CN113499790A - Preparation and application of Ag-doped CdSe nanosheet photocatalytic material separated by uranium reduction - Google Patents
Preparation and application of Ag-doped CdSe nanosheet photocatalytic material separated by uranium reduction Download PDFInfo
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Abstract
The invention discloses a preparation and application of an Ag-doped CdSe nanosheet photocatalytic material separated by uranium reduction, which comprises the following steps: adding CdCl2·2.5H2O and AgNO3Mixing the mixed powder with a first mixed solvent of octylamine and oleylamine, heating for reaction, and cooling to room temperature to obtain a reaction solution; mixing Se powder with a second mixed solvent of octylamine and oleylamine at room temperature to obtain a Se precursor solution; adding Se precursor solution into the reaction solutionAnd heating for reaction, cooling, washing the obtained precipitate for multiple times by using a trichloromethane solution, uniformly mixing the precipitate with a hexadecyl trimethyl ammonium bromide solution, performing ultrasonic treatment, washing with ethanol, and drying to obtain the Ag-doped CdSe nanosheet photocatalytic material subjected to uranium reduction and separation. The Ag-doped CdSe nanosheet photocatalytic material provided by the invention can improve the light absorption capacity and simultaneously meet the photocatalytic reduction of U (VI), and is more beneficial to generation and use of photon-generated carriers.
Description
Technical Field
The invention belongs to the technical field of organic and inorganic nano materials and preparation thereof, and particularly relates to preparation and application of an Ag-doped CdSe nanosheet photocatalytic material separated by uranium reduction.
Background
Nuclear energy is a relatively clean energy source, and has developed rapidly over the past decades, in contrast to traditional fossil fuels, which cause severe environmental pollution and climate change. However, the reserves of uranium ore that have been explored on land are limited. Due to the widespread use of nuclear power, large-scale uranium mining, nuclear accidents, and improper disposal of nuclear waste, large quantities of radioactive uranium permeate the environment, mainly in the form of hexavalent uranium (u (vi)). Therefore, U (VI) extraction is also required while environmental monitoring and protection. However, there are a number of technical difficulties in extracting uranium from uranium-containing waste streams due to interference from low uranium concentrations and large numbers of coexisting ions. At present, a photocatalytic uranium reduction method is a new green and environment-friendly method, but the photocatalytic performance of a semiconductor is influenced by factors such as light absorption wavelength and material stability. Finding suitable band structures and high extraction amount of photocatalyst is still a challenge for extracting U (VI) in uranium-containing wastewater.
The invention takes CdSe nano-sheets with narrow band gaps as research objects, the original CdSe nano-sheets are the combination of two crystal structures of sphalerite and wurtzite, and the crystal structures of the CdSe nano-sheets are adjusted by doping a small amount of Ag, so that the CdSe nano-sheets are mainly based on the sphalerite crystal structures. The change of the crystal structure reduces the band gap width of the CdSe nanosheet, and simultaneously meets the requirements of U (VI) photocatalytic reduction, so that the light absorption wavelength range of the 3% Ag-CdSe nanosheet is enlarged, and the generation and utilization of photon-generated carriers are facilitated.
Disclosure of Invention
An object of the present invention is to solve at least the above problems and/or disadvantages and to provide at least the advantages described hereinafter.
To achieve these objects and other advantages in accordance with the present invention, there is provided a method for preparing an Ag-doped CdSe nanosheet photocatalytic material separated by uranium reduction, comprising the steps of:
step one, CdCl2·2.5H2O and AgNO3The mixed powder is uniformly mixed with a first mixed solvent of octylamine and oleylamine, the mixture is heated to 115-125 ℃ and then reacts for 1-3 hours, and the mixture is naturally cooled to room temperature to obtain a reaction solution;
step two, uniformly mixing Se powder with a second mixed solvent of octylamine and oleylamine at room temperature to obtain a Se precursor solution;
and step three, adding the Se precursor solution in the step two into the reaction solution in the step one, heating to 90-100 ℃, reacting for 14-18 hours, cooling to room temperature, washing the obtained precipitate for multiple times by using a trichloromethane solution, uniformly mixing the precipitate with a hexadecyl trimethyl ammonium bromide solution, performing ultrasonic treatment for 45-90 min, washing the precipitate for multiple times by using ethanol, and performing vacuum drying to obtain the Ag-doped CdSe nanosheet photocatalytic material.
Preferably, in the first step, CdCl2·2.5H2O and AgNO3The molar ratio of (A) to (B) is 1.4-1.5: 0.01-0.035; the volume ratio of the octylamine to the oleylamine is 1: 1; the molar volume ratio of the mixed powder to the first mixed solvent is 1.5mmol:10 mL.
