pubs.acs.

org/ac Article

High-Efficiency CdSe Quantum Dots/Fe3O4@MoS2/S2O82−

Electrochemiluminescence System Based on a Microfluidic Analysis
Platform for the Sensitive Detection of Neuron-Specific Enolase
Tao Feng, Xianzhen Song, Yu Du, Yu Bai, Xiang Ren, HongMin Ma, Dan Wu, YuYang Li,*
and Qin Wei*
Cite This: Anal. Chem. 2022, 94, 9176−9183 Read Online
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ABSTRACT: In this work, based on electrochemiluminescence (ECL) technology and self-assembled portable disease detection
chips, a bioactivity-maintained sensing platform was developed for the quantitative detection of neuron-specific enolase. First, we
prepared Fe3O4@MoS2 nanocomposites as an efficient catalyst to accelerate the reduction of persulfate (S2O82−). Specifically,
abundant sulfate radicals (SO4•−) were generated because of cyclic conversion between Fe2+ and Fe3+. Meanwhile, MoS2
nanoflowers with a high specific surface area could not only load more Fe3O4 but also solve its agglomeration problem, which greatly
improved the catalytic efficiency. Moreover, a biosensor chip was constructed by standard lithography processes for disease
detection, which had good sensitivity and portability. According to the above strategies, the developed portable sensing platform
played the part of promoting the practical application of bioanalysis in early tumor screening and clinical diagnosis. In addition, we
developed a short peptide ligand (NARKFYKG, NAR) to avoid the occupation of antigen binding sites by specifically connecting to
Fc fragments in antibodies. Thus, the binding efficiency of antibodies and the activity of biosensors were improved due to the
introduction of NAR.

■ INTRODUCTION
Electrochemiluminescence (ECL) is a special form of
chemiluminescence.1−4 In short, through the gain and loss of
electrons, luminescent materials produce active intermediates,
then reach the excited state, and finally convert the excited
state back to the luminescent ground state.3,5,6 Because of its
high sensitivity and controllability, ECL has grown into an
important electrochemical detection method.7,8 Neuron-
specific enolase (NSE) is one of the most sensitive markers
of small cell lung cancer (SCLC).9−11 It may indicate the
occurrence of SCLC when the content of NSE exceeds the
normal range level in the human body. Therefore, the
development of an efficient NSE detection method combined
with ECL technology has an important application value for
the diagnosis and treatment of SCLC.
Microfluidics is widely used to accurately control the size
distribution, structure, and composition of nanomaterials
because of the micron-scale channel structure,12,13 excellent
droplet and fluid manipulation performance,14 and fast heat
and mass transfer rates.15 Importantly, microfluidic chips have
a good channel structure, gas permeability, and optical
transparency, which exhibits great compatibility when being
integrated with sensors, electrodes, micropumps, and
valves.16,17 However, there are few studies on the application
of microfluidic technology in electrical analysis, especially ECL.
In this study, electrophysiological electrodes were printed on
indium tin oxide (ITO) by screen printing and wet etching
Received: April 28, 2022
Accepted: June 6, 2022
Published: June 16, 2022

© 2022 American Chemical Society https://doi.org/10.1021/acs.analchem.2c01868

9176 Anal. Chem. 2022, 94, 9176−9183
Analytical Chemistry
Scheme 1. (A) Schematic Diagram of a Microfluidic Detection Chip and (B) the Fabrication Process of a Biosensor
technology, and the microchannels were constructed by
polydimethylsiloxane (PDMS) through a standard lithography
process. Finally, the highly integrated portable chips prepared
based on the above strategy were applied to the detection of
NSE, which displayed good sensitivity.
