CN112264075A - High-efficiency demercuration photocatalyst suitable for medium-low temperature condition and preparation method thereof - Google Patents
High-efficiency demercuration photocatalyst suitable for medium-low temperature condition and preparation method thereof Download PDFInfo
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- 239000011941 photocatalyst Substances 0.000 title claims abstract description 27
- 238000002360 preparation method Methods 0.000 title claims abstract description 15
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims abstract description 107
- 239000011258 core-shell material Substances 0.000 claims abstract description 20
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 claims abstract description 13
- 238000010438 heat treatment Methods 0.000 claims description 29
- 238000000034 method Methods 0.000 claims description 25
- 238000001035 drying Methods 0.000 claims description 22
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 16
- 238000001354 calcination Methods 0.000 claims description 14
- 238000002156 mixing Methods 0.000 claims description 13
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims description 11
- 239000004202 carbamide Substances 0.000 claims description 11
- 238000003756 stirring Methods 0.000 claims description 10
- 238000000137 annealing Methods 0.000 claims description 6
- YHWCPXVTRSHPNY-UHFFFAOYSA-N butan-1-olate;titanium(4+) Chemical compound [Ti+4].CCCC[O-].CCCC[O-].CCCC[O-].CCCC[O-] YHWCPXVTRSHPNY-UHFFFAOYSA-N 0.000 claims description 6
- 238000004140 cleaning Methods 0.000 claims description 6
- 238000001816 cooling Methods 0.000 claims description 6
- 238000001914 filtration Methods 0.000 claims description 6
- 239000007787 solid Substances 0.000 claims description 6
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims description 6
- 238000001027 hydrothermal synthesis Methods 0.000 claims description 4
- 230000007935 neutral effect Effects 0.000 claims description 4
- 238000011065 in-situ storage Methods 0.000 claims description 2
- 239000007788 liquid Substances 0.000 claims description 2
- 230000002194 synthesizing effect Effects 0.000 claims description 2
- 238000007598 dipping method Methods 0.000 claims 1
- 238000004519 manufacturing process Methods 0.000 claims 1
- 239000003054 catalyst Substances 0.000 abstract description 23
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 abstract description 13
- 230000001699 photocatalysis Effects 0.000 abstract description 12
- 229910052753 mercury Inorganic materials 0.000 abstract description 10
- 230000000694 effects Effects 0.000 abstract description 5
- 230000003197 catalytic effect Effects 0.000 abstract description 3
- 230000007613 environmental effect Effects 0.000 abstract description 2
- 239000013078 crystal Substances 0.000 abstract 1
- 239000002994 raw material Substances 0.000 abstract 1
- 239000008367 deionised water Substances 0.000 description 12
- 229910021641 deionized water Inorganic materials 0.000 description 12
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 7
- 239000003546 flue gas Substances 0.000 description 7
- 238000006243 chemical reaction Methods 0.000 description 6
- 239000007789 gas Substances 0.000 description 6
- 238000007146 photocatalysis Methods 0.000 description 6
- 239000000203 mixture Substances 0.000 description 5
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 4
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 4
- 229910052782 aluminium Inorganic materials 0.000 description 4
- 235000011114 ammonium hydroxide Nutrition 0.000 description 4
- 238000005516 engineering process Methods 0.000 description 4
- 239000011888 foil Substances 0.000 description 4
- 230000003647 oxidation Effects 0.000 description 4
- 238000007254 oxidation reaction Methods 0.000 description 4
- 239000011248 coating agent Substances 0.000 description 3
- 238000000576 coating method Methods 0.000 description 3
- 239000000725 suspension Substances 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 239000003153 chemical reaction reagent Substances 0.000 description 2
- 239000004744 fabric Substances 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 150000001412 amines Chemical class 0.000 description 1
- 238000004364 calculation method Methods 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000007872 degassing Methods 0.000 description 1
- 239000003085 diluting agent Substances 0.000 description 1
- 239000012717 electrostatic precipitator Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 238000011031 large-scale manufacturing process Methods 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 229910000474 mercury oxide Inorganic materials 0.000 description 1
