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Talanta 233 (2021) 122546

Contents lists available at ScienceDirect

Talanta
journal homepage: www.elsevier.com/locate/talanta

Electrochemiluminescence aptasensor for lincomycin antigen detection by


using a SnO2/chitosan/g-C3N4 nanocomposite
Xing-Pei Liu, Bo Huang, Chang-Jie Mao *, Jing-Shuai Chen, Bao-Kang Jin
Key Laboratory of Structure and Functional Regulation of Hybrid Materials (Ministry of Education), Key Laboratory of Chemistry for Inorganic/Organic Hybrid
Functionalized Materials of Anhui Province, Key Laboratory of Functional Inorganic Materials of Anhui Province, School of Chemistry & Chemical Engineering, Anhui
University, Hefei, 230601, PR China

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

Keywords: In this paper, hydrothermal method was used for the synthesis of SnO2 quantum dots (QDs). The prepared SnO2
Aptasensor QDs have a uniform particle size distribution and good electrochemiluminescence (ECL) property. Then the
Electrochemiluminescence prepared SnO2 QDs was combined with graphene-like carbon nitride (g-C3N4) through chitosan to form SnO2/
Lincomycin
chitosan/g-C3N4 nanocomposite and used for detecting the lincomycin. The characteristics of SnO2/chitosan/g-
Energy transfer
C3N4 nanocomposite were presented by transmission electron microscopy (TEM), X-ray diffraction (XRD) and
energy dispersive spectroscopy (EDS), and the analytical results proving that the nanocomposite was prepared
successfully. In this strategy, the SnO2/chitosan/g-C3N4 nanocomposite was acted as the substrate of aptasensor.
Then, SH-DNA (aptamer DNA) was assembled on the surface of electrode, after 6-mercaptohexanol (MCH)
blocked the unbound sites of the electrode surface, ferrocene-DNA (Fc-DNA) was incubated on the electrode
surface through base complementation with aptamer DNA. In the absence of lincomycin, due to the low con­
ductivity of Fc-DNA and the photo-excited energy electron transfer, the ECL signal was quenched. In the presence
of lincomycin, the aptamer DNA was specific binding with lincomycin, and ferrocene-DNA (Fc-DNA) was de­
tached from the surface of aptasensor electrode, generating an obviously enhancement of ECL signal. To ensure
the accuracy of the data, each electrode runs continuously for 3600 s. Under optimal experimental conditions,
the detection range of the aptasensor was 0.10 ng mL− 1 - 0.10 mg mL− 1, and the detection limit was 0.028 ng
mL− 1. In addition, the aptasensor has good stability and reproducibility, and also provided a hopeful device for
all kinds of other protein target.

1. Introduction standard analytical techniques in many countries, most of them are


limited because of their expensive instruments, time consuming, com­
Lincomycin is an antibiotic against bacteria, which mainly inhibits plex practical operation and low sensitivity. Therefore, a simple and
the synthesis of bacterial cell proteins, and has remarkable effect on efficient method is required for supervising lincomycin with high
anaerobic bacteria, staphylococcus aureus and pneumococcus. Up to sensitivity.
now, lincomycin has been extensively used in feed and animal products Electrochemiluminescence (ECL), an ultrasensitive analytical tech­
industry, which has led to concern that foods derived from animals nique, which has been widely used in biological analysis and other fields
could be contaminated with antibiotics, and this has become a solemn because of its inherent superiorities, for instance, low cost, high sensi­
public health problem around the world [1–3]. Therefore, it is essential tivity, wide dynamic range, simple format and so on [8,9]. As the major
to detect and monitor residual lincomycin in dairy products and meat component of ECL sensor, ECL luminophores are crucial for the per­
foods. At present, many classic methods have been developed for ana­ formances of ECL sensor. Compared with conventional ECL lumino­
lysing and detecting lincomycin, such as: high performance liquid phores (for example, luminol and Ru(bpy)2+ 3 ), g-C3N4 has inherent
chromatography (HPLC) [4], electrochemistry [5], microbiological advantages, such as good biocompatibility, large specific surface area
assay [6], fluorescence [7]. Although these methods are relatively ac­ [10–12], and it is widely favored by researchers in the construction of
curate in the determination of lincomycin and have been used as ECL sensors. However, the ECL stability of g-C3N4 decreased obviously