Quantum dots (QDs) have different physical and chemical
properties from conventional nanomaterials because of their
obvious quantum size effect,18 surface effect,18 dielectric
confinement effect,19 and quantum tunnel effect.20 As
cadmium-based QDs, CdSe QDs have highly asymmetric
internal variable structures21,22 and many ideal optical
properties, such as sub thermal room temperature linewidth,
spectral diffusion suppression, and high photoluminescence
quantum yield, which promote the application of CdSe QDs in
ECL. However, the luminescence ability of QDs is not strong,
so it is important to choose an efficient co-reaction promoter
to enhance its ECL intensity.23 Fe3O4@MoS2 is a transition
metal oxide with excellent photocatalytic, optoelectronic, and
optical properties. In addition, its catalytic properties have
been widely recognized in many studies.24−27 Fe3O4@MoS2
was selected as a co-reaction promoter for improving ECL
responses, which was designed by making Fe3O4 nanospheres
uniformly grow on the surface of MoS2 nanoflowers (NFs)
through a hydrothermal method.
During the construction process of biosensors, their stability
and sensitivity can be affected by the bioactivity of antibod-
ies.28 As an immunoglobulin, antibodies can specifically
recognize antigens, and the antibody variable region (Fab
fragment) is the main distribution region of antigen-binding
sites. Therefore, developing an appropriate antibody immobi-
lization strategy to avoid Fab fragment occupation is an
important way to protect antibody activity. Here, in order to
maintain the biological activity of the antibody, we introduced
an antibody affinity ligand called NARKFYKG (NAR). NAR is
a short peptide ligand composed of several key amino acid
residues,10 which can maintain the bioactivity and improve the
hatching efficiency of antibodies through specific connection
with antibody Fc fragments. Therefore, it has broad application
prospects in immunoassays.
Based on the above considerations, we selected CdSe QDs
as the illuminant, Fe3O4@MoS2 as the co-reaction promoter,
K2S2O8 as the co-reactant solution, and NAR as the
bifunctional antibody immobilizer, and combined with the
self-designed microfluidic sensor disease detection chips, a
high-performance biosensor was developed to realize the
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ultrasensitive detection of NSE. At first, a ternary reaction
system was designed to enhance the ECL intensity of the
biosensor chip, which included CdSe QDs, Fe3O4@MoS2, and
K2S2O8. As the basis of ternary system construction, CdSe
QDs with good luminescence characteristics provided a
reliable guarantee for the construction of the system. The
appropriate concentration of K2S2O8 could promote the
formation of SO4•−, which significantly amplified the ECL
intensity of CdSe QDs. At the same time, the intervention of a
co-reaction promoter avoided the amplification of ECL signals
by introducing a high-concentration illuminant. Concurrently,
due to the introduction of NAR, the antibody-binding
efficiency was enhanced and the activity of the biosensor was
protected. More importantly, the developed portable micro-
fluidic chips integrated with a microelectrode showed highly
sensitive detection of NSE, showing good application potential
in the clinical diagnosis of SCLC. These sensing strategies
opened up new prospects for the application of QDs as
luminophores in ECL detection and improved the practical
application ability of the constructed biosensor.
■
EXPERIMENTAL SECTION
Preparation of Fe3O4@MoS2. The prepared 0.1 g Fe3O4
nanospheres were added to 30 mL of ultrapure water and
ultrasonicated for 1 h for complete dispersion, and then 0.76 g
of sodium molybdate and 0.6 g of thiourea were added and
ultrasonicated for 30 min again.29 Then, all of above mixed
solution was added to the polytetrafluoroethylene reactor and
kept at 200 °C for 24 h. After all of this, the product was
assembled by magnet separation and rinsed alternately with
ethanol and ultrapure water six times. Finally, the obtained
Fe3O4@MoS2 nanomaterials were dried in a 60 °C vacuum
oven for 10 h. In addition, MoS2 was prepared without the
addition of Fe3O4.
Preparation of CdSe QDs-Au NPs-NAR-Ab2. Based on a
previous work,30 the preparation of CdSe QDs was improved
(Section S5 in the Supporting Information). Also, after the
reaction, the product was cooled to room temperature and
stored in a 4 °C refrigerator. On this basis, 1 mL of Au NPs
solution was added to 5 mL of CdSe QDs solution and shaken
for 8 h at 4 °C to achieve a good connection. Then, 300 μL of
NAR solution was added and shaken for another 4 h. Finally,
300 μL of Ab2 solution was added, and CdSe QDs-Au NPs-
NAR-Ab2 were obtained after incubation for 10 h.
