Brightly near-infrared to blue emission tunable silver-carbon dot nanohybrid for sensing of ascorbic acid and construction of logic gate

Talanta 162 (2017) 135–142

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

Brightly near-infrared to blue emission tunable silver-carbon dot nanohybrid for sensing of ascorbic acid and construction of logic gate ⁎

Tian Tianb, Yaping Zhongb, Chun Dengb, Hao Wangb, Yu Hea,b, , Yili Gea,b, Gongwu Songa,b,

crossmark ⁎

a

Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials, Hubei University, Wuhan 430062, China Ministry-of-Education Key Laboratory for the Synthesis and Application of Organic Functional Molecules, College of Chemistry and Chemical Engineering, Hubei University, Wuhan 430062, China

b

A R T I C L E I N F O

A BS T RAC T

Keywords: Carbon dots Metal-enhanced fluorescence Near-infrared Logic gate

Recently, carbon dots (CDs) have drawn extensive attention owing to their unique properties. While more and more research had been focusing on the exploration of CDs as fluorescence sensors, the blue or green fluorescence emission of CDs restricts further applications of CDs, particularly in the biology-relevant fields due to the commonly blue auto-fluorescence of biological matrix. Therefore, the preparation of CDs with strong emission at long wavelengths is highly desirable. For these situations, a facile, straightforward and extrareductant needless method was established to fabricate silver-carbon dot nanohybrid with enhanced nearinfrared fluorescence through metal-enhanced fluorescence (MEF). We applied the Ag-CD nanohybrid as a probe to detect antioxidants such as ascorbic acid in near-infrared window, and the probe possesses a linear range of 0.2–60 μM. More importantly, this sensor could not only function in aqueous solution, but also display well selective response in intricate biological fluids. In addition, an IMPLICATION logic gate was constructed based on the unique characteristics of Ag-CD nanohybrid which presages more opportunities for application in single and multiple biological sensing.

1. Introduction Compared to conventional measurements made in the ultraviolet (UV)-vis region, interest in near-infrared (NIR) fluorescent biosensors is continue to increase because, in the physiologically relevant optical window (650–900 nm), the features of this technique include minimal levels of interfering absorption from biological samples, reduced scattering, and minimal levels of auto-fluorescence [1,2]. NIR quantum dots (QDs) represent a powerful material in sensing and bio-imaging applications recently for their obvious advantages over NIR fluorescent organic dyes in many aspects such as better aqueous and colloid stability, narrower half peak and higher fluorescence quantum yield [2–7]. However, the biological toxicity of QDs must be carefully considered because the release of Cd2+, Hg2+, Pb2+ ions composing of NIR QDs arouse cytotoxicity and is a potential environmental hazard, which limits the application of NIR QDs [8–10]. Therefore, studies are urgently necessary to explore novel NIR fluorescence nanomaterials for developing advanced smart sensors. Recently, carbon dots (CDs) have drawn extensive attention in various fields owing to their stable physicochemical and photochemical properties. Due to the urgent need of environmentally-friendly fluor-

⁎

escent nanomaterials, the CDs appear to be an encouraging alternative to traditional organic dyes and quantum dots for imaging and sensing because of their superiority in chemical inertness, biocompatibility, easy to be preparation, low toxicity and cheaper cost [11–13]. While more and more research had been focusing on the exploration of CDs as fluorescence sensors, the blue or green fluorescence emission of CDs restricts further applications of CDs, particularly in the biologyrelevant fields due to the commonly blue auto-fluorescence of biological matrix. Therefore, the preparation of CDs with strong emission at long wavelengths is highly desirable, but this task had rarely been achieved so far [1,14–16]. The localized surface plasmon resonance (LSPR) of noble metals can enhance the fluorescence of proximal fluorophores, named as metal-enhanced fluorescence (MEF), when a fluorophore has to be placed in close proximity to a metal surface [17,18]. Plenty of surfaceimmobilized metallic nanostructures for MEF have been developed and the advantages of MEF include the increased photostability of fluorophores and improved detection of targets in biological fluids. These include systems made of Au [19–23], Ag [24,25], and Cu [26] with a variety of shapes. The effects with gold nanorods and nanoclusters for fluorescence enhancements of sulfonated aluminum phthalocyanine

Corresponding authors at: Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials, Hubei University, Wuhan 430062, China. E-mail addresses: [email protected] (Y. He), [email protected] (G. Song).

http://dx.doi.org/10.1016/j.talanta.2016.10.021 Received 19 July 2016; Received in revised form 15 September 2016; Accepted 2 October 2016 Available online 04 October 2016 0039-9140/ © 2016 Elsevier B.V. All rights reserved.