* Corresponding author.
E-mail address: maochangjie@sina.com (C.-J. Mao).

https://doi.org/10.1016/j.talanta.2021.122546
Received 5 February 2021; Received in revised form 13 May 2021; Accepted 19 May 2021
Available online 4 June 2021
0039-9140/© 2021 Elsevier B.V. All rights reserved.
X.-P. Liu et al. Talanta 233 (2021) 122546

with the raising cathode potential, and accompanied by the phenome­ 2. Experiment
non of electrode passivation, which limits the application of g-C3N4
partly. Therefore, some modifications are necessary for g-C3N4 to 2.1. Materials and reagents
improve the performance and expand its application range [13,14].
SnO2 quantum dots, as a typical representation of metal oxide semi­ The materials and reagents were provided in Supplementary
conductor nanomaterials, have absorbed extensive attention own to Material.
their low cost, environmental friendliness, and excellent optoelectronic The sequences of all of the DNA oligonucleotides used in this work
performance, at the same time, they also exhibit suitable band gap are given as follows:
(~3.6 eV) and high stability [15–17]. Chitosan, one kind of biopolymer, SH-DNA(aptamerDNA):5′ –SH–(CH2)6-CGCGTGATGTGGTCGATGC­
riched in amino and hydroxyl, and possess remarkable affinity and GATACGGTGAGTCGCGCCACGGCTACACACGTCTCAGCGA-3′
permeability. Therefore, in this paper, g-C3N4 was served as an ideal Ferrocene-DNA(FcDNA):5′ -
carrier, chitosan was used as stabilizer and binder, and carried plentiful TCGCTGAGACGTGTGTGTAGCCGTGGCGCGACTCACCGTATCGCATC­
SnO2 QDs on the g-C3N4 surface to form SnO2/chitosan/g-C3N4 nano­ GACCACATCACGCG–(CH2)6–Fc-3′
composite. Contradistinguished with whole g-C3N4, the ECL strength
and stability of nanocomposite improved significantly. Therefore, in this 2.2. Synthesis of SnO2 QDs
work, SnO2/chitosan/g-C3N4 nanocomposite was used to establish a
sensitive ECL aptasensor. The prepared of SnO2 QDs was according to the previous report with
In this article, a convenient and new type ECL aptasensor was suc­ some modifications (seen in Supporting Information) [18–20].
cessfully established for detecting lincomycin with high sensitivity. It
can be seen from Scheme 1, the SnO2/chitosan/g-C3N4 nanocomposite 2.3. Preparation of SnO2/chitosan/g-C3N4 nanocomposite
was modified on the bare electrode (GCE) surface. Then, the aptamer
DNA was assembled on the surface of SnO2/chitosan/g-C3N4 nano­ Firstly, 100 mg of prepared g-C3N4 was added into 100 mL deionized
composite through the Sn–S bond. After 6-mercaptohexanol covered the water and ultrasonicated for 4 h. After the precipitate was removed,
unbound sites of the electrode surface, Fc-DNA was introduced and excess chitosan (0.5 wt%) was droped into the homogeneous suspension
combined with aptamer DNA through base complementation. For liquid. After shaking thoroughly, the uniform mixed liquor was purified
monitoring lincomycin, the different concentrations of lincomycin were by centrifuging and the chitosan/g-C3N4 with positively charged was
specific binding with aptamer DNA, and Fc-DNA was released from the obtained. Then, the obtained chitosan/g-C3N4 composite was dispersed
electrode surface, generating an obviously enhanced ECL signal. The in deionized water again with a fixed concentration of 1 mg/mL. At last,
proposed ECL aptasensor exhibited a selective and sensitive detection 1 mg/mL chitosan/g-C3N4 mixture mixed with 5 mg/mL SnO2 QDs so­
for lincomycin and was looked forward to be used in actual sample lution by sonicating for 30 min at a volume ratio of 2:1. The resulting
analysis. product was SnO2/chitosan/g-C3N4 nanocomposite.

Scheme 1. The steps involved in fabrication of the electrochemiluminescence aptasensor.

