A test paper for rapidly detecting beryllium based on fluorescence and a preparation method, detection method and application thereof

Abstract

The application discloses a test paper for rapidly detecting beryllium elements based on fluorescence and a preparation method, a detection method and application thereof. The detection method for the beryllium elements comprises the following steps: S1, wetting and sampling the test paper for rapidly detecting beryllium elements based on fluorescence, and adjusting pH; obtaining a sample to be detected; wherein the test paper for rapidly detecting beryllium elements based on fluorescence comprises filter paper base material, fluorescent molecules and shielding agent disodium ethylenediaminetetraacetate; S2, collecting a fluorescent signal on the sample to be detected, and obtaining the content of beryllium elements in the sample to be detected according to a standard curve. When the detection object is a surface, the detection method for the beryllium elements has high sensitivity, short time consumption, good specificity, simple operation, low cost and low detection limit, and does not need pretreatment.

Description

Technical Field

[0001] This invention relates to a test strip for rapid detection of beryllium based on fluorescence, its preparation method, detection method, and application. Background Technology

[0002] Beryllium is a lightweight, corrosion-resistant metal widely used in aerospace, nuclear industry, and other fields. However, beryllium is extremely toxic and carcinogenic; inhalation of beryllium particles can cause chronic beryllosis and even death, and skin contact can lead to sensitization. Therefore, monitoring the surface beryllium concentration in beryllium-related work environments is crucial. However, traditional detection methods such as inductively coupled plasma mass spectrometry (ICP-MS) and inductively coupled plasma atomic emission spectrometry (ICP-AES) have drawbacks such as long detection times and complex operating procedures.

[0003] Therefore, there is an urgent need to develop a method for detecting beryllium content that is time-efficient and easy to operate. Summary of the Invention

[0004] The technical problem this invention aims to solve is to overcome the shortcomings of existing methods for detecting beryllium content on the surface of an object, which suffer from long detection times and complex operation procedures. This invention provides a fluorescence-based rapid detection test strip for beryllium, along with its preparation method, detection method, and applications. When the object to be detected is a surface, the beryllium detection method of this invention offers high sensitivity, short detection time, good specificity, simple operation, no pretreatment required, low cost, and a low detection limit.

[0005] The present invention solves the above-mentioned technical problems through the following technical solution:

[0006] This invention provides a method for detecting beryllium, comprising the following steps:

[0007] S1. Wet and sample the test paper for rapid fluorescence detection of beryllium, and adjust the pH to obtain the sample to be tested; wherein the test paper for rapid fluorescence detection of beryllium includes filter paper substrate, fluorescent molecules and the shielding agent disodium ethylenediaminetetraacetate;

[0008] S2. Collect the fluorescence signal on the sample to be tested, and determine the beryllium content of the sample to be tested based on the standard curve.

[0009] In S1 of the present invention, the filter paper substrate may be a qualitative filter paper of Whatman Grade 1, preferably a qualitative filter paper of Whatman Grade 1 with a diameter of 1-3 cm, more preferably a qualitative filter paper of Whatman Grade 1 with a diameter of 2.5 cm, such as Whatman Grade 1 1001-325 or Whatman Grade 1 1001-025.

[0010] In S1 of this invention, the fluorescent molecule can be of the conventional type in the art, preferably including one or more of 10-hydroxybenzo[h]quinoline-7-sulfonate, morin, and dibromohydroxyphenylfluorescein, such as morin.

[0011] In S1 of this invention, wetting refers to the state where the test paper for rapid fluorescence detection of beryllium is just completely soaked, and the wetting liquid does not drip off when lifted. Preferably, after wetting, the water content of the test paper for rapid fluorescence detection of beryllium is 0.05-0.15 mL of wetting liquid / 5 cm. 2 The test strip, such as the fluorescent rapid detection test strip for beryllium, has a water content of 0.1 mL of wetting solution / 5 cm. 2 Test strips.

[0012] In S1 of the present invention, the wetting method can be conventional in the art, preferably by using an aqueous solution of an inorganic solvent, such as water, 5% ammonia water or 2% nitric acid aqueous solution.