- UKWHYYKOEPRTIC-UHFFFAOYSA-N mercury(ii) oxide Chemical compound [Hg]=O UKWHYYKOEPRTIC-UHFFFAOYSA-N 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- JMANVNJQNLATNU-UHFFFAOYSA-N oxalonitrile Chemical compound N#CC#N JMANVNJQNLATNU-UHFFFAOYSA-N 0.000 description 1
- 239000010453 quartz Substances 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 238000004088 simulation Methods 0.000 description 1
- 239000000779 smoke Substances 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/24—Nitrogen compounds
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8665—Removing heavy metals or compounds thereof, e.g. mercury
-
- B01J35/39—
-
- B01J35/396—
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/60—Heavy metals or heavy metal compounds
- B01D2257/602—Mercury or mercury compounds
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W10/00—Technologies for wastewater treatment
- Y02W10/30—Wastewater or sewage treatment systems using renewable energies
- Y02W10/37—Wastewater or sewage treatment systems using renewable energies using solar energy
Abstract
The invention discloses a high-efficiency demercuration (Hg) suitable for medium-low temperature conditions0) A photocatalyst and a preparation method thereof. First by highly exposing the (001) crystal plane of TiO2(001) Preparation of g-C of core-shell Structure3N4@TiO2Then adding CeO2Highly dispersed in g-C3N4@TiO2In addition, the utilization efficiency of Ce atoms is obviously improved, so that CeO with high photocatalytic mercury removal activity is prepared2‑g‑C3N4@TiO2. The catalyst shows excellent photocatalytic Hg removal at 50-250 DEG C0The performance and the catalytic performance are kept stable for a long time. The photocatalyst has the advantages of simple preparation method, strong repeatability, low price of raw materials, environmental protection, high practical value andand (4) application potential.
Description
Technical Field
The invention relates to the technical field of catalysts, in particular to a method for removing gaseous Hg in flue gas0The catalyst of (1).
Background
China is the atmosphere mercury (Hg)g) In the most serious countries, the heat power plant becomes Hg due to its huge emissiongOne of the main pollution sources of emissions, the mercury released by which exists mainly in three forms, namely elemental mercury (also known as gaseous elemental mercury, Hg)0) Mercury oxide (Hg)2+) And particulate bound mercury (Hg)p)。Hg2+Easily absorbed by amine solution, HgpEasily trapped by cloth bags, electrostatic precipitators or fabric filters, however, Hg0It is difficult to remove due to its high volatility and insolubility. Currently, Hg is removed from gas streams0The technology of (2) is various, such as wet deep oxidation, catalytic oxidation, photochemical oxidation and adsorption. Catalytic oxidation of Hg in exhaust gas using a catalyst0To make Hg in the exhaust gas0Removal or conversion to Hg2+And the mercury is removed by utilizing the relatively mature wet desulphurization technology and equipment of the coal-fired power plant, so that the method is an economical, effective and promising method in the prior coal-fired flue gas mercury removal technologies. Therefore, there is a need to develop efficient medium and low temperature environmentally friendly catalysts.
Disclosure of Invention
In order to overcome the defects of the prior art, the invention provides a high-efficiency demercuration photocatalyst suitable for medium-low temperature conditions and a preparation method thereof. The demercuration photocatalyst is applied to photocatalytic removal of Hg0In addition, the gaseous elementary mercury Hg in the gas can be effectively removed under the condition of medium and low temperature0Including atmospheric air, flue gas, etc.
One of the technical schemes adopted by the invention for solving the technical problems is as follows:
high-efficiency demercuration (Hg) suitable for medium-low temperature condition0) Photocatalyst which is a supported CeO2G to C of3N4@TiO2And said g-C3N4@TiO2Having a core-shell structure in g-C3N4(graphite phase carbon nitride) as shell and TiO2(001) Is the nucleus.
The invention relates to a high-efficiency degassing state suitable for medium-low temperature conditionsElemental mercury (Hg)0) Photocatalyst by highly exposing (001) plane TiO2(001) Preparation of g-C with core-shell Structure3N4@TiO2Then adding CeO2Highly dispersed in g-C3N4@TiO2In addition, the utilization efficiency of Ce atoms is obviously improved, so that the catalyst CeO with high photocatalytic mercury removal activity is prepared2-g-C3N4@TiO2。
Further, the application temperature range of the demercuration photocatalyst is 50-250 ℃. At 50-250 deg.C, CeO2-g-C3N4@TiO2The photocatalyst has excellent Hg removal effect0And (4) performance. Preferably, Hg is removed at 50-100 DEG C0The effect is optimal.
