd-Au@CDs/GCE. Then, single-stranded probe DNA specific active area for load various molecules on their surfaces.
41
(S1) was fixed by a covalent reaction by the use of EDC/NHS as Furthermore, they play an important role in the reduction of
42
linking reagents (Figure 7). Finally, S1/Pd <-Au@CDs/GCE was novel metal nanoparticles, including Au, Ag, Pd and Pt, to
43
used as a biosensor for target DNA monitoring.[289] The electro- produce nanoparticles/GQDs or nanoparticles/CDs besides this
44
chemical biosensor was utilized for colitoxin DNA sensing in operation doesn’t need any other reducing agent, surfactant or
45
human serum with excellent reproducibility and stability. toxic materials. Also, CNDs are extremely effective for immobi-
46
Applications of CNDs based electrochemical sensors for detec- lization of unmodified oligonucleotides on the electrode surface
47
tion of protein and DNA/RNA are listed in Table 7. via non-covalent interactions. As a matter of fact, the richness
48
of hydrophilic edges as well as hydrophobic plane enhances
49
the oligonucleotides absorption. Furthermore, CNDs improve
50
3. Perspective and Future Applications the efficient adsorption of heavy metal via electrostatic
51
interaction.
52
This article summarized the most recent advancements and Importantly, the emergence of CNDs can be used to reduce
53
developments in electrochemical sensing and biosensing, the substantial cost of sensors/biosensors by substituting
54
dependent on CNDs and their typical applications. It has been expensive noble metal substrates with low-cost carbon materi-
55
attempted to gather a comprehensive collection of all applica- als. In fact, in many aspects, they can replace the well-known
56
tions of CNDs in the construction of electrochemical sensors or quantum dots based on metal chalcogenides as a result of their
57

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4
5
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8
9
10
11
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13
14
15
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17
18
19
20
21
22
23
24
25
26
27
28
29
30
31
32
33
34
35
36
Figure 6. A, B) Illustration of electrochemical immunosensor for avian leucosis virus subgroup J. detection. C) DPV responses of the immunosensor with
37
increasing ALVs-J concentrations under the optimized conditions. D) Calibration curve. Adapted from. Ref.[279] with permission; Copyright (2013) Elsevier.
38
39
40
41
42
43
44
45
46
47
48
49
50
51
52
53 Figure 7. Application of CDs from banana peels for preparing Pd-Au@CDs modified electrode to detect colitoxin DNA. Adapted from Ref.[289] with permission;
54 Copyright (2017) Elsevier.
55
56
57

1 Table 7. A list of applications of CNDs based electrochemical sensors for protein and DNA/RNA sensing.
2 Modified electrode Target Method Linear range Detection limit Refs.
3
4 Fe3O4@GQDs/Cu-apoferritin/Ab2/BSA/Ab1/GCE ALVs-J DPV 102.08–104.50 TCID50/mL 115 TCID50/mL [279]

5 [281]
Au/GQDs/PCys/AuNP Streptavidin-HRP/BSA/Ab/BSA/p53 p53 SWV 0.0244–0.369 pM 12.1 fM
6 PAMAM-CDs/Au nanocrystal AFP DPV 100 fg/mL–100 ng/mL 0.025 pg/mL [19]

7
[290]
8 (ssDNA-2 or thrombin)/ssDNA-1/GQDs/PG target molecules (ssDNA-2 DPV 200–500 nM 100 nM
or thrombin)
9 Ab/GQD/SPE cMyo EIS 0.01–100 ng/mL 0.01 ng/mL [291]

10 HP1/CDs/AuSPE HP1 DPV 0.001 to 20 μM 0.16 nM [282]

[292]
11 BSA/Ab-VD2/CD-CH/ITO Vitamin D DPV – –
12 BSA/anti-CEA/PtPd/N-GQDs@Au/GCE CEA amperometry 5 fg/mL–50 ng/mL 2 fg/mL [293]

