CN110041923A - A kind of preparation method and application of fluorescent carbon quantum dot Phe-CDs - Google Patents
A kind of preparation method and application of fluorescent carbon quantum dot Phe-CDs Download PDFInfo
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- G01N21/6428—Measuring fluorescence of fluorescent products of reactions or of fluorochrome labelled reactive substances, e.g. measuring quenching effects, using measuring "optrodes"
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Abstract
The invention discloses the preparation method and applications of fluorescent carbon quantum dot Phe-CDs a kind of, belong to carbon quantum dot technical field.Citric acid and phenylalanine are dissolved into water and obtain mixed solution A by the present invention；10~50h of mixed solution A hydro-thermal reaction is obtained into Phe-CDs solution；Phe-CDs solution is dialysed through dialysis membrane, is drying to obtain fluorescent carbon quantum dot Phe-CDs powder.For the present invention using phenylalanine and citric acid as synthesis material, one-step synthesis emits blue-fluorescence and the high novel carbon quantum dot of fluorescence intensity, and may be implemented to Fe3+Highly selective detection.
Description
Technical field
The present invention relates to the preparation method and applications of fluorescent carbon quantum dot Phe-CDs a kind of, belong to carbon quantum dot technology neck
Domain.
Background technique
Most commonly used fluorescent nano material is that quantum dot (QDs) quantum dot has exciting light in function nano material
Spectrum width and continuously distributed, and emission spectrum is narrow and symmetrical, Color tunable, the superior fluorescent characteristic such as photochemical stability height, is
A kind of ideal fluorescence probe.Current quantum dot mainly based on sulfide, selenides and tellurides, but such quantum dot because
Relevant environmental problem can also be caused to organism nocuousness containing toxic elements such as heavy metals, so that limiting quantum clicks through one
The application study of step.
Carbon quantum dot (CDs) is the novel carbon nanomaterial of one kind of discovered in recent years, has phase with semiconductor-quantum-point
The environmentally friendly fluorescent nano material of quasi-optical energy, size is in 10nm hereinafter, being that Xu etc. had found for the first time in 2004
A kind of unknown fluorescence carbon nanomaterial.Its property and carbon have apparent difference, and carbon is a kind of atrament, is shone weak, water-soluble
Property it is weak, and carbon quantum dot (CDs) has good water-soluble and bright fluorescence.And carbon material is usually non-toxic to life entity
Or hypotoxicity, the toxicity and latency environment harmfulness of other materials quantum dot can be overcome.With traditional semiconductor-quantum-point and
Organic dyestuff is compared, and the CQDs that shines has highly-water-soluble, extensive chemical stability, is easy to functionalization, is anti-light Bleachability and excellent
Biological nature, good biocompatibility, biomedical aspect have potential application prospect.
The shortcomings that prior art:
At present there are many methods of synthesis CQDs, but its technology of preparing is still immature, and there are some urgently to be resolved to ask
The level of semiconductor-quantum-point has not yet been reached in topic, such as fluorescence quantum yield, is subject to certain restrictions.Therefore carbon quantum dot is improved
Synthetic method has certain research significance with the excellent carbon quantum dot of environmentally protective method synthesising property.
Summary of the invention
The technical issues of for the synthesis of carbon quantum dot in the prior art, the present invention proposes a kind of fluorescent carbon quantum dot Phe-
The preparation method of CDs, the present invention is using phenylalanine and citric acid as synthesis material, and one-step synthesis emits blue-fluorescence and fluorescence is strong
High novel carbon quantum dot is spent, and may be implemented to Fe3+Highly selective detection.
A kind of preparation method of fluorescent carbon quantum dot Phe-CDs, the specific steps are as follows:
(1) citric acid and phenylalanine are dissolved into water and obtain mixed solution A；
(2) step (1) 10~50h of mixed solution A hydro-thermal reaction is obtained into Phe-CDs solution；
(3) step (2) Phe-CDs solution is dialysed through dialysis membrane, is drying to obtain fluorescent carbon quantum dot Phe-CDs powder.
The concentration of citric acid is 5~15mmol/L in step (1) mixed solution A.
The concentration of phenylalanine is 5~15mmol/L in step (1) mixed solution A.
The temperature of step (2) hydro-thermal reaction is 120~220 DEG C.