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X.-P. Liu et al. Talanta 233 (2021) 122546

2.4. Fabrication of the ECL aptasensor and lincomycin analysis electron microscopy (TEM) and high resolution transmission electron
microscopy (HRTEM). It can be seen from Fig. 2A, pure g-C3N4 exhibits a
Firstly, 10 μL of prepared SnO2/chitosan/g-C3N4 nanocomposite was thin and transparent stratified structure. It can be seen from Fig. 2B, the
dropped on the aptasensor electrode and dried naturally. Next, the g-C3N4 surface was uniformly covered with SnO2 QDs and the surface
aptamer DNA which has been pretreated by tris(2-carboxyethyl)- became rough. Fig. 2C displays the HRTEM picture of SnO2/chitosan/g-
phosphine (TCEP) was introduced and aptasensor electrode was incu­ C3N4, it can be seen that, SnO2 QDs exhibited obvious lattice fringes on
bated overnight at 4 ◦ C. After the unbound sites were covered with 15 μL the g-C3N4 surface with an average particle size of about 4.1 nm, which
of MCH, 15 μL of Fc-DNA was incubated at room temperature for 60 min in accord with the lattice plane (110) of SnO2. The chemical composition
to form an aptasensor for lincomycin detection. of the SnO2/chitosan/g-C3N4 nanocomposite was carried out by Energy
For monitoring lincomycin, different concentrations of lincomycin dispersive spectroscopy (EDS). It can be seen from Fig. 2D, the peaks
(15 μL) was incubated on the generating aptasensor electrode surface relevant to N, C, Sn and O elements were observed. The rest of peaks
and washed with Tris-EDTA (TE) buffer. At last, the prepared aptasensor come from the base of the sample tray.
was used to detect lincomycin. Scheme 1 exhibits the entire assembly
processes of the proposed ECL aptamer sensor. 3.2. Electrochemiluminescence behavior and mechanism