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2. Experimental sections

were studied in Xu's work [27]. Zhou [28] and his co-workers proposed a MEF strategy for highly sensitive detection of mercuric ions by using thymine-containing molecular beacon to tune silver nanoparticleenhanced fluorescence. We are interested in direct utilization of Ag to induce the near-infrared fluorescence of CDs to develop label-free biosensors for detecting biomarkers. Here we fabricated the silver-carbon dot nanohybrid as the labelfree biosensor for biomolecule. To demonstrate the proof-of-concept, we chose ascorbic acid (AA) as the target because of its vital role in lots of biochemical processes, including synthesis of collagen and hormone, scavenging free radicals, amino acid metabolism, and reducing the permeability of capillaries for enhancing immunity [29]. A lack of AA can induce oxidative damage to lipids, DNA and proteins [30,31]; thus, AA has been implicated in many chronic diseases. The detection of AA is of great importance for the early and rapid detection of these diseases. While lots of reports [33,36] for AA detection are based on the blue or green emission of the fluorescent sensors, detection of AA in biological matrixes usually suffers interference from other aromatic acids, amino acids, protein and DNA in blue or green light window on account of the auto-fluorescence of the biological matrix. Therefore, it is challenging to detect AA in biological matrixes selectively without the aid of a separation procedure [32,33]. Developing a near-infrared emitting sensor for AA detection may reduce interference from biological matrix. In this work, a novel silver-carbon dot nanohybrid (Ag-CD nanohybrid) was developed for sensitive and selective detection of AA in biological fluids. A facile straightforward and extra-reductant needless method was established to fabricate silver-carbon nanohybrid with enhanced near-infrared fluorescence through MEF. In addition, an IMPLICATION logic gate was constructed based on the unique characteristics of Ag-CD nanohybrid which presaged more opportunities for application in single and multiple biological sensing.

2.1. Reagents Sodium hydroxide (NaOH), ascorbic acid (AA) and ferric chloride hexahydrate (FeCl3·6H2O) were purchased from Sinopharm Chemical Reagent Co., Ltd (Shanghai, China). Glucose (C6H12O6) and silver nitrate (AgNO3) were purchased from Aladdin Chemical Co., Ltd (Shanghai, China). Magnesium sulfate (MgSO4), ethanol (C2H5OH) and hydrochloric acid (HCl) were purchased from Shanghai No.4 Reagent & H.V. Chemical Co., Ltd (Shanghai, China), Bodi Chemical Holding Co., Ltd. (Tianjin, China), Dongda Industry Co., Ltd (Shanxi, China), respectively. All used reagents were of analytical grade. Human serum samples were collected from healthy laboratory volunteers at the college hospital, and urine samples were collected from healthy humans in our laboratory. All solutions were freshly prepared before use.

2.2. Instruments Transmission electron microscopy (TEM) images were obtained on a Tecnai G20 microscope (FEI, America). High resolution transmission electron microscopy (HRTEM) images and energy dispersive X-ray spectroscopy (EDX) chemical mapping were performed on JEM2100UHR STEM/EDS (JEOL, Japan). Fourier-transform infrared (FT-IR) spectra were recorded on FTIR spectrophotometer (Perkin Elmer, America). UV–vis absorption spectra (UV–vis) were performed on Lamber 35 UV spectrometer (Perkin Elmer, America). The fluorescence measurements were recorded on LS55 fluorescence spectrometer (Perkin Elmer, America). X-ray diffraction (XRD) patterns were recorded by a D8 Advance diffractometer (Bruker, Germany). Ultrasonic treatment was reacted on SK2210LHC (Kudos, China).

Fig. 1. TEM images of CDs (a) and Ag-CD nanohybrid (b). HRTEM images of CDs (c) and Ag-CD nanohybrid (d).

