CN110002532B - Method for degrading organic pollutants in water body by using black carbon light - Google Patents
Method for degrading organic pollutants in water body by using black carbon light Download PDFInfo
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- CN110002532B CN110002532B CN201910205392.8A CN201910205392A CN110002532B CN 110002532 B CN110002532 B CN 110002532B CN 201910205392 A CN201910205392 A CN 201910205392A CN 110002532 B CN110002532 B CN 110002532B
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- 239000003738 black carbon Substances 0.000 title claims abstract description 57
- 238000000034 method Methods 0.000 title claims abstract description 34
- 239000002957 persistent organic pollutant Substances 0.000 title claims abstract description 29
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 title claims abstract description 28
- 230000000593 degrading effect Effects 0.000 title claims abstract description 8
- 238000006243 chemical reaction Methods 0.000 claims abstract description 38
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 22
- 239000001301 oxygen Substances 0.000 claims abstract description 22
- 230000015556 catabolic process Effects 0.000 claims abstract description 18
- 238000006731 degradation reaction Methods 0.000 claims abstract description 18
- 238000003756 stirring Methods 0.000 claims abstract description 17
- VLKZOEOYAKHREP-UHFFFAOYSA-N n-Hexane Chemical compound CCCCCC VLKZOEOYAKHREP-UHFFFAOYSA-N 0.000 claims description 35
- 238000002485 combustion reaction Methods 0.000 claims description 23
- 239000000446 fuel Substances 0.000 claims description 22
- STZCRXQWRGQSJD-GEEYTBSJSA-M methyl orange Chemical group [Na+].C1=CC(N(C)C)=CC=C1\N=N\C1=CC=C(S([O-])(=O)=O)C=C1 STZCRXQWRGQSJD-GEEYTBSJSA-M 0.000 claims description 17
- 229940012189 methyl orange Drugs 0.000 claims description 17
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 claims description 15
- IISBACLAFKSPIT-UHFFFAOYSA-N bisphenol A Chemical compound C=1C=C(O)C=CC=1C(C)(C)C1=CC=C(O)C=C1 IISBACLAFKSPIT-UHFFFAOYSA-N 0.000 claims description 14
- DKGAVHZHDRPRBM-UHFFFAOYSA-N Tert-Butanol Chemical compound CC(C)(C)O DKGAVHZHDRPRBM-UHFFFAOYSA-N 0.000 claims description 13
- 150000002430 hydrocarbons Chemical class 0.000 claims description 12
- 238000005286 illumination Methods 0.000 claims description 11
- 239000007864 aqueous solution Substances 0.000 claims description 10
- DIOQZVSQGTUSAI-UHFFFAOYSA-N decane Chemical compound CCCCCCCCCC DIOQZVSQGTUSAI-UHFFFAOYSA-N 0.000 claims description 10
- -1 octyne Chemical compound 0.000 claims description 9
- WPYMKLBDIGXBTP-UHFFFAOYSA-N benzoic acid Chemical compound OC(=O)C1=CC=CC=C1 WPYMKLBDIGXBTP-UHFFFAOYSA-N 0.000 claims description 8
- 239000003153 chemical reaction reagent Substances 0.000 claims description 8
- 238000011049 filling Methods 0.000 claims description 7
- 239000010453 quartz Substances 0.000 claims description 7
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 7
- 229910052724 xenon Inorganic materials 0.000 claims description 7
- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical group [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 0.000 claims description 7
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 claims description 6
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 6
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims description 6
- IMNFDUFMRHMDMM-UHFFFAOYSA-N N-Heptane Chemical compound CCCCCCC IMNFDUFMRHMDMM-UHFFFAOYSA-N 0.000 claims description 6
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 6
- 150000001875 compounds Chemical class 0.000 claims description 6
- 239000002253 acid Substances 0.000 claims description 5
- 239000000203 mixture Substances 0.000 claims description 5
- JRZJOMJEPLMPRA-UHFFFAOYSA-N 1-nonene Chemical compound CCCCCCCC=C JRZJOMJEPLMPRA-UHFFFAOYSA-N 0.000 claims description 4
- FJKROLUGYXJWQN-UHFFFAOYSA-N 4-hydroxybenzoic acid Chemical compound OC(=O)C1=CC=C(O)C=C1 FJKROLUGYXJWQN-UHFFFAOYSA-N 0.000 claims description 4
- 239000005711 Benzoic acid Substances 0.000 claims description 4
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 claims description 4
- HUMNYLRZRPPJDN-UHFFFAOYSA-N benzaldehyde Chemical compound O=CC1=CC=CC=C1 HUMNYLRZRPPJDN-UHFFFAOYSA-N 0.000 claims description 4