[0013] In a preferred embodiment, the wetting step includes: spraying 0.1 mL of water onto the fluorescence-based rapid detection test strip for beryllium, and transferring it between two test strips with a diameter larger than the beryllium detection test strip, pressing to remove excess water.

[0014] In S1 of this invention, the sampling method can be conventional in the art, and preferably includes the following steps: pressing the wetted test paper based on rapid fluorescence detection of beryllium onto the sampling surface and slowly wiping the sampling surface.

[0015] The surface area of ​​the sample is preferably 50-150 cm². 2 For example, 100 cm 2 .

[0016] The sampling method preferably includes: sampling from top to bottom in a "Z" shape, with the wiping process covering the entire sampling surface, and / or sampling from left to right in a "Z" shape, perpendicular to the previous wiping direction.

[0017] In S1 of this invention, the endpoint of pH adjustment can be the pH at which the fluorescent molecules in the fluorescence-based rapid beryllium detection test paper and the beryllium element can undergo a complexation reaction. Preferably, the pH of the fluorescence-based rapid beryllium detection test paper is adjusted to 8-12, for example, 9, 10, or 11. The method of adjusting the pH of the fluorescence-based rapid beryllium detection test paper to 10 can be conventional in the art, preferably including: spraying 0.1 ml of an ammonia-ammonium chloride buffer solution with a pH of 10 onto the fluorescence-based rapid beryllium detection test paper.

[0018] In a preferred embodiment, the preparation method of the ammonia-ammonium chloride buffer solution with pH 10 includes: weighing 5.45g of ammonium chloride, dissolving it in ultrapure water, adding 35ml of ammonia water, and diluting to a volumetric flask of 100ml.

[0019] In S2 of this invention, preferably, the fluorescence signal on the sample to be tested is acquired using a surface fluorescence acquisition device. The surface fluorescence acquisition device can be of a type conventional in the art, for example, consisting of a 405nm semiconductor laser, a transmission optical fiber, a fixed sample stage, a long-pass filter, and a fiber optic spectrometer.

[0020] In S2 of this invention, the method for preparing the standard curve includes the following steps:

[0021] (1) Add at least two beryllium standard solutions of different mass concentrations to the wetted test paper based on rapid fluorescence detection of beryllium, adjust the pH, and obtain the standard test paper;

[0022] (2) Collect the fluorescence signal on the standard test paper, prepare standard points, and obtain a standard curve.

[0023] The beryllium standard solutions of different mass concentrations are preferably eight different concentration gradients, such as 0.1 μg / mL, 0.25 μg / mL, 0.5 μg / mL, 1 μg / mL, 2.5 μg / mL, 5 μg / mL, 10 μg / mL and 25 μg / mL.

[0024] In a preferred embodiment, the standard curve is prepared as follows: 0.1 ml of beryllium standard solutions with mass concentrations of 0.1 μg / mL, 0.25 μg / mL, 0.5 μg / mL, 1 μg / mL, 2.5 μg / mL, 5 μg / mL, 10 μg / mL, and 25 μg / mL are respectively added to the wetted beryllium-based rapid fluorescence detection test paper, and the pH is adjusted to obtain standard test paper; then, the fluorescence signals on the standard test paper are collected to prepare standard points, and the standard curve is obtained.

[0025] In this invention, preferably, the method for detecting beryllium does not require pretreatment of the sample. The pretreatment method can be conventional in the art, such as digestion and / or extraction.

[0026] In this invention, the method for detecting beryllium is preferably used to detect the beryllium content on the surface of a sample.

[0027] This invention provides a test strip for rapid detection of beryllium based on fluorescence, comprising a filter paper substrate, fluorescent molecules, and a shielding agent, disodium ethylenediaminetetraacetate; the fluorescent molecules and the shielding agent, disodium ethylenediaminetetraacetate, are loaded on the filter paper substrate.

[0028] In this invention, the filter paper substrate can be a qualitative filter paper of Whatman Grade 1, preferably a qualitative filter paper of Whatman Grade 1 with a diameter of 1-3 cm, more preferably a qualitative filter paper of Whatman Grade 1 with a diameter of 2.5 cm, such as Whatman Grade 1 1001-325 or Whatman Grade 1 1001-025.