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2.6. Sensitive and selective fluorescent detection of AA by Ag-CD nanohybrid

2.3. Preparation of CDs The CDs were prepared by a preview report [34]. In a typical experimental procedure, amounts of glucose was added into deionized water (100 mL) to form a clear and homogeneous solution (1 M) under stirring. NaOH (1 M, 100 mL) solution was added into the above glucose solution, and then the mixed solution was ultrasonicated for 3 h. The obtained products were adjusted to pH 7 by HCl, and then added 100 mL ethanol into the solution under stirring. In addition, the solution was treated by amounts of MgSO4 (10–20 wt%), stirred for 20 min and stored for 24 h to remove the salts and water. Finally, the obtained carbon dots were dispersed in water (with the concentration of 100 mg mL−1) for further use.

Ag-CD nanohybrid (75 μL, 2 mg mL−1) was mixed with different concentrations of AA, followed by the addition of Fe3+(50 μL, 10 mM). The solutions were diluted to a total volume of 3 mL with deionized water, respectively. After an incubation of 5 min, the fluorescence spectra of the mixture were measured upon being excited at 500 nm. 2.7. Analysis of real sample The potential application of the proposed bioassay was demonstrated by applying it to detecting AA in urine and serum samples. As the results of the experiments, the urine and serum were diluted to avoid the interference from urine and serum sample, and the dilution ratios were 40-fold and 50-fold, respectively. No sample pretreatments were used except for an appropriate dilution.

2.4. Synthesis of Ag-CD nanohybrid The Ag-CD nanohybrid was fabricated according to a published procedure [35] with a slight modification. Typically, 1.2 mL of CDs were diluted to 10 mL and treated ultrasonically for 30 min. The solution was heated to 100 ℃ and stirred for 10 min. And AgNO3 (0.15 M, 1 mL) was added into the above solution under stirring for 40 min. After that, the solution was centrifuged at 10,000 rpm for 10 min, washed several times. The deposit was dispersed in water with the concentration of 2 mg mL−1.

3. Results and discussion 3.1. Preparation and characterization of Ag-CD nanohybrid The Ag-CD nanohybrid was synthesized by mixing and refluxing CDs solution and AgNO3 solution for 40 min [35,36]. Fig. 1(a), (b) and (c), (d) displayed the TEM and HRTEM images of the CDs and Ag-CD nanohybrid, respectively. The prepared CDs and Ag-CD nanohybrid both showed good dispersion without obvious aggregation (Fig. 1(a) and (b)). Fig. 1(c) and S1(a) showed the HRTEM image and fast Fourier transform (FFT) pattern of the CDs. In Fig. 1(c), CDs was a single crystal with a lattice of 0.21 nm, in accordance with the lattice fringes of graphic carbon [37], and the size was about 2.7 nm. After the formation of Ag-CD nanohybrid, the average size of the Ag-CD nanohybrid increased to 4.6 nm. Meanwhile, it could be seen that each particle was composed of multiple single-crystalline domains in Fig. 1(d). The polycrystal symmetry also could be seen from the FFT pattern (Fig. S1(b)). The well resolved lattice fringes on the Ag-CD nanohybrid with an interplanar spacing of 0.23 nm could be indexed to

2.5. Quantum yields of CDs and Ag-CD nanohybrid [36] The quantum yields of CDs and Ag-CD nanohybrid was calculated by a slope method with Rhodamine B in ethanol solution as a reference. The quantum yield was calculated with the following equation:

Φx = Φst (Κx / Κst ) (ηst ηx )2 where Φ is quantum yield, Κ is the slope of the curve, η is the refractive index of the solvent. The subscript “st” refers to the referenced fluorophore (Rhodamine B in ethanol) with known quantum yield and “x” refers as the samples (CDs and Ag-CD nanohybrid in this work) for the determination of quantum yield.

Fig. 2. XRD spectra of CDs (a) and Ag-CD nanohybrid (b). UV–vis absorption spectra (c) and FTIR spectra (d) of CDs and Ag-CD nanohybrid.