2.5. Electrochemiluminescence determination For purpose of proving the superiority of SnO2/chitosan/g-C3N4, the
ECL and cyclic voltammetry (CV) of different materials were acquired
The ECL intensity of the electrode was carried out in 5 mL of 0.1 M and compared under the working potential ranging from − 1.45 to 0 V
phosphate buffered saline (PBS) (0.1 M K2S2O8 and 0.1 M KCl were and the voltage of the photomultiplier tube was set as 400 V. As shown
contained) with a working potential − 1.45 V–0 V, and the voltage of the in Fig. 3A, the ECL signal of SnO2 QDs was as weak as 380 a.u. (curve
photomultiplier tube of the instrument was set to 400 V. Then, ECL black in Fig. 3A), which was produced by the excited state of SnO2 QDs.
signal was used to analyze the concentrations of lincomycin. The ECL signal of g-C3N4 was relatively high (curve red in Figs. 3A and
4215 a.u.), but the stability was poor. For SnO2/chitosan/g-C3N4
3. Results and discussion nanocomposite, the ECL signal was as high as 13,524 a.u. (curve blue in
Fig. 3A). At the same time, the cycling stability of SnO2, g-C3N4 and
3.1. Characterization of SnO2/chitosan/g-C3N4 nanocomposite SnO2/chitosan/g-C3N4 were tested. As shown in Fig. 3B–D, the ECL
signals of SnO2 and g-C3N4 were unstable, simultaneously, the ECL
Fig. 1 displays the X-ray powder diffractions (XRD) spectrogram of signal of g-C3N4 exhibited a significant decrease. After the g-C3N4 sur­
SnO2, g-C3N4 and SnO2/chitosan/g-C3N4 nanocomposite, respectively. face was uniformly covered with SnO2 QDs, a higher and more stable
It can be seen from Fig. 1, SnO2 QDs (curve black) showed diffraction ECL signal was displayed. Fig. 3E–F shows the ECL-potential and CV
peaks at 2θ = 26.7◦ , 34.1◦ and 52.4◦ , all of which were consistent with curves of SnO2, g-C3N4 and SnO2/chitosan/g-C3N4. As shown in Fig. 3E,
the structure of tetragonal rutile SnO2, matching the crystal faces of the ECL intensity of SnO2, g-C3N4 and SnO2/chitosan/g-C3N4 increased
(110), (101), and (211) (JCPDS No.41–1445) [21–23]. The g-C3N4 has with the increasing absolute value of excitation voltage, then, the ECL
two diffraction peaks at 2θ = 13.2◦ and 27.4◦ , which in keeping with the peak appeared at approximate − 1.45 V. After that, the ECL intensity
(100) and (002) lattice planes, respectively (curve red) [24–26]. For the decreased with the excitation voltage from − 1.45 to 0 V. It can be seen
SnO2/chitosan/g-C3N4 nanocomposite, the diffraction peaks corre­ from Fig. 3F, the reduction peak of SnO2/chitosan/g-C3N4 nano­
sponding to the crystal planes of SnO2 and g-C3N4 were both shown. This composite presented a more positive potential at − 0.87 V compared
preliminary test confirmed the successful preparation of SnO2/chito­ with SnO2 (− 1.31 V) and g-C3N4 (− 1.007 V). The phenomenon implied
san/g-C3N4 nanocomposite. the combination of SnO2 and g-C3N4 promote the reduction of S2O2− 8 ,
The microstructures and surface appearances of g-C3N4 and SnO2/ thus enhancing the ECL intensity. The enhancement was ascribed to the
chitosan/g-C3N4 nanocomposite were characterized by transmission strong synergistic effect, which not only supplied more available cata­
lytic active sites, but also improved the electrochemical reaction effi­
ciency to output more strongly oxidizing intermediates (SO•− 4 ) by
facilitating the reduction of S2O2−
8 [27].
For the detection of lincomycin, aptamer DNA which has been pre­
treated by TCEP was attached to the surface of SnO2/chitosan/g-C3N4
nanocomposite through Sn–S bond. Subsequently, the unbond nonspe­
cific binding sites of aptasensor electrode was covered with MCH. After
that, Fc-DNA was incubated on the electrode surface through base
complementation with aptamer DNA. In the absence of lincomycin, the
excited energy was transferred from SnO2/chitosan/g-C3N4* to Fc,
means that the ECL signal was quenched by photo-excited electron
transfer and energy transfer process. In the presence of lincomycin, the
aptamer DNA was specific binding with lincomycin, and the Fc-DNA was
detached from the surface of electrode, then the ECL signal enhanced
gradually. And that’s mainly because the hydrogen bonding between the
DNA double strands is weaker than the specific binding between
aptamer DNA and lincomycin. On the basis of previous research, the
possible ECL mechanism of SnO2/chitosan/g-C3N4 may be as described
below:

SnO2/chitosan/g-C3N4 + e− →SnO2/chitosan/g-C3N•-
4 (1)

S2O2− − •− 2−
8 + e →SO4 + SO4 (2)

Fig. 1. XRD patterns of SnO2 QDS, g-C3N4 and SnO2/chitosan/g-C3N4 SnO2/chitosan/g-C3N•−


4 + SO•−
4 →SnO2/chitosan/g-C3N4* + SO2−
4 (3)
nanocomposites.

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X.-P. Liu et al. Talanta 233 (2021) 122546

Fig. 2. TEM images of (A) g-C3N4 and (B) SnO2/chitosan/g-C3N4. (C) HRTEM image of SnO2/chitosan/g-C3N4. (D) EDS spectra of SnO2/chitosan/g-C3N4.
SnO2/chitosan/g-C3N4*→SnO2/chitosan/g-C3N4+ hv (4)
DNA was forced to leave the surface of aptasensor electrode, generating
Scanning under the negative potential, SnO2/chitosan/g-C3N4 was
2− an increased Ret (curve f). These EIS results in keeping with expecta­
reduced to SnO2/chitosan/g-C3N•-4 , meanwhile, the co-reactant S2O8
tions, proving that the designed ECL aptasensor has been assembled
was transformed into strong oxidant SO4 . Then the strong oxidant SO•-
•-
4
successfully.
oxidized SnO2/chitosan/g-C3N•-
4 to SnO2/chitosan/g-C3N4*. The excited
state SnO2/chitosan/g-C3N4* is unstable, losing electrons transition to
ground state and generating ECL signal. 3.4. Optimization of experimental conditions