[0029] In this invention, the fluorescent molecules can be of conventional types in the art, preferably including one or more of 10-hydroxybenzo[h]quinoline-7-sulfonate, morin, and dibromohydroxyphenylfluorescein, such as morin.

[0030] In this invention, the shielding agent, disodium ethylenediaminetetraacetate, can prevent interference from metal ions other than beryllium ions. The other metal ions can be one or more of Al, Fe, Ni, Pb, Mg, Cu, and Cr.

[0031] This invention provides a method for preparing a test strip for rapid fluorescence detection of beryllium as described above, comprising the following steps:

[0032] S1. The filter paper substrate is immersed in a fluorescent molecule solution to obtain the first test paper;

[0033] S2. Immerse the first test paper in a solution of disodium ethylenediaminetetraacetate (EDTA) as a shielding agent to obtain the test paper for rapid detection of beryllium based on fluorescence.

[0034] In S1 of this invention, the mass concentration of the fluorescent molecule solution is preferably 0.001%-0.2%, more preferably 0.002%-0.15%, for example 0.005%, 0.01%, 0.02%, 0.05%, 0.1%, or 0.2%. The mass concentration represents the percentage of the mass of the fluorescent molecules in the mass of the fluorescent molecule solution. The fluorescent molecule solution preferably comprises fluorescent molecules and a solvent. The solvent can be of a type conventional in the art, such as ethanol.

[0035] In a preferred embodiment, the mass concentration of the fluorescent molecule solution is 0.1%, and the preparation method includes: weighing 0.1 g of fluorescent molecules into a 100 ml volumetric flask and making up to volume with ethanol.

[0036] In S1 of this invention, the endpoint of the impregnation can be that the filter paper substrate reaches a saturated state in the fluorescent molecule solution. Saturation means that even if the impregnation time of the filter paper substrate is further extended, the filter paper substrate will not absorb the fluorescent molecule solution.

[0037] In S1 of this invention, after immersing the filter paper substrate in the fluorescent molecule solution, it is preferable to further perform a process to remove excess fluorescent molecule solution. The method for removing excess fluorescent molecule solution can be conventional in the art, such as immersing the filter paper substrate in the fluorescent molecule solution, transferring it between two filter papers with a diameter larger than the filter paper substrate, pressing to remove excess fluorescent molecule solution, and then allowing it to air dry.

[0038] In S2 of this invention, the mass concentration of the shielding agent disodium ethylenediaminetetraacetate solution can be conventional in the art, preferably 0.5%-5%, more preferably 0.8%-3%, for example 1%. The mass concentration represents the percentage of the mass of the shielding agent disodium ethylenediaminetetraacetate in the shielding agent solution relative to the mass of the shielding agent itself. The shielding agent disodium ethylenediaminetetraacetate solution preferably comprises the shielding agent disodium ethylenediaminetetraacetate and a solvent. The type of solvent can be conventional in the art, such as water.

[0039] In a preferred embodiment, the mass concentration of the shielding agent disodium ethylenediaminetetraacetate solution is 1%, and the preparation method includes: weighing 1g of disodium ethylenediaminetetraacetate into a 100ml volumetric flask and making up to volume with ultrapure water.

[0040] In S2 of this invention, the endpoint of the impregnation can be that the first test paper reaches saturation in the disodium ethylenediaminetetraacetate (EDTA) solution. Saturation means that even if the impregnation time of the first test paper is further extended, the first test paper will not absorb the EDTA solution.

[0041] In S2 of this invention, after immersing the first test paper in a solution of the shielding agent disodium ethylenediaminetetraacetate (EDTA), it is preferable to further perform a process to remove excess EDTA solution. The method for removing excess EDTA solution can be conventional in the art, for example, after immersing the first test paper in the EDTA solution, transferring it between two filter papers with a diameter larger than the first test paper and pressing to remove excess EDTA solution, followed by natural drying.