13
[294]
14 MB-substrate/GQDs-IL-NF/GCE CEA DPV 0.5 fg/mL–0.5ng/mL 0.34 fg/mL
[295]
GQDs/target DNA/NH2-DNA/capture DNA/GE miRNA-155 amperometry 1 fM–100 pM 0.14 fM
15
16 BSA/Apt/GQD/GCE HCV EIS 10–400 pg/mL 3.3 pg/mL [285]
[296]
17 AgNPs/GQD-SH/anti-HCV HCV DPV 0.05 pg/mL–60 ng/mL 3 fg/mL
[297]
S1/GQD/GCE HBV-DNA DPV 10–500 nM 1 nM
18
19 S1/Pd-Au@ CDs/GCE Colitoxin DNA DPV 0.5 fM–0.1 nM 0.0182 fM [289]
[298]
20 S3/ZnFe2O4/GQDs/S2/S1/GrS-Pd NWs/GCE DNA hybridization DPV 0.1 fM–5 nM 0.062 fM
21 Au/MPA-lipid-CD-AgNPs DNA hybridization EIS 10 16 to 10 11 M 10 16 M [299]

22 CQDs@PDA@PtNCs-NGR-3/GCE 8-OH-dG DPV 0.013–16.68 μM 0.45 nM [300]

23 [301]
CQD/PDDA/MWCNT/GCE Lysozyme DPV 50 fM–10 nM 12.9 fM
24 S1/GNDs-Zeo/PAD S. aureus DPV – 0.1 nM [302]

25 anti-PSA/P-Cys/GQDs/GNPs PSA amperometry 2-9 pg/·mL 1.8 pg/mL [303]

[304]
26 Fe3O4@GQD/f-MWCNTs/GCE P4 DPV 0.01–3.0 μM 2.18 nM
[305]
GQDs/PSSA/GCE E2 DPV 0.001–6.0 μM 0.23 nM
27 P4 0.001–6.0 μM 0.31 nM
28 Anti-AXL antibody/(fGQDs)/SPCEs. AXL DPV – 0.5 pg/mL [306]

29 S1/CS/AuPd NWs/D-GQDs-GMA/GCE Ara h 1 DPV 1 × 10 22–1 × 10 17

M 4.7 10 23 M [307]

30 GQD/HRP/auxiliary DNA/MCH/capture DNA/GE M.SssI amperometry 1–40 U/mL 0.3 U/mL [308]

31 MTase
32 PAMAM/GQD/AuSPE cTnI DPV 10 6–10 ng/ml 20 fg/mL [309]

[310]
CDs@ZrHf-MOF/Au HER2 EIS 0.0001–10 ng/ml 30 fg/mL
33 DPV 0.0001–10 ng/ml 19 fg/mL
34 MWCNTs/GQDs-HRP-DAb-IL13sRα2- IL-13 receptor 2 amperometry 2.7–100 ng/mL 0.8 ng/mL [311]

35 BCAb-Strep/p-ABA/SPCE
36 rGO-MWCNT/CS/CQD/GCE Lysozyme DPV 20 fM–10 nM 3.7 fM [312]

37 EIS 10 fM–100 nM 1.9 fM

38 [313]
GQDs/MWCNTs -HRP-DAb/SPCE IL-13Rα2 amperometry 4.92–100 ng/mL 1.4 ng/mL
39 CDH-17 0.11–10 ng/mL 0.03 ng/mL
40
41
42
43
excellent biocompatibility and low-cost facile preparation Conflict of Interest
44
techniques. To further significantly reduce the cost of the
45
starting materials and increase the scale of CND production, a The authors declare no conflict of interest.
46
one-step electrochemical approach utilizing low-cost and read-
47
ily available graphite as a carbon source should be pursued. Keywords: analytical applications · carbon nanodots ·
48
According to the significant properties of CNDs, there is an electrochemical sensors · biosensors · target analytes
49
enormous advancement space for utilization of these modifiers
50
as a low cost, perfect and ideal sensor material. One idea for the
51
future research could be focused on appropriate carbon source
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Paul, H. Lee, K.-H. Kim, A. Deep, Biosens. Bioelectron. 2016, 86, 548.
28 [292] T. Sarkar, H. Bohidar, P. R. Solanki, Int. J. Biol. Macromol 2018, 109, 687. Manuscript received: September 19, 2020
29 [293] Y. Yang, Q. Liu, Y. Liu, J. Cui, H. Liu, P. Wang, Y. Li, L. Chen, Z. Zhao, Y. Revised manuscript received: November 12, 2020
Dong, Biosens. Bioelectron. 2017, 90, 31. Accepted manuscript online: November 16, 2020
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ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 19 © 2020 Wiley-VCH GmbH

