CN107824179A - A kind of preparation method of highlight catalytic active beta bismuth oxide - Google Patents

A kind of preparation method of highlight catalytic active beta bismuth oxide Download PDF

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CN107824179A
CN107824179A CN201710998691.2A CN201710998691A CN107824179A CN 107824179 A CN107824179 A CN 107824179A CN 201710998691 A CN201710998691 A CN 201710998691A CN 107824179 A CN107824179 A CN 107824179A
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solution
bismuth oxide
mol
concentration
catalytic active
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单连伟
毕净净
肖彦薇
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Harbin University of Science and Technology
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Harbin University of Science and Technology
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    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/16Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
    • B01J23/18Arsenic, antimony or bismuth
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J35/00Catalysts, in general, characterised by their form or physical properties
    • B01J35/30Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
    • B01J35/39Photocatalytic properties
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J37/00Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/02Impregnation, coating or precipitation
    • B01J37/03Precipitation; Co-precipitation
    • B01J37/038Precipitation; Co-precipitation to form slurries or suspensions, e.g. a washcoat
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J37/00Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/08Heat treatment

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Physics & Mathematics (AREA)
  • Thermal Sciences (AREA)
  • Catalysts (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Exhaust Gas Treatment By Means Of Catalyst (AREA)

Abstract

The present invention relates to a kind of preparation method of highlight catalytic active beta bismuth oxide.Bismuth oxide has visible light-responded ability, but bismuth oxide be there are problems that in catalytic applications are closed, and the light absorpting ability such as bismuth oxide is not strong, causes photocatalytic activity relatively low, and its relatively low photocatalytic activity, which is difficult to reach, meets actual demand.It is as follows the step of the preparation method of highlight catalytic active beta bismuth oxide in the present invention:Solution containing bismuth nitrate, nitric acid and citric acid is mixed with the solution containing acetic acid and sodium acetate, by adjusting pH value, water-bath, drying, grinding, washing, air atmosphere calcining and H2Highlight catalytic active beta bismuth oxide powder is obtained after being heat-treated under atmosphere.The present invention is easily achieved industrialization, product visible absorption ability is strong, photocatalytic activity is high.