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Figure 1. (A) TEM image and (B) size distribution of CdSe QDs. (C) HRTEM image of CdSe QDs. (D) PL and ECL emission spectra of CdSe
QDs.

Figure 2. (A) SEM image of Fe3O4@MoS2. (B) XRD spectra of Fe3O4, MoS2, and Fe3O4@MoS2 (correspond to black, red, and blue lines,
respectively). XPS spectra of the (C) entire region, (D) Fe 2p region, (E) Mo 3d region, and (F) S 2p region of Fe3O4@MoS2.

Preparation of Microelectrodes. As shown in Scheme
1A and Figure S1, indium tin oxide (ITO) was cropped to the
right size (6 cm × 4 cm) and then was washed with abluent,
acetone, and absolute ethanol in turn.31 After processing, it was
cleaned with ultrapure water and dried with nitrogen. Second,
the obtained ITO was screen-printed with ink and dried at 80
°C for 12 h. Then, the dried ITO was etched with the prepared
etching solution (HCl:HNO3:FeCl3 = 1 M:1 M:0.5 M) at 37
9178
°C for 25 min to remove the conductive layer. Third, the ink
on ITO was cleaned with acetone solution and then soaked in
ethanol and ultrasonicated for 115 min. Next, the treated ITO
was boiled for 15 min, then soaked in 200 mL of isopropanol
containing 2 M KOH solution, and thoroughly cleaned with
ultrapure water. Finally, the completely dispersed Fe3O4@
MoS2 was dropped on the cleaned work electrode (WE)
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Analytical Chemistry
Figure 3. (A) Optimization of pH. (B) K2S2O8 concentration. (C) Fe3O4@MoS2 concentration. (D) ECL signals of the developed biosensor chip
with and without NAR at different antibody incubation times.
microelectrode surface. Thus, the preparation of micro-
electrodes was realized.
Preparation of ECL Biosensor Chips. First, the micro-
electrode was combined with the PDMS cover with micro-
fluidic channels made by soft lithography through bonding
technology. Then, 6 μL of NAR, 8 μL of 1 mg/mL Ab1, 3 μL
of 1 wt % BSA, 10 μL of NSE with different concentrations,
and 8 μL of CdSe QDs-Au NPs-NAR-Ab2 were successively
introduced through 1−5 inlets. Notably, each injection was
carried out on the basis that the uncombined reagents were
cleaned with PBS, and all incubation processes were performed
at 4 °C.
ECL Measurement. First, the biosensor chip was put into
the cassette and connected to a three-electrode system. Then,
the scanning potential was set to −1.6 to 0 V, the scanning rate
was set to 0.1 V/s, and the photomultiplier tube (PMT) was
800 V, which was used to measure the signals of ECL.
■
RESULTS AND DISCUSSION
Characterization of CdSe QDs. The synthesized CdSe
QDs were characterized by transmission electron microscopy
(TEM) images, ECL, and photoluminescence spectroscopy
(PL) spectra. Figure 1A,B displays that the prepared CdSe
QDs have a relatively uniform particle size, which is mainly
distributed between 3 and 6 nm. Meanwhile, by high-
resolution transmission electron microscopy (HRTEM), the
two-dimensional (2D) lattice structure of CdSe QDs was
researched. In Figure 1C, the lattice stripes with a spacing of
about 0.36 nm could be clearly observed, which was consistent
with the (111) crystal plane of CdSe QDs. Figure 1D suggests
the emission spectra of CdSe QDs about PL and ECL. There
was an obvious fluorescence emission peak (red curve) at 657
nm (excitation wavelength was 490 nm), which was near to the
ECL emission peak (purple curve) at 739 nm. The illustration
in Figure 1D shows that the orange CdSe QDs (left) emitted
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red light (right) under the irradiation of an ultraviolet lamp.
The above results confirmed that CdSe QDs with lumines-
cence performance were successfully prepared.