- 235000010233 benzoic acid Nutrition 0.000 claims description 4
- ILLHQJIJCRNRCJ-UHFFFAOYSA-N dec-1-yne Chemical compound CCCCCCCCC#C ILLHQJIJCRNRCJ-UHFFFAOYSA-N 0.000 claims description 4
- ZGEGCLOFRBLKSE-UHFFFAOYSA-N methylene hexane Natural products CCCCCC=C ZGEGCLOFRBLKSE-UHFFFAOYSA-N 0.000 claims description 4
- BKIMMITUMNQMOS-UHFFFAOYSA-N nonane Chemical compound CCCCCCCCC BKIMMITUMNQMOS-UHFFFAOYSA-N 0.000 claims description 4
- TVMXDCGIABBOFY-UHFFFAOYSA-N octane Chemical compound CCCCCCCC TVMXDCGIABBOFY-UHFFFAOYSA-N 0.000 claims description 4
- 150000002989 phenols Chemical class 0.000 claims description 4
- DTUQWGWMVIHBKE-UHFFFAOYSA-N phenylacetaldehyde Chemical compound O=CCC1=CC=CC=C1 DTUQWGWMVIHBKE-UHFFFAOYSA-N 0.000 claims description 4
- WSFSSNUMVMOOMR-NJFSPNSNSA-N methanone Chemical compound O=[14CH2] WSFSSNUMVMOOMR-NJFSPNSNSA-N 0.000 claims description 3
- LIKMAJRDDDTEIG-UHFFFAOYSA-N 1-hexene Chemical compound CCCCC=C LIKMAJRDDDTEIG-UHFFFAOYSA-N 0.000 claims description 2
- CGHIBGNXEGJPQZ-UHFFFAOYSA-N 1-hexyne Chemical compound CCCCC#C CGHIBGNXEGJPQZ-UHFFFAOYSA-N 0.000 claims description 2
- KWKAKUADMBZCLK-UHFFFAOYSA-N 1-octene Chemical compound CCCCCCC=C KWKAKUADMBZCLK-UHFFFAOYSA-N 0.000 claims description 2
- WLJVXDMOQOGPHL-PPJXEINESA-N 2-phenylacetic acid Chemical compound O[14C](=O)CC1=CC=CC=C1 WLJVXDMOQOGPHL-PPJXEINESA-N 0.000 claims description 2
- 229940090248 4-hydroxybenzoic acid Drugs 0.000 claims description 2
- 125000000041 C6-C10 aryl group Chemical group 0.000 claims description 2
- 239000004215 Carbon black (E152) Substances 0.000 claims description 2
- CTQNGGLPUBDAKN-UHFFFAOYSA-N O-Xylene Chemical compound CC1=CC=CC=C1C CTQNGGLPUBDAKN-UHFFFAOYSA-N 0.000 claims description 2
- IKHGUXGNUITLKF-XPULMUKRSA-N acetaldehyde Chemical compound [14CH]([14CH3])=O IKHGUXGNUITLKF-XPULMUKRSA-N 0.000 claims description 2
- 229960004365 benzoic acid Drugs 0.000 claims description 2
- YQGOJNYOYNNSMM-UHFFFAOYSA-N eosin Chemical compound [Na+].OC(=O)C1=CC=CC=C1C1=C2C=C(Br)C(=O)C(Br)=C2OC2=C(Br)C(O)=C(Br)C=C21 YQGOJNYOYNNSMM-UHFFFAOYSA-N 0.000 claims description 2
- YVXHZKKCZYLQOP-UHFFFAOYSA-N hept-1-yne Chemical compound CCCCCC#C YVXHZKKCZYLQOP-UHFFFAOYSA-N 0.000 claims description 2
- AFFLGGQVNFXPEV-UHFFFAOYSA-N n-decene Natural products CCCCCCCCC=C AFFLGGQVNFXPEV-UHFFFAOYSA-N 0.000 claims description 2
- OSSQSXOTMIGBCF-UHFFFAOYSA-N non-1-yne Chemical compound CCCCCCCC#C OSSQSXOTMIGBCF-UHFFFAOYSA-N 0.000 claims description 2
- QNGNSVIICDLXHT-UHFFFAOYSA-N para-ethylbenzaldehyde Natural products CCC1=CC=C(C=O)C=C1 QNGNSVIICDLXHT-UHFFFAOYSA-N 0.000 claims description 2
- 229940100595 phenylacetaldehyde Drugs 0.000 claims description 2
- PYWVYCXTNDRMGF-UHFFFAOYSA-N rhodamine B Chemical compound [Cl-].C=12C=CC(=[N+](CC)CC)C=C2OC2=CC(N(CC)CC)=CC=C2C=1C1=CC=CC=C1C(O)=O PYWVYCXTNDRMGF-UHFFFAOYSA-N 0.000 claims description 2
- 229940043267 rhodamine b Drugs 0.000 claims description 2
- 238000009210 therapy by ultrasound Methods 0.000 claims description 2
- 239000008096 xylene Substances 0.000 claims description 2
- WVDDGKGOMKODPV-UHFFFAOYSA-N Benzyl alcohol Chemical compound OCC1=CC=CC=C1 WVDDGKGOMKODPV-UHFFFAOYSA-N 0.000 claims 3
- XQXPVVBIMDBYFF-UHFFFAOYSA-N 4-hydroxyphenylacetic acid Chemical compound OC(=O)CC1=CC=C(O)C=C1 XQXPVVBIMDBYFF-UHFFFAOYSA-N 0.000 claims 2
- 239000000356 contaminant Substances 0.000 claims 2
- 239000000975 dye Substances 0.000 claims 2
- 125000006736 (C6-C20) aryl group Chemical group 0.000 claims 1
- 150000001298 alcohols Chemical class 0.000 claims 1
- 235000019445 benzyl alcohol Nutrition 0.000 claims 1
- 229960003887 dichlorophen Drugs 0.000 claims 1
- GTUVXOOHBUUGBH-UHFFFAOYSA-N furan;methanol Chemical compound OC.C=1C=COC=1 GTUVXOOHBUUGBH-UHFFFAOYSA-N 0.000 claims 1
- 238000002156 mixing Methods 0.000 claims 1
- 238000001782 photodegradation Methods 0.000 abstract description 7
- 230000007613 environmental effect Effects 0.000 abstract description 4
- 238000002360 preparation method Methods 0.000 abstract description 2
- WXNZTHHGJRFXKQ-UHFFFAOYSA-N 4-chlorophenol Chemical compound OC1=CC=C(Cl)C=C1 WXNZTHHGJRFXKQ-UHFFFAOYSA-N 0.000 description 13
- HFZWRUODUSTPEG-UHFFFAOYSA-N 2,4-dichlorophenol Chemical compound OC1=CC=C(Cl)C=C1Cl HFZWRUODUSTPEG-UHFFFAOYSA-N 0.000 description 9