Preferably, in the second step, the molar volume ratio of the Se powder to the second mixed solvent is 4.5 mmol: 5 mL; the volume ratio of the octylamine to the oleylamine is 1: 1; and the molar ratio of the Se powder to the mixed powder in the second step is 2.5-3.5: 1.
Preferably, in the third step, the concentration of the cetyl trimethyl ammonium bromide solution is 0.05-0.15 mol/L; the molar volume ratio of the mixed powder in the first step to the cetyl trimethyl ammonium bromide solution is 1.5mmol: 25-45 mL.
Preferably, in the third step, the process of uniformly mixing the precipitate and the cetyl trimethyl ammonium bromide solution and then performing ultrasonic treatment for 45-90 min is replaced by: adding the precipitate and a cetyl trimethyl ammonium bromide solution into a supercritical carbon dioxide reaction device, injecting carbon dioxide into the supercritical carbon dioxide reaction device, stirring for 15-30 min under the conditions that the temperature is 35-40 ℃ and the pressure is 12-18 MPa, relieving the pressure, and then carrying out ultrasound for 15-30 min; and washing the precipitate with ethanol for multiple times, and drying in vacuum to obtain the Ag-doped CdSe nanosheet photocatalytic material.
Preferably, in the third step, the obtained Ag-doped CdSe nanosheet photocatalytic material is treated for 1-3 min by using a low-temperature plasma treatment instrument.
Preferably, the atmosphere of the low-temperature plasma processor is argon; the frequency of the low-temperature plasma treatment instrument is 35-45 KHz, the power is 45-60W, and the pressure of the atmosphere is 30-45 Pa.
The invention also provides application of the Ag-doped CdSe nanosheet photocatalytic material separated by uranium reduction in radioactive wastewater treatment, which is characterized in that the radioactive wastewater is uranium-containing radioactive wastewater.
Preferably, the Ag-doped CdSe nanosheet photocatalytic material is added into the uranium-containing radioactive wastewater, and a photocatalytic reaction is carried out under the condition that a xenon lamp simulates sunlight, so that the photocatalytic reduction of hexavalent uranium in the uranium-containing radioactive wastewater is realized; simultaneously, after the photocatalyst material after the photocatalytic reaction is oxidized in the air for 48 hours, the photocatalyst material is dispersed to 0.1mol/L KHCO3Elution reaction in solution to remove UO deposited on the catalyst2And then washed with water, and the collected photocatalyst material is dried and recycled.
The invention at least comprises the following beneficial effects: the Ag-doped CdSe nanosheet is prepared, the original CdSe nanosheet is a combination of sphalerite and wurtzite crystal structures, and the wurtzite crystal structures in the CdSe nanosheet are reduced along with the doping of Ag. According to the analysis of the energy band structure, the change of the crystal structure is found to reduce the band gap width of the CdSe nanosheet and improve the position of the conduction band of the CdSe nanosheet, so that the Ag-CdSe nanosheet can improve the light absorption capability and simultaneously meet the photocatalytic reduction of U (VI), and is more beneficial to the generation and use of photon-generated carriers.
Additional advantages, objects, and features of the invention will be set forth in part in the description which follows and in part will become apparent to those having ordinary skill in the art upon examination of the following or may be learned from practice of the invention.