Characterization of Fe3O4@MoS2 Nanocomposites. As
shown in Figure 2A, Fe3O4 nanospheres were evenly
distributed on the surface of MoS2 nanoflowers (NFs),
which indicated that Fe3O4@MoS2 was successfully synthe-
sized. Figure 2B displays the XRD patterns of Fe3O4, MoS2,
and Fe3O4@MoS2. The diffraction peaks of 30.1, 35.4, 43.1,
53.7, 56.8, and 62.7° belong to the (220), (331), (400), (422),
(511), and (440) crystal planes of Fe3O4, respectively (JCDPS
No. 75-0033, black line). The diffraction peaks of 13.9, 33.2,
and 58.7° belong to the (002), (100), and (110) crystal planes
of MoS2 (JCDPS No. 37-1492, red line). Meanwhile, as shown
in the XRD spectrum (blue line), the characteristic peaks of
Fe3O4 and MoS2 were well retained in Fe3O4@MoS2, which
indicated that the crystal form and crystal phase of Fe3O4 and
MoS2 in the composite have not changed. The elemental
composition and surface electronic valence of Fe3O4@MoS2
were further characterized by X-ray photoelectron spectrosco-
py (XPS). According to Figure 2C, the XPS full spectrum of
Fe3O4@MoS2 demonstrated four elements (Mo, Fe, O, and S).
Figure 2D exhibits the spectrum of the Fe 2p region, and the
peaks at 710.6, 713.0, 724.2, and 727.0 eV correspond to Fe2+
2p3/2, Fe3+ 2p3/2, Fe2+ 2p1/2, and Fe3+ 2p1/2, respectively.
Meanwhile, the satellite peaks in the spectrum of the Fe 2p
region were related to the peaks at 719.0 and 733.4 eV. As
illustrated in Figure 2E, the spectral peaks of Mo4+ 3d5/2 and
Mo4+ 3d3/2 in the Mo 3d region were 228.5 and 231.8 eV,
respectively. Mo5+ was a transition state, and the peaks at 230.1
eV correspond to Mo5+ 3d5/2 and 232.6 eV belong to Mo5+
3d3/2. The peak value of Mo6+ 3d3/2 was 235.3 eV, which may
be related to the partial oxidation of MoS2 to MoO3 in the
atmospheric environment. The peak at 226.0 eV came from S
2s in MoS2. The spectrum of S 2p is presented in Figure 2F.
The main S2− 2p3/2 and S2− 2p1/2 were represented as 161.4
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Analytical Chemistry
Figure 4. (A−C) Schematic diagram of the possible ECL mechanism. (D) ECL−potential curves of CdSe QDs, CdSe QDs + Fe3O4, and CdSe
QDs + Fe3O4@MoS2 in PBS containing 80 mM S2O82−.
and 162.5 eV peaks, respectively. The peak at 164.5 eV can be
attributed to unsaturated sulfur on the surface of MoS2. The
peak at 168.4 eV may be caused by the oxidation of some
sulfur elements to SI(-SOn-). These conclusions strongly
confirm the successful preparation of Fe3O4@MoS2.
Optimization of Experimental Conditions. As a matter
of fact, in order to obtain the finest experimental results, we
optimized the experimental conditions. Figure 3A shows the
effect of pH on the ECL signals. When the pH value was from
6.0 to 7.0, the ECL responses were enhanced. Afterward, the
ECL signals gradually decreased when the pH value increased
from 7.0 to 8.5. These could be attributed to the inhibition of
the ECL responses put down to the rapid reduction of protons
under lower pH conditions and the effect of bioactivity of
target under higher pH conditions. Based on the above
analysis, the most ideal pH was 7.0. Figure 3B suggests the
optimized results of the K2S2O8 concentration. When the
concentration of K2S2O8 was less than 80 mM, the production
of SO4•− gradually enhanced with the increase in its
concentration, and finally more CdSe QDs* were generated
for ECL emission. After that, S2O82− was in excess when its
concentration was greater than 80 mM, which affected the
formation of CdSe QDs* and ultimately affected the ECL
signals. Based on the points discussed above, 80 mM was
considered to be the best concentration of K2S2O8. Figure 3C
reveals that the performance of the biosensor was affected by
the Fe3O4@MoS2 concentration. First, the ECL signals
enhanced with an increase in Fe3O4@MoS2 concentration.