3.3. Electrochemical characteristics of different modified electrodes For purpose of effectively applying the constructed aptasensor to
detect lincomycin, the incubation time of Fc-DNA and aptamer DNA, the
In order to confirm whether the aptasensor electrode assembly was concentration of Fc-DNA, the incubation time of lincomycin and apta­
successful, electrochemical impedance spectroscopy (EIS) and cyclic sensor and the pH of the luminescent solution were optimized. The ECL
voltammetry (CV) tests were conducted. It can be seen from Fig. 4A, the responses of the aptasensor prepared with different concentrations of Fc-
bare electrode (curve a) exhibited a symmetric redox peak and high peak DNA were shown in Fig. 5A. It can be seen that, the ECL signal gradually
current. After the electrode was covered with SnO2/chitosan/g-C3N4 decreased with the raising concentration of Fc-DNA. As the concentra­
nanocomposite (curve b), the peak current was significantly reduced tion of Fc-DNA increased to 5 μM, the ECL intensity maintained stable,
which can be ascribed to the decreased electron transfer rate. After the which means that the binding sites of aptamer DNA were saturated.
aptamer DNA, MCH and Fc-DNA (curve c, d, e respectively) were Therefore, 5 μM of Fc-DNA was the optimal concentration in the
incubated on the electrode surface step by step, the peak current following experiment.
decreased gradually. This can be ascribed to the assembly of the non- When the optimal Fc-DNA concentration was determined, the incu­
conductive substance on the electrode surface reduced the electron bation time between Fc-DNA and aptamer DNA is of great importance
transfer. When lincomycin was incessantly added (curve f) and incu­ for the quenching effect of the substance. As the incubation time of Fc-
bated on the surface of the aptasensor electrode, the aptamer DNA was DNA and aptamer DNA increasing, the ECL signal decreased, and then
specific binding with lincomycin, and Fc-DNA was driven to leave the there is no significant change after 60 min (Fig. 5B). Therefore, the
electrode, the peak current decreased gradually. Therefore, the CV test optimal incubation time between Fc-DNA and aptamer DNA for this
results proved that the assembly of the aptasensor step by step was experiment was 60 min. Similarly, the incubation time of lincomycin
successful. and aptamer DNA was also optimized. As shown in Fig. 5C, the ECL
To further investigate the different assembly steps of the aptasensor, signal enhanced with the raising incubation time of lincomycin and
the EIS spectra of the aptasensor electrode at different assembly steps aptamer DNA, and then the ECL signal had no obvious variation after 70
was carried out (Fig. 4B). The bare electrode displayed a relatively small min. Thus, the incubation time of lincomycin and aptamer DNA was 70
electron transfer resistance (Ret) (curve a). After SnO2/chitosan/g-C3N4 min for the whole experiment.
nanocomposite was added on the surface of the electrode, the Ret Furthermore, the pH value also an significant indicator for the
increased obviously (curve b), indicating that the electron transfer of [Fe property of the aptasensor. Fig. 5D shows the ECL intensity of the
(CN)6]3− /4− on the electrode surface was blocked by SnO2/chitosan/g- aptasensor prepared with different pH value of the luminescent solution.
C3N4. As the aptasensor electrode was incubated with aptamer DNA, As shown in Fig. 5D, the ECL signal gradually enhanced with the
MCH and Fc-DNA stepwise, the Ret was increased continuously (curve c, increasing pH value and then reached the maximum value when pH
d and e respectively). After the aptasensor was incubated with linco­ value is 7.4. After that, the ECL signal decreased as the pH value con­
mycin, the aptamer DNA was specific binding with lincomycin, and Fc- tinues to increase, that’s mainly because under alkaline conditions,

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X.-P. Liu et al. Talanta 233 (2021) 122546

Fig. 3. (A) The ECL intensity of SnO2, g-C3N4 and SnO2/chitosan/g-C3N4. The ECL stability of (B) SnO2, (C) g-C3N4 and (D) SnO2/chitosan/g-C3N4 under a
continuous cyclic potential scan for 500s. (E) ECL-potential and (F) CV curves of SnO2, g-C3N4 and SnO2/chitosan/g-C3N4.