Description of the drawings:
FIG. 1 is a TEM image of uranium reduction-separated Ag-doped CdSe nanosheet photocatalytic materials prepared in comparative example 1(a) and example 2(b) of the present invention;
FIG. 2 is HRTEM of uranium reduction separated Ag doped CdSe nanoplatelet photocatalytic materials prepared in comparative example 1(a) and example 2(b) according to the present invention;
FIG. 3 is an XRD pattern of the photocatalytic materials prepared in examples 1-2 of the present invention and comparative example 1;
FIG. 4 is a Raman spectrum of the photocatalytic materials prepared in examples 1 to 2 of the present invention and comparative example 1;
FIG. 5 is an infrared spectrum of photocatalytic materials prepared in examples 1 to 2 of the present invention and comparative example 1;
FIG. 6 is an XPS spectrum of photocatalytic materials prepared in examples 1-2 of the present invention and comparative example 1;
FIG. 7 shows a Mottky spectra (a) and a band gap value (b) of photocatalytic materials prepared in examples 1 to 2 of the present invention and comparative example 1;
FIG. 8 shows a valence band curve (a) and a secondary electron edge curve (b) of a UPS spectrum of photocatalytic materials prepared in examples 1 to 2 of the present invention and comparative example 1;
FIG. 9 is a diagram showing energy band structures of photocatalytic materials prepared in examples 1 to 2 of the present invention and comparative example 1;
FIG. 10 is a graph showing the U (VI) removal rate under dark conditions of the photocatalytic materials prepared in examples 1-2 of the present invention and comparative example 1;
FIG. 11 is a graph showing the U (VI) removal rate under light conditions of the photocatalytic materials prepared in examples 1-2 of the present invention and comparative example 1;
FIG. 12 is a graph of the U (VI) removal rate under dark conditions for photocatalytic materials prepared in examples 2-4 of the present invention;
FIG. 13 is a graph of the U (VI) removal rate under illumination of the photocatalytic materials prepared in examples 2-4 of the present invention;
FIG. 14 shows the U (VI) removal rate of the photocatalytic material prepared in example 2 of the present invention under different solid-to-liquid ratio conditions;
FIG. 15 shows the U (VI) removal rate of the photocatalytic material prepared in example 2 of the present invention in the presence of competitive ions;
FIG. 16 shows the U (VI) removal rate of the photocatalytic material prepared in example 2 under different pH conditions;
FIG. 17 shows the XPS spectra of U4 f (a), Cd3d (b), Se 3d (c), Ag 3d (d) before and after the photocatalytic reaction of the photocatalytic material prepared in example 2 of the present invention;
fig. 18 shows a valence band curve (a) and a secondary electron side curve (b) of a UPS spectrum before and after a photocatalytic reaction of the photocatalytic material prepared in example 2 according to the present invention.
The specific implementation mode is as follows:
the present invention is further described in detail below with reference to the attached drawings so that those skilled in the art can implement the invention by referring to the description text.
It will be understood that terms such as "having," "including," and "comprising," as used herein, do not preclude the presence or addition of one or more other elements or groups thereof.
Example 1:
a preparation method of an Ag-doped CdSe nanosheet photocatalytic material separated by uranium reduction comprises the following steps:
step one, 1.485mmol of CdCl2·2.5H2O and 0.015mmol AgNO3The mixed powder is uniformly mixed with 5mL of first mixed solvent of octylamine and 5mL of oleylamine, heated to 120 ℃ and reacted for 2 hours, and the reaction is naturalCooling to room temperature to obtain a reaction solution;
step two, uniformly mixing 4.5mmol of Se powder with a second mixed solvent of 2.5mL of octylamine and 2.5mL of oleylamine at room temperature to obtain a Se precursor solution;
and step three, adding the Se precursor solution in the step two into the reaction solution in the step one, heating to 95 ℃, reacting for 16 hours, cooling to room temperature, washing the obtained precipitate for 3 times by using a trichloromethane solution, uniformly mixing the precipitate with 30mL of 0.1mol/L hexadecyl trimethyl ammonium bromide solution, performing ultrasonic treatment for 60min, washing the precipitate for multiple times by using ethanol, and performing vacuum drying at 60 ℃ to obtain the Ag-doped CdSe nanosheet photocatalytic material (1% Ag-CdSe).
Example 2:
a preparation method of an Ag-doped CdSe nanosheet photocatalytic material separated by uranium reduction comprises the following steps:
step one, 1.47mmol CdCl2·2.5H2O and 0.03mmol AgNO3The mixed powder is uniformly mixed with a first mixed solvent of 5mL of octylamine and 5mL of oleylamine, the mixture is heated to 120 ℃ and then reacts for 2 hours, and the mixture is naturally cooled to room temperature to obtain a reaction solution;
step two, uniformly mixing 4.5mmol of Se powder with a second mixed solvent of 2.5mL of octylamine and 2.5mL of oleylamine at room temperature to obtain a Se precursor solution;
and step three, adding the Se precursor solution in the step two into the reaction solution in the step one, heating to 95 ℃, reacting for 16 hours, cooling to room temperature, washing the obtained precipitate for 3 times by using a trichloromethane solution, uniformly mixing the precipitate with 30mL of 0.1mol/L hexadecyl trimethyl ammonium bromide solution, performing ultrasonic treatment for 60min, washing the precipitate for multiple times by using ethanol, and performing vacuum drying at 60 ℃ to obtain the Ag-doped CdSe nanosheet photocatalytic material (3% Ag-CdSe).