Then, the ECL signals began to decrease when the Fe3O4@
MoS2 concentration was greater than 2 mg/mL. The above
results may be attributed to an increase in interface electron
transfer resistance with the existence of excessive Fe3O4@
MoS2. Consequently, the optimal Fe3O4@MoS2 concentration
was at 2 mg/mL. As illustrated in Figure 3D, we found that the
optimal incubation time was approximately 1 h in the presence
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of NAR, which was better than without NAR. Furthermore, the
proposed biosensor with NAR had a stronger ECL signal than
that without NAR due to an effective directional fixation of
antibodies. Based on these conclusions, the optimal detection
results could be obtained by controlling the antibody
incubation time at about 1 h under the condition of NAR.
Importantly, the above studies demonstrated that NAR could
significantly improve the incubation efficiency of antibodies.
Possible Signal Amplification and Luminescence
Mechanism. The possible ECL emission process is shown
in Figure 4. First, CdSe QDs could not produce strong ECL
signals when the co-reactant was absent (Figure 4A). As shown
in Figure 4B, a handful of SO4•− was produced on the
microelectrode surface when S2O82− was present, and then the
generated SO4•− reacted with CdSe QDs•− to produce a weak
ECL signal. In Figure 4C, a large amount of SO4•− was
obtained after Fe3O4@MoS2 was added, which realized the
effective signal amplification. The specific reaction mechanism
was as follows: S2O82− first obtained electrons on the
microelectrode surface and then produced a small amount of
SO4•− to produce a weak ECL signal (Route 1). Route 2 refers
to the reduction of S2O82− by Fe2+ to obtain sufficient SO4•−
for ECL emission. Meanwhile, the reversible cycle of Fe2+ and
Fe3+ ensured the continuous luminescence. In Route 3, the
peroxidase-like properties of Fe3O4@MoS2 promoted the
conversion of H2O2 to OH• and finally further improved the
ECL signal of CdSe QDs. In the ECL emission of CdSe QDs,
it first obtained electrons to generate CdSe QDs•−‑, next CdSe
QDs•− reacted with SO4•− to produce CdSe QDs*, and finally
luminescence was produced. Figure 4D presents the ECL−
potential curves of CdSe QDs-, CdSe QDs/Fe3O4-, and CdSe
QDs/Fe3O4@MoS2-modified microelectrodes, and the signal
trend confirmed our inference of the signal amplification and
luminescence mechanism.
Route 1:
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Analytical Chemistry pubs.acs.org/ac Article

Figure 5. (A) ECL signals of NSE with different concentrations (10 fg/mL to 500 ng/mL, a ∼ l). (B) Calibration curve, (C) storage and (D)
operation stability, (E) selectivity, and (F) reproducibility of the proposed biosensor.

S2 O82 − + e− → SO4 2 − + SO4•−
Route 2:
Fe2 + + S2 O82 − → Fe3 + + SO4 2 − + SO4•−
Fe3 + + e− → Fe 2 +
Route 3:
2H 2O → 4H+ + O2 + 4e−
2H 2O + O2 + 2e− → H 2O2 + 2OH−
H 2O2 + e− → OH− + OH•
or
Fe 2 + + H 2O2 → Fe3 + + OH− + OH•(more)
OH• + S2 O82 − → HSO4 − + O2 + SO4•−(more)
ECL emission:
CdSe QDs + e− → CdSe QDs•−
CdSe QDs•− + SO4•− → CdSe QDs* + SO4 2 −
CdSe QDs* → CdSe QDs + hv
ECL Responses of the Constructed Biosensor to NSE.