The molecule interception of step (3) dialysis membrane is 500~1000kDa.
The dialysis membrane dialysis time be 6~for 24 hours.
The rate of the centrifugal treating is 6000~10000rpm, and the centrifugal treating time is 10~30min.
Fluorescent carbon quantum dot of the present invention can be used for Fe3+Carry out quantitative analysis detection.
Beneficial effects of the present invention:
(1) carbon quantum dot (Phe-CDs) of the present invention using hydrothermal synthesis method one-step synthesis transmitting fluorescence, synthetic method
Simply, synthesis material is easy to get, environmentally friendly pollution-free；
(2) the carbon quantum dot good light stability of the method for the present invention synthesis, fluorescence intensity are high；
(3) for the present invention using phenylalanine and citric acid as synthesis material, one-step synthesis emits blue-fluorescence and fluorescence intensity
High novel carbon quantum dot, and may be implemented to Fe3+Highly selective detection.
Detailed description of the invention
Fig. 1 is 1 Phe-CDs fluorescence excitation-emission spectrogram of embodiment；
Fig. 2 is 1 Phe-CDs uv absorption spectra of embodiment；
Fig. 3 is 1 Phe-CDs transmission electron microscope of embodiment；
Fig. 4 is the infrared absorpting light spectra of 1 Phe-CDs of embodiment；
Fig. 5 is the fluorescence intensity change after embodiment 1Phe-CDs various Action of Metal Ions identical with concentration；
Fig. 6 is the Fe of embodiment 1Phe-CDs and various concentration3+Fluorescence intensity change after effect.
Specific embodiment
Invention is further described in detail combined with specific embodiments below, but protection scope of the present invention is not limited to
The content.
Embodiment 1:
A kind of preparation method of fluorescent carbon quantum dot Phe-CDs, the specific steps are as follows:
(1) citric acid and phenylalanine are dissolved into water and obtain mixed solution A；Wherein citric acid in mixed solution A
Concentration is 5mmol/L, and the concentration of phenylalanine is 8mmol/L；
(2) by step (1) mixed solution A be placed in temperature be 180 DEG C under the conditions of hydro-thermal reaction 30h in the UV lamp show indigo plant
Color fluorescence obtains Phe-CDs solution；
(3) step (3) Phe-CDs solution is dialysed 6h through dialysis membrane, re-dry is up to flaxen fluorescent carbon quantum dot
Phe-CDs powder；Wherein the molecule interception of dialysis membrane is 1000 Da；The rate of centrifugal treating is 6000rpm, centrifugal treating
Time is 10min；
The present embodiment fluorescent carbon quantum dot Phe-CDs fluorescence excitation-emission spectrogram is shown in Fig. 1, and wherein abscissa represents wave
Long, ordinate represents fluorescence intensity；From fig. 1, it can be seen that the maximum excitation wavelength of Phe-CDs is 335nm, maximum emission wavelength is
440nm；
The present embodiment fluorescent carbon quantum dot Phe-CDs uv absorption spectra is shown in Fig. 2, and wherein abscissa represents wavelength, indulges
Coordinate represents absorption intensity；As can be seen from Figure 2, citric acid is without obvious absorption peaks, and phenylalanine is due to containing phenyl ring near 255nm
There is a characteristic absorption peak, and Phe-CDs then shows strong absworption peak near 250nm, it was demonstrated that citric acid and phenylalanine occur
Reaction generates novel substance；
The present embodiment fluorescent carbon quantum dot Phe-CDs transmission electron microscope is shown in Fig. 3, and as can be seen from Figure 3, the partial size of Phe-CDs is general
For 5nm；
The infrared absorpting light spectra of the present embodiment fluorescent carbon quantum dot Phe-CDs is shown in Fig. 4, as can be seen from Figure 4, Phe-CDs's
Infrared spectrum shows that there are different functional groups.3300~2800cm-1: peak shape is wide, dissipates, is attributed to the O-H stretching vibration of carboxylic acid
With the stretching vibration of N-H；1713.05cm-1: strong narrow peak, peak shape is sharply C=O stretching vibration；1318.59cm-1: Qiang Feng, peak
Shape is sharply C-H bending vibration:；1173.71cm-1: middle Qiang Fengwei C-N stretching vibration；752.27cm-1And 700.86cm-1:C-H
Deformation vibration and the vibration of phenyl ring framework deformation.According to the infrared spectrum of Phe-CDs can tentatively judge wherein exist-COOH ,-
The functional groups such as NH2, phenyl ring；