Example 3:
a preparation method of an Ag-doped CdSe nanosheet photocatalytic material separated by uranium reduction comprises the following steps:
step one, 1.47mmol CdCl2·2.5H2O and 0.03mmol AgNO3Mixed powder of (5)Uniformly mixing mL of octylamine and 5mL of oleylamine first mixed solvent, heating to 120 ℃, reacting for 2 hours, and naturally cooling to room temperature to obtain a reaction solution;
step two, uniformly mixing 4.5mmol of Se powder with a second mixed solvent of 2.5mL of octylamine and 2.5mL of oleylamine at room temperature to obtain a Se precursor solution;
step three, adding the Se precursor solution in the step two into the reaction solution in the step one, heating to 95 ℃, reacting for 16 hours, cooling to room temperature, cleaning the obtained precipitate for 3 times by using a trichloromethane solution, adding the precipitate and 30mL of 0.1mol/L hexadecyl trimethyl ammonium bromide solution into a supercritical carbon dioxide reaction device, injecting carbon dioxide into the supercritical carbon dioxide reaction device, stirring for 30min under the conditions of the temperature of 38 ℃ and the pressure of 18MPa, relieving the pressure, and performing ultrasound for 30 min; then washing the precipitate with ethanol for multiple times, and drying in vacuum at 60 ℃ to obtain the Ag-doped CdSe nanosheet photocatalytic material (3% Ag-CdSe-1).
Example 4:
a preparation method of an Ag-doped CdSe nanosheet photocatalytic material separated by uranium reduction comprises the following steps:
step one, 1.47mmol CdCl2·2.5H2O and 0.03mmol AgNO3The mixed powder is uniformly mixed with a first mixed solvent of 5mL of octylamine and 5mL of oleylamine, the mixture is heated to 120 ℃ and then reacts for 2 hours, and the mixture is naturally cooled to room temperature to obtain a reaction solution;
step two, uniformly mixing 4.5mmol of Se powder with a second mixed solvent of 2.5mL of octylamine and 2.5mL of oleylamine at room temperature to obtain a Se precursor solution;
step three, adding the Se precursor solution in the step two into the reaction solution in the step one, heating to 95 ℃, reacting for 16 hours, cooling to room temperature, cleaning the obtained precipitate for 3 times by using a trichloromethane solution, adding the precipitate and 30mL of 0.1mol/L hexadecyl trimethyl ammonium bromide solution into a supercritical carbon dioxide reaction device, injecting carbon dioxide into the supercritical carbon dioxide reaction device, stirring for 30min under the conditions of the temperature of 38 ℃ and the pressure of 18MPa, relieving the pressure, and performing ultrasound for 30 min; washing the precipitate with ethanol for multiple times, vacuum drying at 60 ℃ to obtain an Ag-doped CdSe nanosheet photocatalytic material, and treating the obtained Ag-doped CdSe nanosheet photocatalytic material with a low-temperature plasma treatment instrument for 2 min; obtaining Ag-doped CdSe nanosheet photocatalytic material (3% Ag-CdSe-2); the atmosphere of the low-temperature plasma treatment instrument is argon; the frequency of the low-temperature plasma processor is 45KHz, the power is 60W, and the pressure of the atmosphere is 30 Pa;
comparative example 1:
a preparation method of a CdSe nanosheet photocatalytic material comprises the following steps:
step one, 1.5mmol CdCl2·2.5H2Uniformly mixing O with a first mixed solvent of 5mL of octylamine and 5mL of oleylamine, heating to 120 ℃, reacting for 2 hours, and naturally cooling to room temperature to obtain a reaction solution;
step two, uniformly mixing 4.5mmol of Se powder with a second mixed solvent of 2.5mL of octylamine and 2.5mL of oleylamine at room temperature to obtain a Se precursor solution;
and step three, adding the Se precursor solution in the step two into the reaction solution in the step one, heating to 95 ℃, reacting for 16 hours, cooling to room temperature, washing the obtained precipitate for 3 times by using a trichloromethane solution, uniformly mixing the precipitate with 30mL of 0.1mol/L hexadecyl trimethyl ammonium bromide solution, performing ultrasonic treatment for 60min, washing the precipitate for multiple times by using ethanol, and performing vacuum drying at 60 ℃ to obtain the Ag-doped CdSe nanosheet photocatalytic material (CdSe).
The morphology of the CdSe prepared in comparative example 1 and the 3% Ag-CdSe material prepared in example 2 was characterized, and TEM images showed that the CdSe (FIG. 1(a)) and the 3% Ag-CdSe (FIG. 1(b)) were in the form of nanosheets (FIG. 1). HRTEM image of CdSe, 3% Ag-CdSe is shown in FIG. 2. FIG. 2(a) is an HRTEM image of pristine CdSe nanoplates with lattice fringes of different orientations, where interplanar spacing of 0.37nm corresponds to the (100) plane of the wurtzite structure and 0.35nm corresponds to the (111) plane of the zincblende structure. This indicates that the original CdSe nanosheets are composed of two crystal structures, sphalerite and wurtzite. FIG. 2(b) is an HRTEM image of a 3% Ag-CdSe nanosheet, and it can be clearly seen that the 3% Ag-CdSe nanosheet has a lattice stripe in only one direction, which is a (111) plane with a interplanar spacing of 0.35nm, corresponding to the sphalerite structure of the CdSe nanosheet. This indicates that the introduction of Ag into CdSe nanosheets causes a change in the crystal structure.