[0042] The present invention also provides a method for detecting beryllium as described above, or the application of the fluorescence-based rapid beryllium detection test strip as described above in the field of beryllium contamination detection.

[0043] In this invention, the beryllium contamination detection field is preferably the beryllium contamination surface detection field.

[0044] Based on common knowledge in the field, the above-mentioned preferred conditions can be combined arbitrarily to obtain various preferred embodiments of the present invention.

[0045] The reagents and raw materials used in this invention are all commercially available.

[0046] The positive and progressive effects of this invention are as follows:

[0047] (1) In this invention, the test paper for rapid detection of beryllium based on fluorescence includes a filter paper substrate, fluorescent molecules, and a shielding agent, disodium ethylenediaminetetraacetate. In this test paper, the shielding agent, disodium ethylenediaminetetraacetate, can bind with interfering metal ions that may exist on the sampling surface, preventing interfering metal ions from occupying the complexation sites of the fluorescent molecules and ensuring that the fluorescent molecules are complexed with beryllium ions.

[0048] (2) The fluorescence-based rapid detection test strip for beryllium prepared in this invention has high sensitivity and can be used for surface beryllium collection and content detection. It exhibits good linearity in the range of 0.05 μg-2.5 μg, R0 2 >0.99, good specificity, simple operation, low cost, and low detection limit (detection limit 0.002 μg / 100 cm⁻¹). 2 ).

[0049] (3) The beryllium detection method of the present invention is simple to operate, time-saving and low in cost. Attached Figure Description

[0050] Figure 1 The image shows the characteristic peak shape of beryllium on the surface of a contaminated object detected using the beryllium detection method described in Example 1.

[0051] Figure 2 The image shows the characteristic peak intensity results of beryllium detection on the surface of a contaminated object using the beryllium detection method described in Example 1.

[0052] Figure 3 This is a standard curve diagram for detecting beryllium on the surface of a contaminated object using the beryllium detection method described in Example 1.

[0053] Figure 4 This is a standard curve diagram for detecting beryllium on the surface of a contaminated object using the beryllium detection method described in Example 2.

[0054] Figure 5 The relative fluorescence intensity of the test paper changes under different pH conditions.

[0055] Figure 6 The images show the fluorescence intensity results obtained when the test strips for rapid fluorescence detection of beryllium prepared in Examples 1, 2, and 7-13 were used to detect objects with the same beryllium content.

[0056] Figure 7 This is a graph showing the reliability results of the beryllium detection method of this application. Detailed Implementation

[0057] The present invention will be further illustrated by way of embodiments below, but the present invention is not limited to the scope of the embodiments described herein.

[0058] Example 1

[0059] 1. Preparation of a fluorescence-based rapid detection test strip for beryllium:

[0060] (1) Select Whatman Grade 11001-325 standard qualitative filter paper with a diameter of 2.5cm as the filter paper substrate;

[0061] (2). Prepare a 0.1% (w / w) solution of fluorescent molecular morin: Weigh 0.1 g of fluorescent molecular morin into a 100 ml volumetric flask and dilute to volume with ethanol;

[0062] (3) Preparation of a 1% disodium ethylenediaminetetraacetate solution: Weigh 1g of disodium ethylenediaminetetraacetate into a 100ml volumetric flask and dilute to volume with ultrapure water;

[0063] (4) The above filter paper substrate is immersed in a 0.1% (w / w) solution of fluorescent morin until saturated. It is then transferred between two 7cm diameter filter papers and pressed to remove excess morin solution. The paper is then air-dried in a fume hood to obtain the first test paper. The first test paper is then immersed in a 1% (w / w) solution of disodium ethylenediaminetetraacetate until saturated. It is then transferred between two 7cm diameter filter papers and pressed to remove excess disodium ethylenediaminetetraacetate solution. The paper is then air-dried in a fume hood. This yields the test paper for rapid fluorescence detection of beryllium.