Selectivity test of the carbon quantum dot to metal ion:
The flaxen fluorescent carbon quantum dot Phe-CDs powder for taking the present embodiment, is add to deionized water and is configured to
The fluorescent carbon quantum dot Phe-CDs solution of 5mg/mL takes 200 μ L fluorescent carbon quantum dot Phe-CDs solution to be added to 1.5mL respectively
In centrifuge tube, then it is separately added into the different metal ions solution of 50 μ L, 10mmol/L, vibrates 30s, divide after placing response 30min
Its fluorescence spectrum is not measured；
Fluorescence intensity change after the present embodiment Phe-CDs various Action of Metal Ions identical with concentration as shown in figure 5,
Wherein abscissa represents each metal ion species, and ordinate represents relative intensity of fluorescence, as can be known from Fig. 5, Fe3+It can make Phe-
The fluorescence of CDs generates apparent Quenching, and is added after other metal ions then without significant change, and Phe-CDs is shown
To Fe3+With highly selective；
Detection of the carbon quantum dot to the folic acid of various concentration:
The flaxen fluorescent carbon quantum dot Phe-CDs powder for taking the present embodiment, is add to deionized water and is configured to
The fluorescent carbon quantum dot Phe-CDs solution of 5mg/mL takes 200 μ L fluorescent carbon quantum dot Phe-CDs solution to be added to 1.5mL respectively
In centrifuge tube, then it is separately added into the Fe of various concentration3+Solution vibrates 30s, measures its fluorescence light respectively after placing response 30min
Spectrum；
The Fe of the present embodiment Phe-CDs and various concentration3+Fluorescence intensity change after effect is as shown in fig. 6, wherein horizontal seat
Mark represents Fe3+Concentration, ordinate represent fluorescence intensity, as can be known from Fig. 6, with the Fe of addition3+The increase of concentration, Phe-CDs
Fluorescence gradually weaken.
Embodiment 2:
A kind of preparation method of fluorescent carbon quantum dot Phe-CDs, the specific steps are as follows:
(1) citric acid and phenylalanine are dissolved into water and obtain mixed solution A；Wherein citric acid in mixed solution A
Concentration is 5mmol/L, and the concentration of phenylalanine is 10mmol/L；
(2) by step (1) mixed solution A be placed in temperature be 180 DEG C under the conditions of hydro-thermal reaction 30h in the UV lamp show indigo plant
Color fluorescence obtains Phe-CDs solution；
(3) step (3) Phe-CDs solution is dialysed 6h through dialysis membrane, re-dry is up to flaxen fluorescent carbon quantum dot
Phe-CDs powder；Wherein the molecule interception of dialysis membrane is 1000 Da；The rate of centrifugal treating is 6000rpm, centrifugal treating
Time is 10min；
Selectivity test of the carbon quantum dot to metal ion:
The flaxen fluorescent carbon quantum dot Phe-CDs powder for taking the present embodiment, is add to deionized water and is configured to
The fluorescent carbon quantum dot Phe-CDs solution of 5mg/mL takes 200 μ L fluorescent carbon quantum dot Phe-CDs solution to be added to 1.5mL respectively
In centrifuge tube, then it is separately added into the different metal ions solution of 50 μ L, 10mmol/L, vibrates 30s, divide after placing response 30min
Its fluorescence spectrum is not measured；
Fluorescence intensity change after the present embodiment Phe-CDs various Action of Metal Ions identical with concentration is it is found that Fe3+Energy
So that the fluorescence of Phe-CDs is generated apparent Quenching, and is added after other metal ions then without significant change, Phe-
CDs is shown to Fe3+With highly selective；
Detection of the carbon quantum dot to the folic acid of various concentration:
The flaxen fluorescent carbon quantum dot Phe-CDs powder for taking the present embodiment, is add to deionized water and is configured to
The fluorescent carbon quantum dot Phe-CDs solution of 5mg/mL takes 200 μ L fluorescent carbon quantum dot Phe-CDs solution to be added to 1.5mL respectively
In centrifuge tube, then it is separately added into the Fe of various concentration3+Solution vibrates 30s, measures its fluorescence light respectively after placing response 30min
Spectrum；
The Fe of the present embodiment Phe-CDs and various concentration3+Fluorescence intensity change after effect it is found that with addition Fe3+
The fluorescence of the increase of concentration, Phe-CDs gradually weakens.