Further, in the demercuration photocatalyst, CeO2The relative content (mass percent) of (B) is 1-7 wt%. Preferably, CeO2The relative content of (A) is 2-4 wt%.
The second technical scheme adopted by the invention for solving the technical problems is as follows:
high-efficiency demercuration (Hg) suitable for medium-low temperature condition0) Method for preparing photocatalyst from TiO2(001) Synthesizing g-C with core-shell structure by in-situ growth method on the basis3N4@TiO2And then CeO is impregnated2Highly dispersed in g-C3N4@TiO2And calcining at a high temperature (e.g., 200 to 500 ℃) to obtain CeO2-g-C3N4@TiO2A photocatalyst.
Further, the method also comprises the step of preparing TiO by a hydrothermal method2(001) Mixing tetrabutyl titanate and HF according to the volume ratio of 3-5: 1, carrying out hydrothermal reaction at 190-210 ℃ for 22-26 h, cooling, adjusting the pH value to be neutral, drying, raising the temperature to 540-560 ℃ at the heating rate of 1-3 ℃/min, calcining for 1-3 h, and thus obtaining TiO2(001). Among them, preferable preparation parameters include, for example: mixing 18-22 mL of tetrabutyl titanate and 4-6 mL of 47-49% HF, putting into a high-pressure reaction kettle, and heating at 195-205 ℃ for 23-25 h; coldAfter cooling, adjusting the pH value to 6.8-7.2 by using deionized water, drying, raising the temperature to 545-555 ℃ at the temperature rise speed of 1.5-2.5 ℃/min, and calcining for 1.5-2.5 h to obtain TiO2(001)。
Further, g-C with core-shell structure3N4@TiO2The preparation method comprises the following steps: mixing urea and TiO2(001) Dissolving in water, mixing thoroughly in vacuum, solid-liquid separating, drying, and dissolving the obtained solid in N2Heating to 510-530 ℃ at a heating rate of 4-6 ℃/min in the atmosphere, and annealing for 1-3 h to obtain g-C with a core-shell structure3N4/TiO2. Among them, preferable preparation parameters include, for example: mixing urea and TiO with different mass proportions2(001) Dissolving in 25-35 mL deionized water, magnetically stirring in a vacuum system for 0.5-1.5 h, mixing thoroughly, centrifuging at 4000-6000 r/min, and drying; wrapping the centrifuged solid with 2-4 layers of aluminum foil, and adding N2Heating to 515-525 ℃ at a heating rate of 4.5-5.5 ℃/min and annealing for 1.5-2.5 h in the atmosphere to obtain g-C with a core-shell structure3N4/TiO2。
Wherein, urea and TiO2(001) The mass ratio of (A) to (B) is 5: 1-30: 1. Preferably urea and TiO2(001) The mass ratio of (A) to (B) is 18-22: 1, and the prepared catalyst has excellent performance.
Further, the CeO is added2Loaded at g-C3N4@TiO2The method comprises the following steps: g-C with core-shell structure3N4@TiO2Uniformly dispersing in water, adjusting the pH value to 8.8-9.2, and adding Ce (NO)3)3·6H2O, stirring and reacting at normal temperature, filtering and cleaning until the pH value is neutral, and drying to obtain the CeO-loaded carrier2G to C of3N4@TiO2；
Further, the CeO is obtained by calcination2-g-C3N4@TiO2The method of photocatalyst comprises: will be loaded with CeO2G to C of3N4@TiO2Raising the temperature to 290-310 ℃ at a heating rate of 3-5 ℃/min in an air atmosphereCalcining for 1-3 h to obtain CeO2-g-C3N4@TiO2A photocatalyst.
Among them, preferable preparation parameters include, for example: 0.40-0.60 g of core-shell g-C3N4@TiO2Uniformly dispersing in 70-80 mL of deionized water, adding ammonia water to adjust the pH value to about 8.9-9.1, and adding Ce (NO) according to a certain proportion3)3·6H2And O, stirring for 2-3 h at normal temperature, filtering and cleaning until the pH value is about 6.8-7.2, and drying. And finally, heating the mixture to 295-305 ℃ at a heating rate of 3.5-4.5 ℃/min in the air atmosphere, and calcining for 1.5-2.5 h.