[0064] 2. Methods for detecting beryllium:

[0065] (1) Wet the test paper for rapid fluorescence detection of beryllium so that it can dissolve 100% of the beryllium on the sampling surface: Spray 0.1 ml of water onto the test paper for rapid fluorescence detection of beryllium, transfer it between two 7 cm diameter filter papers and press to remove excess water;

[0066] (2). Beryllium surface sampling: Press the wetted test paper from (1) onto the sampling surface (100 cm). 2 Within the box, slowly wipe the sampling surface. First, take samples from top to bottom in a "Z" shape, covering the entire sampling surface during the wiping process. Then, take samples from left to right in a "Z" shape, perpendicular to the previous wiping direction.

[0067] (3). Adjust the pH of the test paper: Spray 0.1 ml of ammonia-ammonium chloride buffer solution with pH 10 onto the test paper. After 1 minute, collect the intensity signal on the filter paper using a surface fluorescence collection device.

[0068] The preparation method of the ammonia-ammonium chloride buffer solution with pH 10 is as follows: Weigh 5.45g of ammonium chloride, dissolve it in ultrapure water, add 35ml of ammonia water, and dilute to a volumetric flask of 100ml. The area of ​​the excitation light spot of the surface fluorescence acquisition device is larger than the area of ​​the test paper, so that all fluorescence signals on the surface of the test paper can be collected. During acquisition, the excitation wavelength is 405nm, the excitation power is 60mW, and the spectrometer exposure time is 90ms. The emission spectrum of the beryllium-morin complex on the test paper is collected, and the peak in the 470-520nm band is integrated to obtain the fluorescence intensity of the beryllium-morin complex. The results are as follows. Figure 1 and Figure 2 As shown, Figure 1 and Figure 2 During the reaction, the fluorescence signal rapidly increased after 3 minutes, gradually forming the characteristic fluorescence peak of the beryllium-morin complex at 495 nm. At 9 minutes, the fluorescence signal intensity of the beryllium-morin complex reached its maximum, the peak shape stabilized without significant change, and the intensity remained stable without significant change. Furthermore, within the range of 9-60 minutes, the fluorescence signal intensity change did not exceed 3%, making it stable for quantitative detection. This indicates that the fluorescence signal of the beryllium-morin complex stabilized within 9 minutes, allowing for quantitative testing. In summary, this method can achieve rapid and accurate quantitative detection of beryllium within 10 minutes.

[0069] The surface fluorescence acquisition device consists of a 405nm semiconductor laser, a transmission optical fiber, a fixed sample stage, a long-pass filter, and a fiber optic spectrometer. During operation, the 405nm semiconductor laser excites the sample surface via the incident optical fiber, causing the analyte to emit fluorescence; the emitted fluorescence is then collected by the same optical fiber. To suppress the influence of scattered excitation light peaks and improve the signal-to-noise ratio of fluorescence detection, a 405nm long-pass filter is installed in the fluorescence transmission optical path to filter out residual excitation scattered light. After the fluorescence signal is transmitted to the spectrometer via the optical fiber, spectral acquisition is completed across the entire wavelength range of 200-900 nm. During detection, the distance between the transmitting and receiving optical fibers and the sample surface can be flexibly adjusted to control the size of the incident light spot, ensuring that the excitation spot completely covers the test area, allowing the sample to be fully and uniformly excited, thereby obtaining stable and accurate fluorescence spectral detection results.

[0070] (4) Determine the beryllium content on the test strip based on the standard curve;

[0071] The standard curve was prepared as follows: 0.1 ml of beryllium standard solutions with concentrations of 0.1 μg / mL, 0.25 μg / mL, 0.5 μg / mL, 1 μg / mL, 2.5 μg / mL, 5 μg / mL, 10 μg / mL, and 25 μg / mL were added to moistened test paper, and the pH was adjusted to obtain standard test papers with concentrations of 0.01 μg / mL, 0.025 μg / mL, 0.05 μg / mL, 0.1 μg / mL, 0.25 μg / mL, 0.5 μg / mL, 1 μg / mL, and 2.5 μg / mL. Subsequently, fluorescence signals on the standard test papers were collected to prepare standard points, thus generating the standard curve, as shown below. Figure 3 As shown; Figure 3 The horizontal axis represents the beryllium content on the test strip (unit: μg), and the vertical axis represents the relative fluorescence intensity. The linear regression equation between the relative fluorescence intensity y and the beryllium content x is y = 0.3822x + 0.0458. It can be seen that this method exhibits a good linear relationship (R²) within the beryllium content range of 0.01-2.5 μg. 2 > 0.99).