Embodiment 3:
A kind of preparation method of fluorescent carbon quantum dot Phe-CDs, the specific steps are as follows:
(1) citric acid and phenylalanine are dissolved into water and obtain mixed solution A；Wherein citric acid in mixed solution A
Concentration is 5mmol/L, and the concentration of phenylalanine is 12mmol/L；
(2) by step (1) mixed solution A be placed in temperature be 180 DEG C under the conditions of hydro-thermal reaction 30h in the UV lamp show indigo plant
Color fluorescence obtains Phe-CDs solution；
(3) step (3) Phe-CDs solution is dialysed 6h through dialysis membrane, re-dry is up to flaxen fluorescent carbon quantum dot
Phe-CDs powder；Wherein the molecule interception of dialysis membrane is 1000kDa；The rate of centrifugal treating is 6000rpm, centrifugal treating
Time is 10min；
Selectivity test of the carbon quantum dot to metal ion:
The flaxen fluorescent carbon quantum dot Phe-CDs powder for taking the present embodiment, is add to deionized water and is configured to
The fluorescent carbon quantum dot Phe-CDs solution of 5mg/mL takes 200 μ L fluorescent carbon quantum dot Phe-CDs solution to be added to 1.5mL respectively
In centrifuge tube, then it is separately added into the different metal ions solution of 50 μ L, 10mmol/L, vibrates 30s, divide after placing response 30min
Its fluorescence spectrum is not measured；
Fluorescence intensity change after the present embodiment Phe-CDs various Action of Metal Ions identical with concentration is it is found that Fe3+Energy
So that the fluorescence of Phe-CDs is generated apparent Quenching, and is added after other metal ions then without significant change, Phe-
CDs is shown to Fe3+With highly selective；
Detection of the carbon quantum dot to the folic acid of various concentration:
The flaxen fluorescent carbon quantum dot Phe-CDs powder for taking the present embodiment, is add to deionized water and is configured to
The fluorescent carbon quantum dot Phe-CDs solution of 5mg/mL takes 200 μ L fluorescent carbon quantum dot Phe-CDs solution to be added to 1.5mL respectively
In centrifuge tube, then it is separately added into the Fe of various concentration3+Solution vibrates 30s, measures its fluorescence light respectively after placing response 30min
Spectrum；
The Fe of the present embodiment Phe-CDs and various concentration3+Fluorescence intensity change after effect it is found that with addition Fe3+
The fluorescence of the increase of concentration, Phe-CDs gradually weakens.
Embodiment 4:
A kind of preparation method of fluorescent carbon quantum dot Phe-CDs, the specific steps are as follows:
(1) citric acid and phenylalanine are dissolved into water and obtain mixed solution A；Wherein citric acid in mixed solution A
Concentration is 8mmol/L, and the concentration of phenylalanine is 10mmol/L；
(2) by step (1) mixed solution A be placed in temperature be 160 DEG C under the conditions of hydro-thermal reaction 30h in the UV lamp show indigo plant
Color fluorescence obtains Phe-CDs solution；
(3) step (3) Phe-CDs solution is dialysed 6h through dialysis membrane, re-dry is up to flaxen fluorescent carbon quantum dot
Phe-CDs powder；Wherein the molecule interception of dialysis membrane is 1000kDa；The rate of centrifugal treating is 6000rpm, centrifugal treating
Time is 10min；
Selectivity test of the carbon quantum dot to metal ion:
The flaxen fluorescent carbon quantum dot Phe-CDs powder for taking the present embodiment, is add to deionized water and is configured to
The fluorescent carbon quantum dot Phe-CDs solution of 5mg/mL takes 200 μ L fluorescent carbon quantum dot Phe-CDs solution to be added to 1.5mL respectively
In centrifuge tube, then it is separately added into the different metal ions solution of 50 μ L, 10mmol/L, vibrates 30s, divide after placing response 30min
Its fluorescence spectrum is not measured；
Fluorescence intensity change after the present embodiment Phe-CDs various Action of Metal Ions identical with concentration is it is found that Fe3+Energy
So that the fluorescence of Phe-CDs is generated apparent Quenching, and is added after other metal ions then without significant change, Phe-
CDs is shown to Fe3+With highly selective；
Detection of the carbon quantum dot to the folic acid of various concentration:
The flaxen fluorescent carbon quantum dot Phe-CDs powder for taking the present embodiment, is add to deionized water and is configured to
The fluorescent carbon quantum dot Phe-CDs solution of 5mg/mL takes 200 μ L fluorescent carbon quantum dot Phe-CDs solution to be added to 1.5mL respectively
In centrifuge tube, then it is separately added into the Fe of various concentration3+Solution vibrates 30s, measures its fluorescence light respectively after placing response 30min
Spectrum；
The Fe of the present embodiment Phe-CDs and various concentration3+Fluorescence intensity change after effect it is found that with addition Fe3+
The fluorescence of the increase of concentration, Phe-CDs gradually weakens.