4 CQDs/GCE H2O2 amperometry 100 nM–1 mM 300 nM [52]

13 GQDs/AuNPs-PDA-GQD/ITO H2O2 amperometry 0.1–20000 μM 5.8 nM [57]

25 Cyt c/CD-MWCNTs/GCE H2O2 amperometry 2–30 μM 1.02 μM [67]

31 AuNPs@CDs/GCE H2O2 amperometry – – [71]

40 GQDs/CoNiAl-LDH/CPE GLC amperometry 0.01–14.0 mM 6 μM [77]

43 CQDs/AuNPs-GOx/Au GLC amperometry 0.05–2.85 mM 17 μM [81]

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 20 © 2020 Wiley-VCH GmbH

with the unmodified electrode (N-CD and Fc@β-CD,

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 21 © 2020 Wiley-VCH GmbH

7 NCDs/GCE DA DPV 50 nM-8 μM 1.2 nM [93]

13 CDs/GCE DA DPV 0.05–2.0 μM 4.6 nM [97]

16 CDs/GCE DA DPV 0.15 μM–0.15 mM 26 nM [101]

22 AuNPs-CPE DA DPV 10–600 μM 0.7 μM [108]

46 GQDs/GCE HSA CV 0–80 nM – [122]

49 D-AA DPV 6.0–155.0 nM 0.002 nM

52 MoS2-CNTs Que DPV 0.002–1.6 μM 0.82 nM [125]

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 22 © 2020 Wiley-VCH GmbH

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 23 © 2020 Wiley-VCH GmbH

Importantly, Ou et al. proposed a platform for electro-

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 24 © 2020 Wiley-VCH GmbH

31 INZ 0.1–14.0 μM 0.041 μM

43 NH2fMWCNT/ZnO/GQDs/GCE PZ DPV 0.063 nM- 0.12 μM 0.01 nM [188]

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 25 © 2020 Wiley-VCH GmbH

19 GQDs/AgNP/GCE TBHQ DPV 0.15–300 μM 0.07 μM [201]

25 RF/GQDs/GCE S2O82 amperometry 1.0 μM–1 mM 0.2 μM [206]

28 NGQDs @ NCNFs/GCE NO2 DPV 5–3000 μM 3 μM [208]

34 GQDs-hNiNS/MIECS/GCE BPS DPV 0.1–50 μM 0.03 μM [213]

40 Pt/NCQDs-MWCNT/GCE CH3OH CV – – [219]

46 Apt/GA/Glu-GQD/Au/GCE Acetamiprid DPV 1.0 fM–105 fM 0.37 fM [225]

52 C3N4 NTs@ GQDs/(MIP)/GCE CHL SWV 0.01 nM–1 nM 2 pM [229]

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 26 © 2020 Wiley-VCH GmbH

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 27 © 2020 Wiley-VCH GmbH

16 NH2-GQDs/β-CD/GCE TRP enantiomers DPV 1.0–30.0 μM 0.65 μM [247]

26 D-Tyr 0.1–1.0 mM 0.103 μM

28 GQD/SPE DA DPV – – [111]

29 Tyr 1.0–900.0 μM 0.5 μM

37 rCDs-CS/PB/ITO L-Cys amperometry – – [256]

43 A DPV 0.30 ~ 130 μM 0.026 μM

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 28 © 2020 Wiley-VCH GmbH

14 Cd(Π) 1.9 μg/L

19 Cu (Π) 20–300 ppb 1.6 ppb

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 29 © 2020 Wiley-VCH GmbH

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 30 © 2020 Wiley-VCH GmbH

10 HP1/CDs/AuSPE HP1 DPV 0.001 to 20 μM 0.16 nM [282]

22 CQDs@PDA@PtNCs-NGR-3/GCE 8-OH-dG DPV 0.013–16.68 μM 0.45 nM [300]

25 anti-PSA/P-Cys/GQDs/GNPs PSA amperometry 2-9 pg/·mL 1.8 pg/mL [303]

29 S1/CS/AuPd NWs/D-GQDs-GMA/GCE Ara h 1 DPV 1 × 10 22–1 × 10 17

37 EIS 10 fM–100 nM 1.9 fM

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 31 © 2020 Wiley-VCH GmbH

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ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 33 © 2020 Wiley-VCH GmbH

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 34 © 2020 Wiley-VCH GmbH

ChemElectroChem 2021, 8, 15 – 35 www.chemelectrochem.org 35 © 2020 Wiley-VCH GmbH

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