Preferably, the drying temperature in the above step is 60-80 ℃, and the drying time is 8-15 h, for example 11-13 h.
In a preferred embodiment of the invention, the prepared catalyst is applied to the photocatalytic removal of Hg0In 50-250 deg.c, CeO2-g-C3N4@TiO2The photocatalyst has excellent Hg removal effect0And (4) performance.
The equipment, reagents, processes, parameters and the like related to the invention are conventional equipment, reagents, processes, parameters and the like except for special description, and no embodiment is needed.
All ranges recited herein include all point values within the range.
As used herein, "about" or "approximately" means within plus or minus 20% of the stated range or value.
In the present invention,% is mass% and ratio is mass ratio unless otherwise specified.
In the invention, the normal temperature, namely the normal environmental temperature, can be 10-30 ℃. The medium and low temperature refers to 50-250 ℃.
Compared with the background technology, the technical scheme has the following advantages:
1. according to the invention, by TiO2(001) Preparation of g-C of core-shell Structure3N4@TiO2Then adding CeO2Dispersed in g-C3N4@TiO2The obtained CeO was prepared2-g-C3N4@TiO2The photocatalyst can maintain excellent photocatalytic removal of Hg at medium and low temperature0The performance and the stability are good, and the material can be repeatedly used.
2. The catalyst prepared by the method of the invention does not cause secondary pollution to the environment in the using process.
3. The catalyst prepared by the method has simple operation process and high repeatability, only needs conventional equipment and instruments in the preparation process of the catalyst, and is suitable for industrial large-scale production.
Drawings
FIG. 1 shows different urea and TiO compounds prepared in the examples of the present invention2(001) 3 percent of CeO2-g-C3N4@TiO2With commercial TiO2Removing Hg by photocatalysis at 50-250 DEG C0Graph of Performance with temperature on the horizontal axis and Hg on the vertical axis0The removal rate of (3).
Detailed Description
The technical solution of the present invention will be further illustrated and described below with reference to the accompanying drawings by means of specific embodiments.
Example 1:
using prepared CeO2-g-C3N4@TiO2The catalyst is used for removing Hg in coal-fired flue gas by photocatalysis0. The specific implementation steps are as follows:
(1) mixing 20mL of tetrabutyl titanate and 5mL of 48% HF, putting into a high-pressure reaction kettle, and heating at 200 ℃ for 24 hours; cooling, adjusting pH to 7 with deionized water, drying for 12h, heating to 550 deg.C at a rate of 2 deg.C/min, and calcining for 2h to obtain TiO2(001)。
(2) 20g of urea and 1g of TiO2(001) Dissolving in 30mL deionized water, magnetically stirring the uniform suspension in a vacuum system for 1h, centrifuging at the rotating speed of 5000r/min, and drying for 12 h; coating the solid with 3 layers of aluminum foil, adding N2Heating to 520 ℃ at a heating rate of 5 ℃/min and annealing for 2h under the atmosphere to obtain g-C with a core-shell structure3N4/TiO2。
(3) 0.50g of g-C3N4@TiO2Uniformly dispersing in 75mL deionized water, adding ammonia water to adjust pH to about 9, adding a certain amount of Ce (NO)3)3·6H2O in CeO23 percent by mass, stirring for 2.5 hours at normal temperature, filtering and cleaning until the pH value is about 7, and drying for 12 hours. Finally, the mixture is heated to 300 ℃ at the heating rate of 4 ℃/min in the air atmosphere, and is calcined for 2h to obtain CeO2-g-C3N4@TiO2Catalyst, 3% CeO2-g-C3N4@TiO2(20:1)。
Example 2:
using prepared CeO2-g-C3N4@TiO2The catalyst is used for removing Hg in coal-fired flue gas by photocatalysis0. The specific implementation steps are as follows:
(1) mixing 20mL of tetrabutyl titanate and 5mL of 48% HF, putting into a high-pressure reaction kettle, and heating at 200 ℃ for 24 hours; cooling, adjusting pH to 7 with deionized water, drying for 12h, heating to 550 deg.C at a rate of 2 deg.C/min, and calcining for 2h to obtain TiO2(001)。
(2) 25g of urea and 1g of TiO2(001) Dissolving in 30mL deionized water, magnetically stirring the uniform suspension in a vacuum system for 1h, centrifuging at the rotating speed of 5000r/min, and drying for 12 h; coating the solid with 3 layers of aluminum foil, adding N2Heating to 520 ℃ at the heating rate of 5 ℃/min and annealing for 2h under the atmosphere to obtain the g-C core shell3N4/TiO2。
(3) 0.50g of core shell g-C3N4@TiO2Uniformly dispersing in 75mL deionized water, adding ammonia water to adjust pH to about 9, adding a certain amount of Ce (NO)3)3·6H2O in CeO23 percent by mass, stirring for 2.5 hours at normal temperature, filtering and cleaning until the pH value is about 7, and drying for 12 hours. Finally, the mixture is heated to 300 ℃ at the heating rate of 4 ℃/min in the air atmosphere, and is calcined for 2h to obtain CeO2-g-C3N4@TiO2Catalyst, 3% CeO2-g-C3N4@TiO2(25:1)。
Example 3:
using prepared CeO2-g-C3N4@TiO2The catalyst is used for removing Hg in coal-fired flue gas by photocatalysis0. The specific implementation steps are as follows:
(1) mixing 20mL of tetrabutyl titanate and 5mL of 48% HF, putting into a high-pressure reaction kettle, and heating at 200 ℃ for 24 hours; cooling, adjusting pH to 7 with deionized water, drying for 12h, heating to 550 deg.C at a rate of 2 deg.C/min, and calcining for 2h to obtain TiO2(001)。
(2) Mixing 15g of urea and 1g of TiO2(001) Dissolving in 30mL deionized water, magnetically stirring the uniform suspension in a vacuum system for 1h, centrifuging at the rotating speed of 5000r/min, and drying for 12 h; coating the solid with 3 layers of aluminum foil, adding N2Heating to 520 ℃ at the heating rate of 5 ℃/min and annealing for 2h under the atmosphere to obtain the g-C core shell3N4/TiO2。
(3) 0.50g of core shell g-C3N4@TiO2Uniformly dispersing in 75mL deionized water, adding ammonia water to adjust pH to about 9, adding a certain amount of Ce (NO)3)3·6H2O in CeO23 percent by mass, stirring for 2.5 hours at normal temperature, filtering and cleaning until the pH value is about 7, and drying for 12 hours. Finally, the mixture is heated to 300 ℃ at the heating rate of 4 ℃/min in the air atmosphere, and is calcined for 2h to obtain CeO2-g-C3N4@TiO2Catalyst, 3% CeO2-g-C3N4@TiO2(15:1)。
Examples 4 to 5
The urea and TiO in step (2) were changed by the method of reference examples 1 to 32(001) In a mass ratio of 30:1 and 10:1, respectively, to obtain a catalyst of 3% CeO2-g-C3N4@TiO2(30:1) and catalyst 3% CeO2-g-C3N4@TiO2(10:1)。
0.20g of the catalyst prepared in example 1-5 was used for removing Hg by photocatalysis0And (4) reacting. The reaction simulation smoke takes high-purity nitrogen as carrier gasHg is carried by the superheated vapor generator0And (3) feeding the mixture into a mixer, and simultaneously introducing the other path of air as diluent gas to be mixed with mercury vapor, wherein the total gas inlet flow is 1L/min. The simulated flue gas was passed into a quartz reactor containing 0.20g of catalyst, the reactor was maintained at 50 deg.C, 100 deg.C, 150 deg.C, 200 deg.C, 250 deg.C, respectively, and Hg at the outlet was recorded0Change in concentration, calculation of Hg0The removal rate of (3). The results are shown in FIG. 1. As can be seen from FIG. 1, CeO2-g-C3N4@TiO2Has good Hg removal by photocatalysis0Properties, Hg at 50 ℃ and 100 ℃0The removal rate of the catalyst is stabilized to about 100 percent, and Hg is at 250 DEG C0The removal rate of the catalyst is stabilized to be about 58.2 percent compared with commercial TiO2The mercury removal efficiency is remarkably improved.