Embodiment 5:
A kind of preparation method of fluorescent carbon quantum dot Phe-CDs, the specific steps are as follows:
(1) citric acid and phenylalanine are dissolved into water and obtain mixed solution A；Wherein citric acid in mixed solution A
Concentration is 8mmol/L, and the concentration of phenylalanine is 10mmol/L；
(2) by step (1) mixed solution A be placed in temperature be 200 DEG C under the conditions of hydro-thermal reaction 30h in the UV lamp show indigo plant
Color fluorescence obtains Phe-CDs solution；
(3) step (3) Phe-CDs solution is dialysed 6h through dialysis membrane, re-dry is up to flaxen fluorescent carbon quantum dot
Phe-CDs powder；Wherein the molecule interception of dialysis membrane is 1000 Da；The rate of centrifugal treating is 6000rpm, centrifugal treating
Time is 10min；
Selectivity test of the carbon quantum dot to metal ion:
The flaxen fluorescent carbon quantum dot Phe-CDs powder for taking the present embodiment, is add to deionized water and is configured to
The fluorescent carbon quantum dot Phe-CDs solution of 5mg/mL takes 200 μ L fluorescent carbon quantum dot Phe-CDs solution to be added to 1.5mL respectively
In centrifuge tube, then it is separately added into the different metal ions solution of 50 μ L, 10mmol/L, vibrates 30s, divide after placing response 30min
Its fluorescence spectrum is not measured；
Fluorescence intensity change after the present embodiment Phe-CDs various Action of Metal Ions identical with concentration is it is found that Fe3+Energy
So that the fluorescence of Phe-CDs is generated apparent Quenching, and is added after other metal ions then without significant change, Phe-
CDs is shown to Fe3+With highly selective；
Detection of the carbon quantum dot to the folic acid of various concentration:
The flaxen fluorescent carbon quantum dot Phe-CDs powder for taking the present embodiment, is add to deionized water and is configured to
The fluorescent carbon quantum dot Phe-CDs solution of 5mg/mL takes 200 μ L fluorescent carbon quantum dot Phe-CDs solution to be added to 1.5mL respectively
In centrifuge tube, then it is separately added into the Fe of various concentration3+Solution vibrates 30s, measures its fluorescence light respectively after placing response 30min
Spectrum；
The Fe of the present embodiment Phe-CDs and various concentration3+Fluorescence intensity change after effect it is found that with addition Fe3+
The fluorescence of the increase of concentration, Phe-CDs gradually weakens.