In order to verify the detection ability of the biosensor, we
detected the ECL responses of different concentrations of NSE
in the finest experimental conditions. In line with Figure 5A,
when the concentrations of NSE gradually increased from 10
fg/mL to 500 ng/mL, the signals of the biosensor were
enhanced. Meanwhile, the logarithm of the NSE concentration
was linearly correlated with the ECL responses in the above
detection range. As shown in Figure 5B, the linear equation
(1) was I = 1698.7 lg c + 10,028 (I is the ECL intensity and c is the
NSE concentration), with a correlation coefficient of 0.998,
and the detection limit was 3.67 fg/mL (S/N = 3). Therefore,
the biosensor had a wide linear detection range and low
(2)
detection limit, which was better than the previous work
(3) (Table S1). The above results showed that the proposed
biosensor chip exhibited excellent application potential in the
ultrasensitive detection of NSE.
Performance Test of the Proposed Biosensor. In order
(4)
to verify the storage stability of the biosensor, parallel
(5) experiments were carried out on the designed biosensor for
4 weeks with and without NAR. As shown in Figure 5C, the
(6) signal attenuation was less after NAR was introduced, which
showed that NAR protected the activity of the proposed
biosensor chip. As illustrated in Figure 5D, the luminescence
(7)
intensity of the biosensor maintained good stability in the
presence of different concentrations of CEA, indicating that
the obtained signals were reliable. The selectivity of the sensing
(8)
platform was explored by using carcinoembryonic antigen
(CEA), procalcitonin (PCT), bovine serum albumin (BSA),
alpha fetoprotein (AFP), trypsin (TPS), alanine (Ala), insulin
(9)
(Ins), and amyloid-β proteins (Aβ) as interferences. Figure 5E
displays that their ECL signals were different from that of NSE,
(10)
and their signals were close to the blank sample. Meanwhile,
when NSE coexisted with interfering substances (10 ng/mL
(11)
NSE + 100 ng/mL), the ECL intensity of the biosensor chip
did not change substantially, which indicated that the
constructed biosensor had excellent selectivity. To investigate
the reproducibility of the biosensor, seven different sensing
chips were selected for ECL tests. In Figure 5F, the RSD of the
ECL signals measured by these chips were 1.3%, which
indicated that the proposed biosensor chip had good
reproducibility.
Analysis of Serum Samples. We used the standard
addition method to add a series of spiked samples (different
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Analytical Chemistry
concentrations of NSE) to the original human serum samples
and calculated the corresponding recovery and RSD after 11
tests so as to research the practicability of the constructed
biosensor chip in clinical application. Table S2 suggests that
the recovery rate was 98.5−103% and the RSD was 1.4−3.0%,
which demonstrated that the built biosensor chip was reliable
for detection of human serum samples.
■
CONCLUSIONS
On the whole, we developed a portable biosensor chip that
integrated a multidimensional sensing device for bioanalysis
based on electrochemiluminescence and microfluidic tech-
nologies. The prepared biosensor chip had remarkable
characteristics of small sample consumption, rapid signal
response, and excellent analytical performance. Fe3O4@MoS2
with high catalytic performance was used as a co-reaction
promoter to achieve the effective amplification of the
luminescence signals, thus improving the sensitivity of the
biosensor chip, which had reference significance for the
application of QDs in ECL systems. The designed NAR
short peptide ligand ensured the bioactivity and improved the
incubation efficiency of antibodies by specifically binding to
the Fc fragments. The proposed biosensor chip had high
stability and detection accuracy in serum sample detection,
which broadened the direction for the clinical application of
biosensing analysis.
■ ASSOCIATED CONTENT
* Supporting Information
sı
The Supporting Information is available free of charge at
https://pubs.acs.org/doi/10.1021/acs.analchem.2c01868.