Description

A kind of preparation method of highlight catalytic active beta bismuth oxide
Technical field
The present invention relates to a kind of preparation method of highlight catalytic active beta bismuth oxide, applied to depollution of environment field.
Background technology
Photocatalitic Technique of Semiconductor has boundless application prospect in degraded organic pollutants etc., and gradual One of heat subject as research.Titanium dioxide(TiO2, band gap is 3.2 eV)And zinc oxide(ZnO, band gap are 3.4 eV)Deng only having ultraviolet light response ability, and bismuth oxide has visible light-responded ability.Bismuth oxide is increasingly becoming in recent years The study hotspot of novel photocatalyst development field.Yan etc. is with Bi (NO3)3•5H2O primary raw materials, by hydro-thermal method synthesized β- Bi2O3(Journal of Alloys and Compounds, 2014,605:102-108), disclosed in patent CN104826623B A kind of bismuth oxide photocatalyst and its preparation method and application, has obtained nano flower-like beta oxidation bismuth visible light catalyst.On State document and patent all Successful utilization hydro-thermal methods and prepare beta oxidation bismuth nano material.β-Bi at present2O3In photocatalysis field internal memory In problem, as visible absorption is indifferent, cause quantum efficiency relatively low, and relatively low photocatalytic activity is difficult to reach satisfaction Actual demand.Therefore, it is necessary to further develop the strong β-Bi of visible light-responded ability2O3
The content of the invention
It is an object of the invention to provide a kind of preparation method of highlight catalytic active beta bismuth oxide.
Above-mentioned purpose is realized by following technical scheme:
A kind of preparation method of highlight catalytic active beta bismuth oxide, preparation method step are as follows:
Step 1, at normal temperatures, by glass container by 5.145 grams of Bi (NO3)3•5H2It is 1~4 mol/L that O, which is dissolved in concentration, HNO3In solution, then add concentration and form mixed solution, the magnetic force in course of dissolution for 0.2~2 mol/L citric acids Stirring, after above-mentioned chemical substance is completely dissolved, continues 30~90min of stirring, then with the NaOH that concentration is 1~4 mol/L Solution adjusts pH value, and the rate of addition of NaOH solution is controlled in 0.5~3mL/min, molten until mixing by progressively testing pH value The pH=7 of liquid.
Step 2, at normal temperatures, by glass container by 2mmol citric acid and 2mmol Na [Al (OH)4] be added to In deionized water, its compound concentration is set to be 0.2~2 mol/L, while magnetic agitation, after solution to be mixed is completely dissolved, continue Stop after 30~90min of stirring.
Step 3, at normal temperatures, solution made from step 1 is added dropwise into described step 2 by new glass container to be made Solution in, then with concentration be 1~4 mol/L NaOH solution adjust solution pH value, NaOH solution rate of addition control In 0.5~2mL/min, until the pH=7 of solution, continue 30~90min of stirring, then under 70~100oC heating-up temperature Stop after 4~15h of water-bath, stirred during water-bath using electric mixer, rotating speed control is 20~90rpm.
Step 4, under 120~160oC heating-up temperatures, viscous solution made from baking step 3, drying time control is 6 ~12h, precursor powder is obtained after grinding, at normal temperatures, precursor powder is cleaned 3~5 times repeatedly with deionized water, removed Na in precursor powder+And Al3+Ion, then under 60~120 °C of heating-up temperatures, dry 12~24h.
Step 5, in air atmosphere, powder made from step 4 is calcined into 2~7h under 315~370 °C, obtain β- Bi2O3Powder, by a certain amount of β-Bi2O3Powder is put into H2In atmosphere furnace, after vacuumizing, H is passed through2Gas, maintain H2Point 20~100kPa is pressed in, 2~6h is heat-treated under 200~330 °C, obtains highlight catalytic active beta bismuth oxide powder.
Beneficial effect:
1. highlight catalytic active beta bismuth oxide prepared by the present invention, compared with prior art, the invention provides one kind to be easy to Realize industrialized method.
2. the present invention is figure it is seen that H2Under atmosphere after atmosphere heat treatment beta bismuth oxide, its ABSORPTION EDGE there occurs One obvious red shift, the purer beta bismuth oxide of light absorpting ability have a more obvious enhancing, it is seen that light absorpting ability Enhancing, which improves, produces light induced electron and the probability in hole in photochemical catalyst, promote the increase of photocatalysis efficiency.
Brief description of the drawings:
Accompanying drawing 1 is that highlight catalytic active beta bismuth oxide X-ray diffraction made from the embodiment of the present invention 1 contrasts collection of illustrative plates.
Accompanying drawing 2 is the optical absorption map of highlight catalytic active beta bismuth oxide made from the embodiment of the present invention 1.
Embodiment:
Below by specific embodiment, the present invention is described in further detail, and following examples can make this professional technique The present invention, but do not limit the invention in any way is more completely understood in personnel.
Embodiment 1:
Step 1, at normal temperatures, by glass container by 5.145 grams of Bi (NO3)3•5H2It is 1.5 mol/L's that O, which is dissolved in concentration, HNO3In solution, then add concentration and formed to mix for 0.5 mol/L citric acids and hold liquid, the magnetic agitation in course of dissolution, After above-mentioned chemical substance is completely dissolved, continue to stir 30min, then adjust pH with the NaOH solution that concentration is 1.5 mol/L Value, the rate of addition control of NaOH solution is in 2mL/min, by progressively testing pH value until the pH=7 of mixed solution.