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vibrations [40]. In the FTIR curve of Ag-CD nanohybrid, the change of O-H stretch absorption intensity in the composite sample was attributed to interactions between silver ions and hydroxyl group of CDs. The variation of the other peaks (1667, 1416, and 1031 cm−1) in the case of Ag-CD nanohybrid demonstrated the interaction between silver ions and functional groups through the formation of a coordination bond or through simple electrostatic attraction. Unlike most of previously reported CDs, the Ag-CD nanohybrid showed an excitation-dependent feature with the emission maximum at 625 nm (Fig. 4(a) and (b)). Taking Rhodamine B as a standard, the fluorescence quantum yield of Ag-CD nanohybrid under 500 nm excitation was determined to be 1.0%, while CDs had nearly no emission at 650 nm when excited at 500 nm. Fig. 3(a)–(c) showed the fluorescence emission spectra of CDs and Ag-CD nanohybrid with different excitation wavelength from 320 to 520 nm, and 320–620 nm, respectively. The naked CDs exhibited fluorescence only at visible light region, while the CDs exhibited obviously fluorescence at NIR region once modified by Ag for the nanohybrid designed with a significant scattering cross section at that wavelength. In addition, the Ag-CD nanohybrid was observed to be relatively stable emission at broad ranges of pH 4–12), high photostability under continuous irradiation by ultraviolet light, and long-term storage stability under ambient conditions (Figs. S3–S5).

the (111) plane of Ag (Fig. 1(d)). The dark Ag nanoparticles were formed nanohybrid with the low-contrast CDs (Fig. 1(d)). To further testify the CDs and Ag nanoparticles in the composite, EDX was performed. In Fig. S2(b) and (c), Ag element appeared in the Ag-CD nanohybrid only, and a high proportion of carbon bonded with a bit of silver in the nanohybrid. Those results further demonstrated the formation of Ag-CD nanohybrid. No additional reducing agent was used during the reduction process from Ag+ to Ag nanoparticles. The driving force of the spontaneous redox reaction could be attributed to the different standard reduction potential of Ag+ and oxidation potential of carbon [38]. The crystalline phase of CDs and Ag-CD nanohybrid was verified by the XRD spectrum (Fig. 2(a) and (b)). A wide peak around 24° was shown in the XRD pattern of CDs, indicating the graphite structure (002) (JCPDS No. 01–0646). After the formation of Ag-CD nanohybrid, the XRD pattern of Ag-CD nanohybrid showed four distinct diffraction peaks at 2θ=38.2°, 44.4°, 64.5° and 77.8°, which corresponded to the (111), (200), (220) and (311) crystalline planes of metallic Ag (JCPDS No. 04–0783). Fig. 2(c) showed the UV–vis absorption change of the CDs and Ag-CD nanohybrid. CDs had strong absorption at 284 nm which was attributed to n→π* transition of C=O band and π→π* transition of C=C. In the absorption curve of Ag-CD nanohybrid, the peak at 284 nm shifted to 275 nm, and a new peak at 450 nm was exhibited because of the introduction of Ag. The FTIR spectra were employed to confirm the functional groups on the surface of CDs and reveal which functional groups had played important roles in the recombination process of CDs and Ag+(Fig. 2(d)). In the FTIR curve of CDs, the peaks at 3390 cm−1 could be ascribed to the characteristic absorption of O-H stretching vibration and the peaks at 1031 cm−1 were from C-OH bending vibration. The peaks of C-H stretching vibration could be observed at about 2924 cm−1. C=O stretching vibrations were at around 1711 cm−1, while the peaks at 1667 cm−1 were resulted from the vibrations of the absorbed water molecules and the skeletal vibrations of carbon domains [39]. Peaks at 1416 cm−1 and 1360 cm−1 were assigned to the O-H or C-H bending

3.2. The feasibility of Ag-CD nanohybrid as the fluorescence sensor for AA Bestowed with superior optical properties (e.g. bright near-infrared to blue emission and high photostability), the as-prepared Ag-CD nanohybrid was proposed to serve as a potential biological probe. We designed Fe3+ as the quencher to quench the fluorescence of Ag-CD nanohybrid through electron transfer effect. Once Fe3+ was added to Ag-CD nanohybrid in the present of AA, the redox reaction between Fe3+ and AA happened prior to the electron transfer between Fe3+ and Ag-CD nanohybrid leading to no change of the fluorescence of Ag-CD

Fig. 3. Fluorescence spectra of CDs (a) and Ag-CD nanohybrid (b). (c) Normalized fluorescence spectra of Ag-CD nanohybrid. (d) Fluorescence excitation and emission Fluorescence spectra of Ag-CD nanohybrid.

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Fig. 4. Schematic illustration of AA sensor based on the fluorescent probe of Ag-CD nanohybrid adjusted with Fe3+.