Additional experimental details, materials, and methods,
including materials, apparatus, preparation of micro-
electrodes and the photolithography process of the
microfluidic chip, preparation of Fe3O4 and CdSe QDs,
EDS of Fe3O4@MoS2 and XPS of O 1s, electrochemical
characterizations of the biosensor, comparison with
other analysis platforms for NSE detection, and
preliminary evaluation of NSE in human serum samples
(PDF)
■
AUTHOR INFORMATION
Corresponding Authors
YuYang Li − Collaborative Innovation Center for Green
Chemical Manufacturing and Accurate Detection, Key
Laboratory of Interfacial Reaction & Sensing Analysis in
Universities of Shandong, School of Chemistry and Chemical
Engineering, University of Jinan, Jinan, Shandong 250022,
China; orcid.org/0000-0002-1399-9381; Phone: +86
531 82765730; Email: chm_liyy@ujn.edu.cn; Fax: +86
531 82765969
Qin Wei − Collaborative Innovation Center for Green
Chemical Manufacturing and Accurate Detection, Key
Laboratory of Interfacial Reaction & Sensing Analysis in
Universities of Shandong, School of Chemistry and Chemical
Engineering, University of Jinan, Jinan, Shandong 250022,
China; Department of Chemistry, Sungkyunkwan University,
Suwon 16419, Republic of Korea; orcid.org/0000-0002-
3034-8046; Phone: +86 531 82765730;
Email: sdjndxwq@163.com; Fax: +86 531 82765969
9182
pubs.acs.org/ac Article
Authors
Tao Feng − Collaborative Innovation Center for Green
Chemical Manufacturing and Accurate Detection, Key
Laboratory of Interfacial Reaction & Sensing Analysis in
Universities of Shandong, School of Chemistry and Chemical
Engineering, University of Jinan, Jinan, Shandong 250022,
China
Xianzhen Song − Collaborative Innovation Center for Green
Chemical Manufacturing and Accurate Detection, Key
Laboratory of Interfacial Reaction & Sensing Analysis in
Universities of Shandong, School of Chemistry and Chemical
Engineering, University of Jinan, Jinan, Shandong 250022,
China
Yu Du − Collaborative Innovation Center for Green Chemical
Manufacturing and Accurate Detection, Key Laboratory of
Interfacial Reaction & Sensing Analysis in Universities of
Shandong, School of Chemistry and Chemical Engineering,
University of Jinan, Jinan, Shandong 250022, China;
orcid.org/0000-0002-9002-8845
Yu Bai − Collaborative Innovation Center for Green Chemical
Manufacturing and Accurate Detection, Key Laboratory of
Interfacial Reaction & Sensing Analysis in Universities of
Shandong, School of Chemistry and Chemical Engineering,
University of Jinan, Jinan, Shandong 250022, China
Xiang Ren − Collaborative Innovation Center for Green
Chemical Manufacturing and Accurate Detection, Key
Laboratory of Interfacial Reaction & Sensing Analysis in
Universities of Shandong, School of Chemistry and Chemical
Engineering, University of Jinan, Jinan, Shandong 250022,
China; orcid.org/0000-0002-4321-4282
HongMin Ma − Collaborative Innovation Center for Green
Chemical Manufacturing and Accurate Detection, Key
Laboratory of Interfacial Reaction & Sensing Analysis in
Universities of Shandong, School of Chemistry and Chemical
Engineering, University of Jinan, Jinan, Shandong 250022,
China; orcid.org/0000-0002-7061-8944
Dan Wu − Collaborative Innovation Center for Green
Chemical Manufacturing and Accurate Detection, Key
Laboratory of Interfacial Reaction & Sensing Analysis in
Universities of Shandong, School of Chemistry and Chemical
Engineering, University of Jinan, Jinan, Shandong 250022,
China; orcid.org/0000-0002-8732-5988
Complete contact information is available at:
https://pubs.acs.org/10.1021/acs.analchem.2c01868
Notes
The authors declare no competing financial interest.
■
ACKNOWLEDGMENTS
This study was supported by the National Natural Science
Foundation of China (nos. 21777056 and 21427808) and
Special Foundation for Taishan Scholar Professorship of
Shandong Province, Jinan Scientific Research Leader Work-
shop Project (2018GXRC024 and 2018GXRC021).
■
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https://doi.org/10.1021/acs.analchem.2c01868
Anal. Chem. 2022, 94, 9176−9183
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9183 https://doi.org/10.1021/acs.analchem.2c01868
Anal. Chem. 2022, 94, 9176−9183