The XRD pattern is shown in figure 3, the original CdSe nanosheet is a combination of two crystal structures of sphalerite (JCPDS NO.19-0191) and wurtzite (JCPDS NO.08-0459), the wurtzite crystal structure in the CdSe nanosheet is reduced along with the doping of Ag, and gradually tends to be the sphalerite crystal structure, which shows that the crystal structure of the original CdSe nanosheet can be changed by the doping of a small amount of Ag. This conclusion can also be confirmed from the raman spectrum, as shown in fig. 4, the peaks of the a region and the B region disappear with the increase of the doping amount of Ag, which indicates that the doping amount of Ag causes the change of chemical bonds, and further causes the change of the crystal structure of the CdSe nanosheet. The FT-IR spectrum of Ag-CdSe is shown in FIG. 5.
FIG. 6(a) is an Ag-CdSe nanosheet XPS total spectrum. FIG. 6(b) is an Ag-CdSe nanosheet Cd3d XPS spectrum. It can be clearly seen that the 3d peak of Cd shifts to low binding energy after Ag is doped into CdSe nanosheets, indicating that electrons on Se are partially transferred to Cd after Ag is doped. At the same time, the 3d XPS spectrum of Se also shifted toward lower binding energy with the doping of Ag, indicating that the doping of Ag lowers the electronic valence of some Se (FIG. 6 (c)). Fig. 6(d) is a Ag 3d XPS spectrum, from which it can be clearly seen that Ag has been successfully doped into CdSe nanoplates. In conclusion, the Ag-doped CdSe nanosheets are successfully synthesized, and the crystal structure of the CdSe nanosheets is changed by the small amount of Ag doping.
In the photocatalytic reduction process of U (VI), the energy required for the photocatalytic reduction of U (VI) to U (IV) is about 4.91V, generally speaking, the position of the conduction band of the semiconductor is required to be higher than 4.91V for the complete photocatalytic reduction of U (VI), and under the condition, the generated photoproduction electrons can participate in the photocatalytic reduction of U (VI) after the semiconductor is excited by a light source. Therefore, the change of the energy band structure of the Ag-doped CdSe nanosheet is analyzed by utilizing the Mott-Schottky, the ultraviolet diffuse reflection and the UPS. As shown in fig. 7(a), the positive slopes of the two straight lines indicate that the CdSe and the 3% Ag-CdSe nanosheet are both n-type semiconductors, and compared with the original CdSe nanosheet, the carrier density of the 3% Ag-CdSe nanosheet after doping with Ag is higher, which indicates that the Ag doping can improve the conductive capability of CdSe and is more beneficial to the transfer of photogenerated carriers. Fig. 7(b) shows the band gap widths of CdSe, 1% Ag-CdSe, and 3% Ag-CdSe nanosheets calculated according to the ultraviolet diffuse reflection data, and it can be seen that the doping of Ag can reduce the band gap width of the CdSe nanosheets, and the narrow band gap structure can increase the light absorption wavelength range, which is more beneficial to the generation and transition of photogenerated carriers.
FIGS. 8(a) and (b) are the valence band spectra of CdSe, 1% Ag-CdSe, and 3% Ag-CdSe nanosheets, respectively. According to the UPS valence band curve and the secondary electron side curve, a corresponding energy band structure diagram can be obtained (figure 9). The conduction band positions of CdSe, 1% Ag-CdSe and 3% Ag-CdSe are respectively-4.68 eV, -4.63eV and-4.55 eV, and the difference between the theoretical energy needed by the photocatalytic reduction of uranium and 4.91eV is respectively 0.23eV, 0.28eV and 0.36 eV. It can be seen that the Ag doping is accompanied with the reduction of the band gap of the CdSe nanosheets, and the conduction band position is relatively shifted upwards, so that the photocatalytic reduction of U (VI) is more facilitated.
Carrying out U (VI) adsorption-catalytic reduction experiment on the Ag-doped CdSe nanosheet photocatalytic material separated by uranium reduction prepared in the comparative example 1 and the examples 1-4:
after the uranium is subjected to photocatalytic reduction, azoarsine III is mixed with the reacted solution, and the UO in the solution is monitored by using an ultraviolet visible absorption spectrum with the wavelength of 651.8nm2 2+The concentration of (c).