Fig. 5. (a) Concentration dependence of the fluorescence behavior of Ag-CD nanohybrid in aqueous solution. (b) The quenching effect of the concentration of Fe3+ to FL intensity of AgCD nanohybrid. (c) Kinetic behavior of the FL intensity of the Ag-CD nanohybrid with the addition of Fe3+ in the present of AA. (d) The FL intensity of (1) 0.05 mg mL−1 Ag-CD nanohybrid, (2) 0.05 mg mL−1 Ag-CD nanohybrid +60 μM AA, (3) 0.05 mg mL−1 Ag-CD nanohybrid +60 μM AA +160 μM Fe3+, (4) 0.05 mg mL−1 Ag-CD nanohybrid +160 μM Fe2+ and (5) 0.05 mg mL−1 Ag-CD nanohybrid +160 μM Fe3+.(e) The FL spectra of Ag-CD nanohybrid-Fe3+ mixture with different concentrations of AA. (f) The plot of the difference fluorescence intensity change before and after quenching against the AA concentration within 0.2–60 μM.

with the concentration when the concentration was below 0.05 mg mL−1, but it decreased with the concentration when the concentration was greater than 0.05 mg mL−1. Hence, the optimal concentration of Ag-CD nanohybrid was 0.05 mg mL−1. The decrease of fluorescence intensity of Ag-CD nanohybrid at high concentration was caused by self-absorption [41]. Fig. 5(b) indicated the effect of the concentration of Fe3+ on the degree of quenching. The degree of

nanohybrid. Therefore, we fabricated the sensor for AA based on the redox reaction between Fe3+ and AA (Fig. 4). Compared with previously published methods, that this sensor detected AA in near-infrared window could reduce interference from the real sample matrix efficiently. To optimize the AA detection, several different conditions were investigated (Fig. 5(a)–(c)). As shown in Fig. 5(a), the fluorescence intensity of Ag-CD nanohybrid increased

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Table 1 Comparison of this work with other fluorescent probes for AA detection.

Table 3 Analytical results for real samples (n=5).

Method

Analytical range (μmol/L)

Detection limit (nmol/L)

Reference

Samples

Spiked (μM)

Found (μM)

Recovery (%)

RSD (%)

Carbon dots Fe3+-functionalized carbon quantum dots Cr(VI) modulated graphene quantum dots Au nanoclusters Tris-derived carbon dots Carbon quantum dotsMnO2 Carbon quantum dots/ AuNCs nanohybrid Cu nanoclusters Carbon dots Carbon dots PbS quantum dots-Au nanoclusters nanohybrid Silver-carbon dot nanohybrid

30–100 0.1–50

/ 9.1

[36] [43]

0.5–250

0.28

[44]

0.5 5 40 0.5

0.46 ± 0.06 5.19 ± 0.18 39.06 ± 0.84 0.52 ± 0.05

92.00 103.8 97.66 104.00

8.83 1.91 1.50 5.44

5

5.32 ± 1.31

106.4

1.21

5–100 0.1–20 0.18–90

/ 50 42

[33] [45] [46]

Urine sampleⅠ Urine sampleⅠ Urine sampleⅠ Human serum sample Ⅰ Human serum sample Ⅰ Human serum sample Ⅰ

40

39.31 ± 2.6

98.28

4.33

0.15–15

105

[47]

0.5–10 136–227 98–1250 3–40

110 / / 1500

[48] [49] [50] [51]

0.2–60

25

This work

The selectivity of Ag-CD nanohybrid towards AA was studied. The interference of common molecule and ions were studied under the optimum experimental conditions, and the results were shown in Table 2. The results exposed that most of the molecules or ions induced little interference with the sensor for AA detection. In order to explore the utility of the sensor, this Ag-CD nanohybrid was studied in the real samples. An appropriate dilution was applied to avoid the inference from urine samples and serum samples. The dilution ratios were 40-fold and 50-fold, respectively. The method was further validated by spiking recoveries of AA in the three parallel samples. The analytical results were illustrated in Table 3. It was obvious that the results are satisfactory. Recoveries within 92–106% were achieved, indicating the accuracy and reliability of the present method and its suitability in routine analysis.