The above description is only a preferred embodiment of the present invention, and therefore should not be taken as limiting the scope of the invention, which is defined by the appended claims and their equivalents.
Claims (10)
1. The demercuration photocatalyst suitable for medium and low temperature conditions is characterized in that: it is loaded with CeO2G to C of3N4@TiO2And said g-C3N4@TiO2Having a core-shell structure in g-C3N4As a shell, with TiO2(001) Is the nucleus.
2. The demercuration photocatalyst as defined in claim 1, wherein: the application temperature range of the demercuration photocatalyst is 50-250 ℃.
3. The demercuration photocatalyst as defined in claim 1, wherein: in the demercuration photocatalyst, CeO2The mass percentage of (B) is 1-7 wt%.
4. A method for preparing the demercuration photocatalyst according to any one of claims 1 to 3, characterized in that: by TiO 22(001) Synthesizing g-C with core-shell structure by in-situ growth method on the basis3N4@TiO2Then, CeO is added by dipping2Loaded at g-C3N4@TiO2CeO was obtained by calcination2-g-C3N4@TiO2A photocatalyst.
5. The method of claim 4, wherein: the CeO is obtained by calcination2-g-C3N4@TiO2In the process of the photocatalyst, the calcining temperature is 200-500 ℃.
6. The method of claim 4, wherein: further comprising: preparation of TiO by hydrothermal method2(001): mixing tetrabutyl titanate and HF according to the volume ratio of 3-5: 1, carrying out hydrothermal reaction at 190-210 ℃ for 22-26 h, cooling, adjusting the pH value to be neutral, drying, raising the temperature to 540-560 ℃ at the heating rate of 1-3 ℃/min, calcining for 1-3 h, and thus obtaining TiO2(001)。
7. The method of claim 4, wherein: the g-C with the core-shell structure3N4@TiO2The preparation method comprises the following steps: mixing urea and TiO2(001) Dissolving in water, mixing thoroughly in vacuum, solid-liquid separating, drying, and dissolving the obtained solid in N2Heating to 510-530 ℃ at a heating rate of 4-6 ℃/min in the atmosphere, and annealing for 1-3 h to obtain g-C with a core-shell structure3N4/TiO2。
8. The method of claim 7, wherein: the urea and TiO2(001) The mass ratio of (A) to (B) is 5: 1-30: 1.
9. The method of claim 4, wherein: the CeO is added2Loaded at g-C3N4@TiO2The method comprises the following steps: will have a core-shell structureg-C3N4@TiO2Uniformly dispersing in water, adjusting the pH value to 8.8-9.2, and adding Ce (NO)3)3·6H2O, stirring and reacting at normal temperature, filtering and cleaning until the pH value is neutral, and drying to obtain the CeO-loaded carrier2G to C of3N4@TiO2(ii) a The CeO is obtained by calcination2-g-C3N4@TiO2The method of photocatalyst comprises: will be loaded with CeO2G to C of3N4@TiO2Heating to 280-320 ℃ at a heating rate of 3-5 ℃/min in an air atmosphere, and calcining for 1-3 h to obtain CeO2-g-C3N4@TiO2A photocatalyst.
10. The production method according to claim 6, 7 or 9, characterized in that: the drying temperature is 60-80 ℃, and the drying time is 8-15 h.
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| CN202011239219.9A CN112264075B (en) | 2020-11-09 | 2020-11-09 | High-efficiency demercuration photocatalyst suitable for medium-low temperature condition and preparation method thereof |
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| CN202011239219.9A CN112264075B (en) | 2020-11-09 | 2020-11-09 | High-efficiency demercuration photocatalyst suitable for medium-low temperature condition and preparation method thereof |
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| CN113058630A (en) * | 2021-03-15 | 2021-07-02 | 华侨大学 | Preparation method and application of photocatalyst suitable for efficiently removing formaldehyde at room temperature |
| CN113559852A (en) * | 2021-07-23 | 2021-10-29 | 华侨大学 | Hg removal suitable for medium and low temperature conditions0Catalyst and preparation method thereof |
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| CN113559852A (en) * | 2021-07-23 | 2021-10-29 | 华侨大学 | Hg removal suitable for medium and low temperature conditions0Catalyst and preparation method thereof |
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