Fig. 4. (A) The curves of CV and (B) EIS for the stepwise aptasensor fabrication measured in 2.0 mM [Fe(CN)6]3− /4−
containing 0.1 M KCl, with the scan range of
− 0.2 to 0.6 V and rate of 100 mV/s.

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X.-P. Liu et al. Talanta 233 (2021) 122546

Fig. 5. Effects of (A) concentration of Fc-DNA, incubation time of (B) aptamer DNA with Fc-DNA and (C) aptamer DNA with Lincomycin, (D) the pH value.

excessive anions were stored up on the electrode surface, hence pre­ reproducibility. Moreover, the stability of the constructed aptasensor
venting SO•−
4 from approaching the electrode surface, resulting in was also explored. After the incubated electrode was scanned continu­
reduced ECL signal. Thus, the pH value of 7.4 was selected for the whole ously for 20 cycles, the ECL intensity had no significant change (Fig. 6C).
experiment process. The results showed that the aptasensor has a stable detection for
lincomycin.
3.5. Detection of lincomycin Selectivity is crucial for ECL aptasensor and plays an important role
in analytical methods. In order to assess the response of the established
The capability of the aptasensor was investigated by monitoring a aptasensor to other chaff interferents, the interference tests were carried
suite of different concentrations of lincomycin under the optimal con­ out with prostate-specific antigen (PSA, 10 mg mL− 1), carcinoembryonic
ditions. As shown in Fig. 6A, the ECL signal gradually enhanced as the antigen (CEA, 10 mg mL− 1), mucin 1 (MUC1, 10 mg mL− 1), bovine
concentration of lincomycin increasing. After the aptasensor was incu­ serum albumin (BSA, 10 mg mL− 1), platelet-derived growth factor
bated with lincomycin, the aptamer DNA was specific binding with (PDGF-BB, 10 mg mL− 1) and mixture. As shown in Fig. 6D, in compar­
lincomycin, and Fc-DNA was forced to leave the electrode surface, the ison with the blank, the ECL signals for 10 mg mL− 1 of PSA, CEA, MUC1,
photo-excited electron transfer and energy transfer reduced, then the BSA and PDGF-BB were almost no changed. However, the ECL signal of
ECL intensity gradually recovered. It can be seen from Fig. 6B, the ECL the aptasensor for lincomycin (0.10 mg mL− 1) showed an significantly
signal enhanced as the raising logarithm of lincomycin concentration in increase. At the same time, compared with the aptasensor only incu­
the range of 0.10 ng mL− 1 - 0.10 mg mL− 1. The linear regression bated with lincomycin, the ECL signal of the aptasensor incubated with
equation between logarithm of lincomycin concentration and ECL signal lincomycin (0.10 mg mL− 1) containing all kinds of the above in­
was ECL = 14294.7 + 1218.2lgC. The linearly correlation coefficient terferences (10 mg mL− 1) was almost no changed. These mean that the
was 0.998, and the limit of detection was 0.028 ng mL− 1. Compared established ECL aptasensor exhibited a selective detection for linco­
with the previous literatures on the detection of lincomycin (Table 1), mycin.(see Fig. 6).
the aptasensor exhibited a wider linear range and lower limit of
detection 3.7. Practical application of ECL aptasensor

3.6. Reproducibility, stability and selectivity of the aptasensor In order to explore the practical application performance, the prac­
ticality of the aptasensor was further examined. To be specific, the
Reproducibility is a remarkable indicator for aptasensor, which is standard addition method was used to detect lincomycin in milk sample
also an important index for analytical detection method. In the cause of with the proposed aptasensor. The milk sample used in the experiment
assessing the reproducibility of the proposed aptasensor, the ECL re­ was purchased from supermarket and the package was intact. The milk
sponses of six sensor electrodes in the same conditions were analyzed. sample was centrifuged for 20 min at 12,000 rpm, after placed at room
The relative standard deviation (RSD) was 3.56% for lincomycin with temperature for 30 min, the obtained centrifugal product was diluted 10
same concentration, which indicates that the aptasensor has good folds. Then, the milk sample with certain concentration of lincomycin