quenching increased with the increasing of the concentration of Fe3+ when the concentration of Fe3+ was below 160 μM, and changed slightly while the concentration of Fe3+ was more than 160 μM, which manifested a quenching saturation of Fe3+ was 160 μM. The effect of incubation time was investigated and the optimal incubation time was 5 min (in Fig. 5(c)). The fluorescence intensity of Ag-CD nanohybrid was more than 95% of its original intensity in the presence of AA and Fe3+ in Fig. 5(d). In a control experiment only contained AA, an ignorable effect on the fluorescence intensity of Ag-CD nanohybrid was caused. Meanwhile, the reversibility of the fluorescence quenching was also evaluated (in Fig. S6). The fluorescence intensity of Ag-CD nanohybrid quenched by Fe3+ failed to recover, even in the presence of 10-fold concentration of AA. This phenomenon indicated the irreversible electron transfer reaction between Fe3+ and Ag-CD nanohybrid. As shown in Fig. 5(e), the quenched fluorescence intensity of Ag-CD nanohybrid by Fe3+ reduced gradually with the increasing concentration of AA. As indicated in Fig. 5(f), the fluorescence intensity versus the AA concentration was linear over a concentration range of 0.2– 60 μM with a limit of detection of 25 nM, and the equation was ΔF=3.42+0.6471C (R2=0.986), where C was the concentration of AA (μM), ΔF was the degree of quenching of the Ag-CD nanohybrid-Fe3+ system in the presence of AA. To our knowledge, the linear range and the limit of detection were lower than the recently reported by other fluorescent chemosensors of AA detection (in Table 1) [33,36,43–51].

3.3. Molecular logic gates based on Ag-CD nanohybrid On the basis of the phenomenon that the fluorescence of Ag-CD nanohybrid was quenched by Fe3+, and protected in the presence of AA, IMPLICATION logic gate was developed to show the potential of the sensor for multiplexed detection of analytes. IMPLICATION is ‘A implies B’ or ‘if A, then B’ [42]. It indicated competition of sensor AgCD nanohybrid and AA towards Fe3+. Fe3+ and AA were used as inputs and the fluorescence intensity of Ag-CD nanohybrid at 650 nm as output in Fig. 6. For input, the presence of Fe3+ or AA was as ‘1’ and their absence as ‘0’. ‘1’ signed maximum fluorescence and ‘0’ as corresponding quenching response for output. The fluorescence quenched significantly and giving an output signal of ‘0’ only in the presence of input 1 and absence of input 2. In order to investigate the selectivity of this logic gate, urea was tested as the interfering analyte, and the result was shown in Fig. S7. This IMPLICATION logic gate could be used to reflect the relative concentration of the quencher and the target analyte.

Table 2 Effect of co-existing substances on the FL intensity of Ag-CD nanohybrid-Fe3+ with 20 μM AA. Coexisting substances +

K Na+ NH4+ Ca2+ Mg2+ Ba2+ Mn2+ Cd2+ Ce3+ Pb2+ Fe2+ Zn2+ Cu2+ Hg2+

Concentration (μM) 4000 12,000 60 100 60 500 120 250 60 150 60 10 60 60

ΔF/F0 (%)

Coexisting substances

Concentration (μM)

ΔF/F0 (%)

4.0 2.5 3.7 2.9 4.5 4.1 4.5 4.1 4.1 −4.9 4.5 3.6 4.1 4.4

SO42-

20,000 120 60 2500 60 200 120 600 60 1200 2300 120 1200 60

4.4 0.2 4.3 4.0 4.6 4.4 4.7 3.1 4.7 −3.6 −4.5 −2.1 3.6 4.6

HPO4− Ac− NO3− EDTA Phenylalanine Lysine Glucose Glutamic acid Aspartic acid Threonine Arginne Urea Glutathione

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Fig. 6. The truth table for IMPLICATION logic gate; operational working of output logic gate.

4. Conclusion [13]

In summary, Ag-CD nanohybrid, a facile nanomaterial which has near-infrared to blue tunable emission, was successfully fabricated through MEF and was applied to sense AA which is a typical antioxidant in near-infrared window. The sensing mechanism was based on the competition between Ag-CD nanohybrid and AA to Fe3+. Benefit from the unique characteristics of the probe, an IMPLICATION logic gate was proposed which provided potential applications in further sensing.

[14]

[15]

[16]

Acknowledgements

[17]

This work was financially supported by the Natural Science Foundation of Hubei Province (2015CFB273, 2011CDB059 and 2011CDA111).

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Appendix A. Supporting information

[20]

[18]

[21]

Supplementary data associated with this article can be found in the online version at doi:10.1016/j.talanta.2016.10.021.

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