Dark conditions: respectively in 20mL UO2 2+Solution (C)0Adding 5mg of sample (Ag doped CdSe nanosheet photocatalytic material prepared in comparative example 1 and examples 1-4 and separated by uranium reduction) into 200mg/L solution with pH of 4, stirring at 600r/min for 120min at room temperature under dark condition, and measuring absorbance of the reacted solution by using an ultraviolet spectrophotometer (monitoring UO of different reaction times under the wavelength of 651.8nm by using ultraviolet visible absorption spectrum)2 2+Concentration), calculating the efficiency of photocatalytic reduction of uranium; all experiments were performed in triplicate and the mean values were taken; wherein the removal rate is (C)0-Ct)/C0×100％，C0As initial concentration, CtIs the post-adsorption concentration;
the illumination condition is as follows: respectively in 20mL UO2 2+Solution (C)0200mg/L and pH 4, 5mg of sample (Ag doped CdSe nanosheet photocatalytic material separated by uranium reduction prepared in comparative example 1 and examples 1-4) was added, simulated solar irradiation (300-W Xe lamp BL-GHX-V equipped with AM1.5G filter) was applied at room temperature, stirring was carried out at a speed of 600r/min for 160min, and the absorbance of the reacted solution was measured by an ultraviolet spectrophotometer (UO monitoring for different reaction times at a wavelength of 651.8nm for ultraviolet visible absorption spectroscopy)2 2+Concentration), calculating the efficiency of photocatalytic reduction of uranium; all experiments were performed in triplicate and the mean values were taken; wherein the removal rate is (C)0-Ct)/C0×100％，C0As initial concentration, CtIs the post-adsorption concentration;
FIG. 10 is a U (VI) removal rate curve under dark reaction for CdSe, 1% Ag-CdSe, 3% Ag-CdSe nanosheets; fig. 11 is a graph of u (vi) removal rate under photoreaction of CdSe, 1% Ag-CdSe, 3% Ag-CdSe nanoplates, and when there is no light, the removal rate of u (vi) by all nanoplates is below 3%, because CdSe nanoplates have a small specific surface area and few surface adsorption points, and therefore the adsorption to u (vi) is limited (fig. 10). In contrast, when light is introduced, under the influence of excitation of a light source, the CdSe nanosheets generate photo-generated electrons and holes to participate in the photocatalytic reduction of U (VI). As shown in fig. 11, the removal rate of u (vi) by 3% Ag-CdSe nanoplates was as high as 95.65%, which is 1.9 and 1.2 times that of CdSe nanoplates (49.7%) and 1% Ag-CdSe nanoplates (81.3%), respectively. The Ag-doped CdSe nanosheet is more beneficial to the photocatalytic reduction of the U (VI) reaction due to the change of the crystal structure and the band gap width.
FIG. 12 is a U (VI) removal rate curve under dark reaction for 3% Ag-CdSe, 3% Ag-CdSe-1, 3% Ag-CdSe-2 nanosheets; FIG. 13 is a U (VI) removal rate curve under the photoreaction of 3% Ag-CdSe, 3% Ag-CdSe-1 and 3% Ag-CdSe-2 nanosheets, and the reaction effect of the precipitate and hexadecyl trimethyl ammonium bromide can be remarkably improved by carrying out the reaction of the precipitate and a hexadecyl trimethyl ammonium bromide solution in a supercritical reaction device, so that the hydrophilicity of the Ag-doped CdSe nanosheet photocatalytic material separated by uranium reduction is further improved, and further the removal of U (VI) is improved; in addition, the Ag-doped CdSe nanosheet catalytic material is subjected to surface treatment through low-temperature plasma, so that the hydrophilicity of the Ag-doped CdSe nanosheet photocatalytic material subjected to uranium reduction and separation is further improved, and the removal of U (VI) is more remarkably improved.