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X.-P. Liu et al. Talanta 233 (2021) 122546

Fig. 6. (A) ECL intensity and (B) the corresponding calibration curve of the aptasensor for the detection of different concentration of lincomycin. (C) The ECL
stability of the aptasensor with the concentration of lincomycin (0.10 mg mL− 1) under a continuous cyclic potential scan for 20 cycles. (D) The selectivity of the
proposed ECL aptasensor detection of lincomycin (0.10 mg mL− 1) against different targets: PSA (10 mg mL− 1), CEA (10 mg mL− 1), MUC1 (10 mg mL− 1), BSA (10 mg
mL− 1), PDGF-BB (10 mg mL− 1) and a mixture (0.10 mg mL− 1 lincomycin, 10 mg mL− 1 PSA, 10 mg mL− 1 CEA, 10 mg mL− 1 MUC1, 10 mg mL− 1 BSA, 10 mg mL− 1
PDGF-BB). Error bars: SD, n = 3.

Table 1 Table 2
Comparison of various methods for target lincomycin detection. Determination of lincomycin in milk by standard addition.
Analytical Linear range Limit of detection Reference Milk samples Added (ng⋅mL− 1) Found (ng⋅mL− 1) Recovery(%) RSD(%)
method
1 1 1.03 103.0 2.81
Fluorescence 0.2 μg/mL-4.8 μg/mL 0.061 μg/mL [28] 2 10 10.84 108.40 3.52
Electroanalysis 0.5 μM–125 μM 0.02 μM [29] 3 100 96.15 96.15 4.07
PEC 0.1 nM–300 nM 0.076 nM [30]
ECL 0.1 ng/mL-0.10 mg/mL 0.028 ng/mL This work
(0.225 nM-0.225 mM) (0.063 nM) Credit author statement

Xing-Pei Liu: Conceptualization, Investigation, Writing – original


was studied. As shown in Table 2, the recovery rate of the added
draft. Bo Huang: Methodology, Investigation. Chang-Jie Mao: Supervi­
lincomycin was 96.15%~108.40%, and the relative standard deviation
sion, Writing - review& editing. Jing-Shuai Chen: Validation. Bao-Kang
wass 2.81%~4.17%. The experimental results proved that the estab­
Jin: Writing – review & editing.
lished aptasensor was acceptable for lincomycin detection in practical
application.
Declaration of competing interest
4. Conclusion
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
In this work, a sensitive and effective ECL aptasensor was established
the work reported in this paper.
successfully based on SnO2/chitosan/g-C3N4 nanocomposite for the
detection of lincomycin. Compared with previous detection methods,
Acknowledgments
the prepared aptasensor showd a lower limit of detection (0.028 ng
mL− 1) and wider detection range from 0.10 ng mL− 1 to 0.10 mg mL− 1
This work was supported by the National Natural Science Foundation
for lincomycin detection and it performed well in actual sample test. At
of China (Grant Nos. 21976001), Natural Science Foundation of Anhui
the same time, the aptasensor also showd good selectivity and repro­
Province (1808085QB53). Open fund for Discipline Construction of
ducibility, high sensitivity and stability. Consequently, the constructed
Institute of Physical Science and Information Technology.
ECL aptasensor exhibits great promise for monitoring lincomycin.

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X.-P. Liu et al. Talanta 233 (2021) 122546

Appendix A. Supplementary data [14] J.W. Gao, H.W. Xiong, W. Zhang, Y. Wang, H.X. Wang, W. Wen, X.H. Zhang, S.
F. Wang, Electrochemiluminescent aptasensor based on β-cyclodextrin/graphitic
carbon nitride composite for highly selective and ultrasensitive assay of platelet
Supplementary data to this article can be found online at https://doi. derived growth factor BB, Carbon 130 (2018) 416–423, https://doi.org/10.1016/j.
org/10.1016/j.talanta.2021.122546. carbon.2018.01.026.
[15] S. Sohila, M. Rajalakshmi, C. Muthamizhchelvan, S. Kalavathi, Optical properties
of Fe-doped SnO2 nanoparticles, AIP Conf. Proceed. 1447 (2012) 251–252, https://
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