Step 2, at normal temperatures, by glass container by 2mmol citric acid and 2mmol Na [Al (OH)4] be added to In deionized water, its compound concentration is set to be 0.5 mol/L, while magnetic agitation, after solution to be mixed is completely dissolved, continue to stir Stop after 30~90min
Step 3, at normal temperatures, described solution A is added dropwise in described solution B by new glass container, then uses concentration The pH value of solution is adjusted for 1.5 mol/L NaOH solution, the rate of addition control of NaOH solution is in 2mL/min, until solution PH=7, then proceed to stir 30min, rotating speed control be 30rpm.
Step 4, under 120oC heating-up temperatures, viscous solution made from baking step 3, drying time control is 12h, is ground Precursor powder is obtained after mill, at normal temperatures, precursor powder is cleaned 3 times repeatedly with deionized water, then in 80 °C of heating At a temperature of, dry 14h.
Step 5, in air atmosphere, powder made from step 4 is calcined into 3h under 355 °C, obtains β-Bi2O3Powder, will A certain amount of β-Bi2O3Powder is put into H2In atmosphere furnace, after vacuumizing, H is passed through2Gas, maintain H2Partial pressure in 40kPa, It is heat-treated 5 hours under 240 °C, obtains highlight catalytic active beta bismuth oxide powder.In the experiment of photocatalytic water degraded methyl orange, The catalytic performance of highlight catalytic active beta bismuth oxide is 4.3 times of beta bismuth oxide.
Embodiment 2:
Step 1, at normal temperatures, by glass container by 5.145 grams of Bi (NO3)3•5H2It is 2.5 mol/L's that O, which is dissolved in concentration, HNO3In solution, then add concentration and formed to mix for 1.5 mol/L citric acids and hold liquid, the magnetic agitation in course of dissolution, After above-mentioned chemical substance is completely dissolved, continue to stir 30min, then adjust pH with the NaOH solution that concentration is 2.5 mol/L Value, the rate of addition control of NaOH solution is in 1mL/min, by progressively testing pH value until the pH=7 of mixed solution.
Step 2, at normal temperatures, by glass container by 2mmol citric acid and 2mmol Na [Al (OH)4] be added to In deionized water, its compound concentration is set to be 1.5 mol/L, while magnetic agitation, after solution to be mixed is completely dissolved, continue to stir Stop after 50min
Step 3, at normal temperatures, described solution A is added dropwise in described solution B by new glass container, then uses concentration The pH value of solution is adjusted for 2.5 mol/L NaOH solution, the rate of addition control of NaOH solution is in 1mL/min, until solution PH=7, then proceed to stir 50min, rotating speed control be 30rpm.
Step 4, under 140oC heating-up temperatures, viscous solution made from baking step 3, drying time control is 10h, is ground Precursor powder is obtained after mill, at normal temperatures, precursor powder is cleaned 3 times repeatedly with deionized water, then in 80 °C of heating At a temperature of, dry 14h.
Step 5, in air atmosphere, powder made from step 4 is calcined into 3h under 355 °C, obtains β-Bi2O3Powder, will A certain amount of β-Bi2O3Powder is put into H2In atmosphere furnace, after vacuumizing, H is passed through2Gas, maintain H2Partial pressure in 50kPa, It is heat-treated 4 hours under 260 °C, obtains highlight catalytic active beta bismuth oxide powder.
Embodiment 3:
Step 1, at normal temperatures, by glass container by 5.145 grams of Bi (NO3)3•5H2It is 2.5 mol/L's that O, which is dissolved in concentration, HNO3In solution, then add concentration and formed to mix for 1.5 mol/L citric acids and hold liquid, the magnetic agitation in course of dissolution, After above-mentioned chemical substance is completely dissolved, continue to stir 30min, then adjust pH with the NaOH solution that concentration is 2.5 mol/L Value, the rate of addition control of NaOH solution is in 1mL/min, by progressively testing pH value until the pH=7 of mixed solution.
Step 2, at normal temperatures, by glass container by citric acid and Na [Al (OH)4] be added in deionized water, make it Compound concentration is 1.5 mol/L, while magnetic agitation, after solution to be mixed is completely dissolved, continues to stop after stirring 50min
Step 3, at normal temperatures, described solution A is added dropwise in described solution B by new glass container, then uses concentration The pH value of solution is adjusted for 2.5 mol/L NaOH solution, the rate of addition control of NaOH solution is in 1mL/min, until solution PH=7, then proceed to stir 50min, rotating speed control be 30rpm.
Step 4, under 140oC heating-up temperatures, viscous solution made from baking step 3, drying time control is 10h, is ground Precursor powder is obtained after mill, at normal temperatures, precursor powder is cleaned 3 times repeatedly with deionized water, then in 80 °C of heating At a temperature of, dry 14h.
Step 5, in air atmosphere, powder made from step 4 is calcined into 3h under 355 °C, obtains β-Bi2O3Powder, will A certain amount of β-Bi2O3Powder is put into H2In atmosphere furnace, after vacuumizing, H is passed through2Gas, maintain H2Partial pressure in 60kPa, It is heat-treated 4 hours under 260 °C, obtains highlight catalytic active beta bismuth oxide powder.
Above said content is only the basic explanation under present inventive concept, by reading description of the invention and to the present invention Any equivalent conversion that technical scheme is taken, all should belong to protection scope of the present invention.