The solid-liquid ratio, the anti-ion interference capability and the pH dependence of the 3% Ag-CdSe nanosheet are further analyzed. FIG. 14 is the solid-to-liquid ratio of 3% Ag-CdSe nanosheets (20mL UO)2 2+Solution, C0The graph of the relationship between simulated sunlight irradiation (300-W Xe lamp BL-GHX-V equipped with AM1.5G filter), addition of different amounts of 3% Ag-CdSe nanosheets, stirring for 120min) and U (VI) removal rate at room temperature under 200mg/L and pH 4 shows that the removal rate of U (VI) is balanced when the solid-liquid ratio is 0.25 as the solid-liquid ratio increases, which indicates that the optimal solid-liquid ratio for 3% Ag-CdSe nanosheet photocatalytic reduction of uranium is 0.25. Generally, the photocatalytic reduction method is selective, mainly to ions having reducing properties (e.g., U (VI) and U (IV)), so that non-reducing ions (e.g., Ca) coexist in the solution2+、K+、Mg2+) The photocatalytic reduction method can selectively reduce U (VI) to U (IV) without being influenced by other ions. FIG. 15 is an anti-ion interference plot of 3% Ag-CdSe nanoplates with Na coexisting in solution+、K+、Sr2+、Zn2+、Mg2+、SO4 2-, Br-, Cl-and U6+When the molar ratio of (A) to (B) is 1 to 1, the removal rate of the 3% Ag-CdSe nanosheets to U (VI) can be maintained at about 90% (20mL UO)2 2+Solution, C0Applying simulated sunlight irradiation (300-W Xe lamp BL-GHX-V with AM1.5G filter) at room temperature of 10mg/L, pH 4, 3% Ag-CdSe nanosheet 5mg, stirring for 120 min; for ions having reducing properties, e.g. Cu2+The removal rate of U (VI) by 3% Ag-CdSe nanosheets is slightly reduced. In addition, the surface electronegativity of the material also affects the removal rate of u (vi), and the surface electronegativity of the material is easily affected by the pH of the solution, so the pH dependence of 3% Ag-CdSe nanosheets was analyzed (fig. 16) (20mL UO)2 2+Solution, C0Applying simulated sunlight irradiation (package) at room temperature under the condition of 200mg/L300-W Xe lamp BL-GHX-V) with AM1.5G filter, different pH conditions, 5mg of 3% Ag-CdSe nanosheet, stirring for 120 min); it can be seen that, as the pH of the solution increases, the removal rate of u (vi) by the 3% Ag-CdSe nanosheets tends to increase first and then decrease, reaching an extreme point at about pH 4.0; based on the above analysis, the optimal experimental conditions for the 3% Ag-CdSe nanosheet were found, i.e., the 3% Ag-CdSe nanosheet had high selectivity to u (vi) at pH 4.0 and a solid-to-liquid ratio of 0.25.
In order to study the stability of the products and materials generated by the 3% Ag-CdSe nanosheets after the reaction of photocatalytic reduction of uranium, the corresponding products were collected and subjected to XPS analysis and testing, and the results are shown in FIG. 17. FIG. 17(a) shows the U4 f XPS spectra on 3% Ag-CdSe nanosheets after photocatalytic reaction, the U4 f XPS spectra can be divided into two main peaks, one is the U4 f XPS spectrum at 392.3eV5/2Peak, one is U4 f at 381.5eV5/2Peaks, U (VI) and U (IV) coexist in each peak. This result indicates that two ions, U (VI) and U (IV), coexist on the 3% Ag-CdSe nanosheets after the photocatalytic reaction, further indicating that the product of the photocatalytic reduction is U (IV). FIGS. 17(b) - (d) are Cd3d, Se 3d, and Ag 3d XPS spectra of 3% Ag-CdSe nanosheets after photocatalytic reaction (before and after photocatalytic reaction, respectively). After the photocatalytic reaction, a new peak appears in a 3d XPS spectrogram of Se at 52.3eV, and the peak is shifted to a position with low binding energy by about 1.1eV compared with the original peak at 53.4eV, which indicates that Se is slightly oxidized in the photocatalytic reaction process, and correspondingly, the peaks of Cd3d and Ag 3d are still kept unchanged. Therefore, under the illumination condition, the photoproduction electrons generated by the CdSe nano sheets participate in the photoreduction of U (VI), and the photoproduction holes cause the slight oxidation of Se, so that a state of surface electronegativity imbalance is generated, and the adsorption of U (VI) is better facilitated, and the U (VI) is photo-reduced to U (VI) under the action of photocatalysis.
Further using UPS to demonstrate the above conclusions, as shown in fig. 18, the valence band edge (fig. 18(a)) and secondary electron edge curve (fig. 18(b)) of 3% Ag-CdSe nanosheet UPS before and after photocatalytic reaction were plotted. It can be clearly seen that after the photocatalytic reaction, the secondary electron edge of the 3% Ag-CdSe nanosheet has a peak due to the presence of the tetravalent uranium species, which also laterally proves that the 3% Ag-CdSe nanosheet successfully realizes the photocatalytic reduction of u (vi).
While embodiments of the invention have been described above, it is not limited to the applications set forth in the description and the embodiments, which are fully applicable in various fields of endeavor to which the invention pertains, and further modifications may readily be made by those skilled in the art, it being understood that the invention is not limited to the details shown and described herein without departing from the general concept defined by the appended claims and their equivalents.