Embodiment 6:
A kind of preparation method of fluorescent carbon quantum dot Phe-CDs, the specific steps are as follows:
(1) citric acid and phenylalanine are dissolved into water and obtain mixed solution A；Wherein citric acid in mixed solution A
Concentration is 8mmol/L, and the concentration of phenylalanine is 10mmol/L；
(2) by step (1) mixed solution A be placed in temperature be 180 DEG C under the conditions of hydro-thermal reaction 40h in the UV lamp show indigo plant
Color fluorescence obtains Phe-CDs solution；
(3) step (3) Phe-CDs solution is dialysed 6h through dialysis membrane, re-dry is up to flaxen fluorescent carbon quantum dot
Phe-CDs powder；Wherein the molecule interception of dialysis membrane is 1000kDa；The rate of centrifugal treating is 6000rpm, centrifugal treating
Time is 10min；
Selectivity test of the carbon quantum dot to metal ion:
The flaxen fluorescent carbon quantum dot Phe-CDs powder for taking the present embodiment, is add to deionized water and is configured to
The fluorescent carbon quantum dot Phe-CDs solution of 5mg/mL takes 200 μ L fluorescent carbon quantum dot Phe-CDs solution to be added to 1.5mL respectively
In centrifuge tube, then it is separately added into the different metal ions solution of 50 μ L, 10mmol/L, vibrates 30s, divide after placing response 30min
Its fluorescence spectrum is not measured；
Fluorescence intensity change after the present embodiment Phe-CDs various Action of Metal Ions identical with concentration is it is found that Fe3+Energy
So that the fluorescence of Phe-CDs is generated apparent Quenching, and is added after other metal ions then without significant change, Phe-
CDs is shown to Fe3+With highly selective；
Detection of the carbon quantum dot to the folic acid of various concentration:
The flaxen fluorescent carbon quantum dot Phe-CDs powder for taking the present embodiment, is add to deionized water and is configured to
The fluorescent carbon quantum dot Phe-CDs solution of 5mg/mL takes 200 μ L fluorescent carbon quantum dot Phe-CDs solution to be added to 1.5mL respectively
In centrifuge tube, then it is separately added into the Fe of various concentration3+Solution vibrates 30s, measures its fluorescence light respectively after placing response 30min
Spectrum；
The Fe of the present embodiment Phe-CDs and various concentration3+Fluorescence intensity change after effect it is found that with addition Fe3+
The fluorescence of the increase of concentration, Phe-CDs gradually weakens.
Claims (7)
1. a kind of preparation method of fluorescent carbon quantum dot Phe-CDs, which is characterized in that specific step is as follows:
(1) citric acid and phenylalanine are dissolved into water and obtain mixed solution A；
(2) step (1) 10~50h of mixed solution A hydro-thermal reaction is obtained into Phe-CDs solution；
(3) step (2) Phe-CDs solution is dialysed through dialysis membrane, is drying to obtain fluorescent carbon quantum dot Phe-CDs powder.
2. the preparation method of fluorescent carbon quantum dot Phe-CDs according to claim 1, it is characterised in that: step (1) mixing
The concentration of citric acid is 5~15mmol/L in solution A.
3. the preparation method of fluorescent carbon quantum dot Phe-CDs according to claim 2, it is characterised in that: step (1) mixing
The concentration of phenylalanine is 5~15mmol/L in solution A.
4. the preparation method of fluorescent carbon quantum dot Phe-CDs according to claim 1, it is characterised in that: step (2) hydro-thermal is anti-
The temperature answered is 120~220 DEG C.
5. the preparation method of fluorescent carbon quantum dot Phe-CDs according to claim 1, it is characterised in that: step (3) dialysis membrane
Molecule interception be 500~1000kDa.
6. the preparation method of fluorescent carbon quantum dot Phe-CDs according to claim 5, it is characterised in that: when dialysis membrane is dialysed
Between for 6~for 24 hours.
7. fluorescent carbon quantum dot prepared by the preparation method of any one of the claim 1~6 fluorescent carbon quantum dot Phe-CDs
Phe-CDs is to Fe3+Carry out the application in quantitative analysis detection.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2021087646A1 (en) * | 2019-11-04 | 2021-05-14 | Beijing Normal University | Carbon quantum dots and uses thereof |
| CN113845906A (en) * | 2021-10-27 | 2021-12-28 | 南京师范大学 | Synthesis and application of nitrogen-doped carbon quantum dot fluorescent probe |
| CN114410300A (en) * | 2022-01-30 | 2022-04-29 | 安徽大学 | Fluorescent probe and preparation method and biological application thereof |
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| CN113845906A (en) * | 2021-10-27 | 2021-12-28 | 南京师范大学 | Synthesis and application of nitrogen-doped carbon quantum dot fluorescent probe |
| CN114410300A (en) * | 2022-01-30 | 2022-04-29 | 安徽大学 | Fluorescent probe and preparation method and biological application thereof |
| CN114410300B (en) * | 2022-01-30 | 2023-04-21 | 安徽大学 | Fluorescent probe and preparation method and biological application thereof |
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