Claims (6)

1. a kind of preparation method of highlight catalytic active beta bismuth oxide, it is characterised in that comprise the following steps:
Step 1, at normal temperatures, by glass container by 5.145 grams of Bi (NO3)3•5H2It is 1~4 mol/L that O, which is dissolved in concentration, HNO3In solution, then add concentration and form mixed solution, the magnetic force in course of dissolution for 0.2~2 mol/L citric acids Stirring, after above-mentioned chemical substance is completely dissolved, continues 30~90min of stirring, then with the NaOH that concentration is 1~4 mol/L Solution adjusts pH value, and the rate of addition of NaOH solution is controlled in 0.5~3mL/min, molten until mixing by progressively testing pH value The pH=7 of liquid;
Step 2, at normal temperatures, by glass container by 2mmol citric acid and 2mmol Na [Al (OH)4] be added to from In sub- water, its compound concentration is set to be 0.2~2 mol/L, while magnetic agitation, after solution to be mixed is completely dissolved, continue to stir Stop after 30~90min;
Step 3, at normal temperatures, solution made from step 1 is added dropwise to by new glass container molten made from described step 2 In liquid, then the pH value with the NaOH solution adjustment solution that concentration is 1~4 mol/L, the rate of addition of NaOH solution are controlled 0.5 ~2mL/min, until the pH=7 of solution, continue 30~90min of stirring, the then water-bath 4 under 70~100oC heating-up temperature Stop after~15h, stirred during water-bath using electric mixer, rotating speed control is 20~90rpm;
Step 4, under 120~160oC heating-up temperatures, viscous solution made from baking step 3, drying time control for 6~ 12h, precursor powder is obtained after grinding, at normal temperatures, precursor powder is cleaned 3~5 times, before removal repeatedly with deionized water Drive the Na in body powder+Ion, then under 60~120 °C of heating-up temperatures, dry 12~24h;
Step 5, in air atmosphere, powder made from step 4 is calcined into 2~7h under 315~370 °C, obtains β-Bi2O3Powder End, by a certain amount of β-Bi2O3Powder is put into H2In atmosphere furnace, after vacuumizing, H is passed through2Gas, maintain H2Partial pressure 20~ 100kPa, 2~6h is heat-treated under 200~330 °C, obtains highlight catalytic active beta bismuth oxide powder.
2. the preparation method of highlight catalytic active beta bismuth oxide according to claim 1, it is characterised in that the step In 1:HNO3The concentration of solution is 1~4 mol/L, and the concentration of citric acid solution is 0.2~2 mol/L, the time of magnetic agitation For 30~90min, the concentration of NaOH solution is 1~4 mol/L, and the rate of addition of NaOH solution is 0.5~2mL/min.
3. the preparation method of highlight catalytic active beta bismuth oxide according to claim 1, it is characterised in that the step In rapid 2:The concentration of citric acid solution is 0.2~2 mol/L, Na [Al (OH)4] concentration of solution is 0.2~2 mol/L, stirring Time is 30~90min, and the concentration of NaOH solution is 1~4 mol/L, and the rate of addition of NaOH solution is 0.5~2mL/min, Mixing time is 30~90min.
4. the preparation method of highlight catalytic active beta bismuth oxide according to claim 1, it is characterised in that the step In 3:1~4 mol/L NaOH solution rate of addition is 0.5~2mL/min, and bath temperature is 70~100oC, and water bath time is 4~15h, mixing speed are 20~90rpm.
5. the preparation method of highlight catalytic active beta bismuth oxide according to claim 1, it is characterised in that the step In 4:Drying temperature is 120~160oC, and drying time is 6~12h.
6. the preparation method of highlight catalytic active beta bismuth oxide according to claim 1, it is characterised in that the step In 5:Powder calcination atmosphere made from step 4 is air, and calcining heat is 315~370 °C, and calcination time is 2~7h, β-Bi2O3 The heat-treating atmosphere of powder is H2, H2Partial pressure in 20~100kPa, heat treatment temperature is 200~330 °C, heat treatment time 2 ~6h.
CN201710998691.2A 2017-10-24 2017-10-24 A kind of preparation method of highlight catalytic active beta bismuth oxide Pending CN107824179A (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113651358A (en) * 2020-10-21 2021-11-16 上海紫迈纳米科技有限公司 Method for preparing high-purity superfine bismuth oxide

Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1655869A (en) * 2002-03-25 2005-08-17 住友钛株式会社 Titanium oxide-based photocatalyst, manufacturing method therefor and its application

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1655869A (en) * 2002-03-25 2005-08-17 住友钛株式会社 Titanium oxide-based photocatalyst, manufacturing method therefor and its application
US20050227008A1 (en) * 2002-03-25 2005-10-13 Katsumi Okada Titanium oxide photocatalyst, process for producing the same and application

Non-Patent Citations (2)

* Cited by examiner, † Cited by third party
Title
LIANWEI SHAN ET AL.: "Band alignment and enhanced photocatalytic activation of α/β-Bi2O3 heterojunctions via in situ phase transformation", 《PAPER》 *
孙奉玉等: "二氧化钛表面光学特性与光催化活性的关系", 《催化学报》 *

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113651358A (en) * 2020-10-21 2021-11-16 上海紫迈纳米科技有限公司 Method for preparing high-purity superfine bismuth oxide

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