[0072] Furthermore, under the same experimental conditions, the blank test strip was subjected to 7 independent parallel measurements. The standard deviation of three times the 7 measurements divided by the slope of the standard curve was the detection limit of 0.002 μg.

[0073] Example 2

[0074] The only difference from Example 1 is that the mass concentration of the fluorescent molecule mulberry pigment solution is 0.01%; the preparation method is as follows: weigh 0.01g of fluorescent molecule mulberry pigment into a 100ml volumetric flask and dilute to volume with ethanol;

[0075] The standard curve was prepared as follows: 0.1 mL of beryllium standard solutions with concentrations of 0.1 μg / mL, 0.25 μg / mL, 0.5 μg / mL, 1 μg / mL, 2.5 μg / mL, and 5 μg / mL were added to moistened test paper, and the pH was adjusted to obtain standard test papers with concentrations of 0.01 μg / mL, 0.025 μg / mL, 0.05 μg / mL, 0.1 μg / mL, 0.25 μg / mL, and 0.5 μg / mL, respectively. Subsequently, fluorescence signals on the standard test papers were collected to prepare standard points, thus generating the standard curve. Figure 4 As shown; Figure 4 The horizontal axis represents the beryllium content on the test strip (unit: μg), and the vertical axis represents the relative fluorescence intensity. The linear regression equation between the relative fluorescence intensity y and the beryllium content x is y = 1.9583x + 0.002. It can be seen that within the beryllium content range of 0.01-0.5 μg, this method exhibits a good linear relationship (R²). 2 > 0.99); the detection limit was 0.002 μg.

[0076] Example 3

[0077] The only difference from Example 1 is that the pH of the test strip is adjusted to 8.

[0078] Example 4

[0079] The only difference from Example 1 is that the pH of the test strip is adjusted to 9.

[0080] Example 5

[0081] The only difference from Example 1 is that the pH of the test strip is adjusted to 11.

[0082] Example 6

[0083] The only difference from Example 1 is that the pH of the test strip is adjusted to 12.

[0084] The fluorescence signals obtained in Examples 1 and 3-6 at different pH values ​​were compared, and the results are as follows: Figure 5 As shown in the figure, the red curve represents the relative fluorescence signal of the beryllium-loaded test paper after reacting with morin, while the blue curve represents the background relative fluorescence signal of the blank test paper without beryllium. The results show that the relative fluorescence signal of the beryllium-morin complex is strongest at pH 11; however, the background signal of the blank test paper also reaches its maximum value at the same time. At pH 10, although the fluorescence signal of the target analyte decreases to 60% of the pH 11 peak, the background signal intensity is only one-eighth of the former. Considering both signal response and detection limit, the buffer solution at pH 10 is the most effective.

[0085] Example 7

[0086] The only difference from Example 1 is that the mass concentration of fluorescent molina in the fluorescent molina solution is 0.002%.

[0087] Example 8

[0088] The only difference from Example 1 is that the mass concentration of fluorescent molina in the fluorescent molina solution is 0.005%.

[0089] Example 9

[0090] The only difference from Example 1 is that the mass concentration of fluorescent molina in the fluorescent molina solution is 0.01%.

[0091] Example 10

[0092] The only difference from Example 1 is that the mass concentration of fluorescent molina in the fluorescent molina solution is 0.02%.

[0093] Example 11

[0094] The only difference from Example 1 is that the mass concentration of fluorescent molina in the fluorescent molina solution is 0.05%.

[0095] Example 12

[0096] The only difference from Example 1 is that the mass concentration of fluorescent molina in the fluorescent molina solution is 0.1%.

[0097] Example 13

[0098] The only difference from Example 1 is that the mass concentration of fluorescent molina in the fluorescent molina solution is 0.2%.