Claims (9)
1. A preparation method of an Ag-doped CdSe nanosheet photocatalytic material separated by uranium reduction is characterized by comprising the following steps of:
step one, CdCl2·2.5H2O and AgNO3The mixed powder is uniformly mixed with a first mixed solvent of octylamine and oleylamine, the mixture is heated to 115-125 ℃ and then reacts for 1-3 hours, and the mixture is naturally cooled to room temperature to obtain a reaction solution;
step two, uniformly mixing Se powder with a second mixed solvent of octylamine and oleylamine at room temperature to obtain a Se precursor solution;
and step three, adding the Se precursor solution in the step two into the reaction solution in the step one, heating to 90-100 ℃, reacting for 14-18 hours, cooling to room temperature, washing the obtained precipitate for multiple times by using a trichloromethane solution, uniformly mixing the precipitate with a hexadecyl trimethyl ammonium bromide solution, performing ultrasonic treatment for 45-90 min, washing the precipitate for multiple times by using ethanol, and performing vacuum drying to obtain the Ag-doped CdSe nanosheet photocatalytic material.
2. The method for preparing Ag-doped CdSe nanosheet photocatalytic material separated by uranium reduction according to claim 1, wherein in the first step, CdCl2·2.5H2O and AgNO3The molar ratio of (A) to (B) is 1.4-1.5: 0.01-0.035; the volume ratio of the octylamine to the oleylamine is 1: 1; the molar volume ratio of the mixed powder to the first mixed solvent is 1.5mmol:10 mL.
3. The method for preparing Ag-doped CdSe nanosheet photocatalytic material separated by uranium reduction according to claim 1, wherein in the second step, the molar volume ratio of Se powder to the second mixed solvent is 4.5 mmol: 5 mL; the volume ratio of the octylamine to the oleylamine is 1: 1; and the molar ratio of the Se powder to the mixed powder in the second step is 2.5-3.5: 1.
4. The method for preparing Ag-doped CdSe nanosheet photocatalytic material separated by uranium reduction according to claim 1, wherein in the third step, the concentration of cetyl trimethyl ammonium bromide solution is 0.05-0.15 mol/L; the molar volume ratio of the mixed powder in the first step to the cetyl trimethyl ammonium bromide solution is 1.5mmol: 25-45 mL.
5. The method for preparing Ag-doped CdSe nanosheet photocatalytic material separated by uranium reduction according to claim 1, wherein in the third step, the process of ultrasonically treating the precipitate and hexadecyl trimethyl ammonium bromide solution for 45-90 min after the precipitate and the hexadecyl trimethyl ammonium bromide solution are uniformly mixed is replaced by: adding the precipitate and a cetyl trimethyl ammonium bromide solution into a supercritical carbon dioxide reaction device, injecting carbon dioxide into the supercritical carbon dioxide reaction device, stirring for 15-30 min under the conditions that the temperature is 35-40 ℃ and the pressure is 12-18 MPa, relieving the pressure, and then carrying out ultrasound for 15-30 min; and washing the precipitate with ethanol for multiple times, and drying in vacuum to obtain the Ag-doped CdSe nanosheet photocatalytic material.
6. The method for preparing Ag-doped CdSe nanosheet photocatalytic material separated by uranium reduction according to claim 1, wherein in the third step, the obtained Ag-doped CdSe nanosheet photocatalytic material is treated for 1-3 min by using a low-temperature plasma treatment instrument.
7. The method of claim 6, wherein the atmosphere of the low temperature plasma processor is argon; the frequency of the low-temperature plasma treatment instrument is 35-45 KHz, the power is 45-60W, and the pressure of the atmosphere is 30-45 Pa.
8. The application of the Ag-doped CdSe nanosheet photocatalytic material obtained through reductive separation of uranium according to any one of claims 1 to 8 in radioactive wastewater treatment, wherein the radioactive wastewater is uranium-containing radioactive wastewater.
9. The application of the Ag-doped CdSe nanosheet photocatalytic material separated by uranium reduction in radioactive wastewater treatment according to claim 8, wherein the Ag-doped CdSe nanosheet photocatalytic material is added into the radioactive wastewater containing uranium to perform a photocatalytic reaction under the condition that a xenon lamp simulates sunlight, so that the photocatalytic reduction of hexavalent uranium in the radioactive wastewater containing uranium is realized; simultaneously, after the photocatalyst material after the photocatalytic reaction is oxidized in the air for 48 hours, the photocatalyst material is dispersed to 0.1mol/L KHCO3Elution reaction in solution to remove UO deposited on the catalyst2And then washed with water, and the collected photocatalyst material is dried and recycled.
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