[0099] When the fluorescence-based rapid detection test strips for beryllium prepared in Examples 1, 2, and 7-13 were used to detect objects with the same beryllium content, the obtained fluorescence intensity was as follows: Figure 6 As shown in the table below. Figure 6 In the fluorescent molecule morin solution, with a mass concentration of morin between 0.001% and 0.01%, the fluorescence signal intensity increases with increasing morin concentration. When the mass concentration of morin in the solution exceeds 0.01%, the fluorescence signal weakens with increasing morin concentration. Although the fluorescence intensity of the test strip treated with 0.1% morin is weaker than that treated with 0.01% morin, its linear detection range is wider.

[0100]

[0101] Example 1

[0102] A series of test paper samples with different concentrations (n=20) were taken, and the beryllium content in them was first determined using the detection method in Example 1. Then, the test paper was digested, and the digested solution was quantitatively analyzed using inductively coupled plasma mass spectrometry (ICP-MS, Thermo Fisher iCAP MSX).

[0103] The digestion method was as follows: The test paper was placed in a digestion tube, and 10 mL of a 20% (w / w) nitric acid solution was added to completely submerge the test paper. The digestion tube was then placed on a graphite heating plate and heated at 90°C for 10 min to ensure complete dissolution of the elements adsorbed on the test paper. After naturally cooling to room temperature, the digestion solution was brought to a final volume of 50 mL and then analyzed by ICP-MS.

[0104] Comparison of detection results of two methods for 20 groups of samples Figure 7As shown, the average relative deviation between the beryllium detection method of this application and the ICP-MS method is 7.4%. This demonstrates that the beryllium detection method of this application has better reliability and operational stability.

[0105] While specific embodiments of the present invention have been described above, those skilled in the art should understand that these are merely illustrative examples, and the scope of protection of the present invention is defined by the appended claims. Those skilled in the art can make various changes or modifications to these embodiments without departing from the principles and essence of the present invention, but all such changes and modifications fall within the scope of protection of the present invention.

Claims

1. A method for detecting beryllium, characterized in that, It includes the following steps: S1. Wet and sample the test paper for rapid fluorescence detection of beryllium, and adjust the pH to obtain the sample to be tested; wherein the test paper for rapid fluorescence detection of beryllium includes filter paper substrate, fluorescent molecules and the shielding agent disodium ethylenediaminetetraacetate; S2. Collect the fluorescence signal on the sample to be tested, and determine the beryllium content of the sample to be tested based on the standard curve.

2. The method for detecting beryllium as described in claim 1, characterized in that, The method for detecting beryllium satisfies one or more of the following conditions: (1) In S1, the filter paper substrate is a qualitative filter paper of type Whatman Grade 1, preferably a qualitative filter paper of type Whatman Grade 1 with a diameter of 1-3cm, more preferably a qualitative filter paper of type Whatman Grade 1 with a diameter of 2.5cm, such as Whatman Grade 1 1001-325 or Whatman Grade 1 1001-025; (2) In S1, the fluorescent molecule includes one or more of 10-hydroxybenzo[h]quinoline-7-sulfonate, morin and dibromohydroxyphenylfluorescein, for example morin; (3) In S1, the wetting method is to wet with an aqueous solution of an inorganic solvent, such as water, 5% ammonia water or 2% nitric acid aqueous solution; (4) In S1, the sampling method includes the following steps: pressing the wetted test paper based on rapid fluorescence detection of beryllium onto the sampling surface and slowly wiping the sampling surface.

3. The method for detecting beryllium as described in claim 1, characterized in that, In S1, the endpoint of pH adjustment is the pH at which the fluorescent molecules in the fluorescence-based rapid detection test paper for beryllium can undergo a complexation reaction with the beryllium element. Preferably, the pH of the fluorescence-based rapid detection test paper for beryllium is adjusted to 8-12, such as 9, 10 or 11.

4. The method for detecting beryllium as described in claim 2, characterized in that, The method for detecting beryllium satisfies one or more of the following conditions: (1) The surface area of ​​the sample is preferably 50-150 cm². 2 For example, 100 cm 2 ; (2) The sampling methods include: sampling from top to bottom in a "Z" shape, the wiping process should cover the entire sampling surface, and / or sampling from left to right in a "Z" shape, perpendicular to the previous wiping movement direction.

5. The method for detecting beryllium as described in claim 1, characterized in that, The method for detecting beryllium satisfies one or more of the following conditions: (1) In S2, the method for preparing the standard curve includes the following steps: ① Add at least two beryllium standard solutions of different mass concentrations to the wetted fluorescent rapid detection beryllium test paper, adjust the pH, and obtain the standard test paper; ② Collect the fluorescence signal on the standard test strip, prepare standard points, and obtain a standard curve; The beryllium standard solutions of different mass concentrations are preferably eight different concentration gradients, such as 0.1 μg / mL, 0.25 μg / mL, 0.5 μg / mL, 1 μg / mL, 2.5 μg / mL, 5 μg / mL, 10 μg / mL and 25 μg / mL; (2) The method for detecting beryllium does not require pretreatment of the sample to be tested; the pretreatment method is, for example, digestion and / or extraction; (3) The method for detecting beryllium is used to detect the beryllium content on the surface of a sample.

6. A test strip for rapid detection of beryllium based on fluorescence, characterized in that, It includes a filter paper substrate, fluorescent molecules, and a shielding agent, disodium ethylenediaminetetraacetate; the fluorescent molecules and the shielding agent, disodium ethylenediaminetetraacetate, are loaded on the filter paper substrate.

7. The test strip for rapid fluorescence detection of beryllium as described in claim 6, characterized in that, The test strip for rapid fluorescence detection of beryllium meets the following conditions (1) and / or (2): (1) The filter paper substrate is a qualitative filter paper of type Whatman Grade 1, preferably a qualitative filter paper of type Whatman Grade 1 with a diameter of 1-3cm, more preferably a qualitative filter paper of type Whatman Grade 1 with a diameter of 2.5cm, such as Whatman Grade 1 1001-325 or Whatman Grade 1 1001-025; (2) The fluorescent molecules include one or more of 10-hydroxybenzo[h]quinoline-7-sulfonate, morin and dibromohydroxyphenylfluorescein, such as morin.

8. A method for preparing a test strip for rapid fluorescence detection of beryllium as described in claim 6 or 7, characterized in that, It includes the following steps: S1. The filter paper substrate is immersed in a fluorescent molecule solution to obtain the first test paper; S2. Immerse the first test paper in a solution of disodium ethylenediaminetetraacetate (EDTA) as a shielding agent to obtain the test paper for rapid detection of beryllium based on fluorescence.

9. The method for preparing the test strip for rapid fluorescence detection of beryllium as described in claim 8, characterized in that, The method for preparing the fluorescence-based rapid detection test strip for beryllium meets one or more of the following conditions: (1) In S1, the mass concentration of the fluorescent molecule solution is preferably 0.001%-0.2%, preferably 0.002%-0.15%, for example 0.005%, 0.01%, 0.02%, 0.05%, 0.1% or 0.2%; the mass concentration represents the percentage of the mass of the fluorescent molecules to the mass of the fluorescent molecule solution; The fluorescent molecule solution includes fluorescent molecules and a solvent, such as ethanol. (2) In S1, the endpoint of the impregnation is that the filter paper substrate is saturated in the fluorescent molecule solution; (3) In S2, the mass concentration of the shielding agent disodium ethylenediaminetetraacetate solution is 0.5%-5%, more preferably 0.8%-3%, for example 1%; the mass concentration represents the percentage of the mass of the shielding agent disodium ethylenediaminetetraacetate in the shielding agent solution relative to the mass of the shielding agent. (4) In S2, the endpoint of the impregnation is when the first test paper is saturated in the solution of the shielding agent ethylenediaminetetraacetic acid disodium salt.

10. A method for detecting beryllium as described in any one of claims 1-5, or the application of the fluorescence-based rapid beryllium detection test strip as described in claim 6 or 7 in the field of beryllium contamination detection.

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