- 230000000052 comparative effect Effects 0.000 description 8
- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 description 6
- 238000002474 experimental method Methods 0.000 description 6
- 230000035484 reaction time Effects 0.000 description 6
- 239000000243 solution Substances 0.000 description 6
- 238000002604 ultrasonography Methods 0.000 description 5
- 238000004128 high performance liquid chromatography Methods 0.000 description 4
- 239000000725 suspension Substances 0.000 description 4
- 239000003054 catalyst Substances 0.000 description 3
- 230000003247 decreasing effect Effects 0.000 description 3
- XPFVYQJUAUNWIW-UHFFFAOYSA-N furfuryl alcohol Chemical compound OCC1=CC=CO1 XPFVYQJUAUNWIW-UHFFFAOYSA-N 0.000 description 3
- 206010028980 Neoplasm Diseases 0.000 description 2
- 230000009471 action Effects 0.000 description 2
- 230000001699 photocatalysis Effects 0.000 description 2
- 239000011941 photocatalyst Substances 0.000 description 2
- 238000001179 sorption measurement Methods 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 238000002371 ultraviolet--visible spectrum Methods 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 208000024172 Cardiovascular disease Diseases 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 208000031320 Teratogenesis Diseases 0.000 description 1
- 238000004847 absorption spectroscopy Methods 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 208000026106 cerebrovascular disease Diseases 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000035622 drinking Effects 0.000 description 1
- 230000002526 effect on cardiovascular system Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 229910021645 metal ion Inorganic materials 0.000 description 1
- 238000005065 mining Methods 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- WVDDGKGOMKODPV-ZQBYOMGUSA-N phenyl(114C)methanol Chemical compound O[14CH2]C1=CC=CC=C1 WVDDGKGOMKODPV-ZQBYOMGUSA-N 0.000 description 1
- 238000007146 photocatalysis Methods 0.000 description 1
- 238000013033 photocatalytic degradation reaction Methods 0.000 description 1
- 238000013032 photocatalytic reaction Methods 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N titanium dioxide Inorganic materials O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 1
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
- 238000000870 ultraviolet spectroscopy Methods 0.000 description 1
- 238000003911 water pollution 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
- B01J31/00—Catalysts comprising hydrides, coordination complexes or organic compounds
- B01J31/02—Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides
-
- 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
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/30—Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
- B01J35/39—Photocatalytic properties
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/30—Treatment of water, waste water, or sewage by irradiation
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/308—Dyes; Colorants; Fluorescent agents
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/34—Organic compounds containing oxygen
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/34—Organic compounds containing oxygen
- C02F2101/345—Phenols
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/36—Organic compounds containing halogen
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/38—Organic compounds containing nitrogen
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/40—Organic compounds containing sulfur
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/10—Photocatalysts
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- Engineering & Computer Science (AREA)
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- Hydrology & Water Resources (AREA)
- Water Supply & Treatment (AREA)
- Environmental & Geological Engineering (AREA)
- Health & Medical Sciences (AREA)
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Abstract
The invention provides a method for degrading organic pollutants in a water body by using black carbon light. The method comprises the following steps: 1) burning C under the condition of controllable combustion-oxygen ratio6‑C20Hydrocarbons produce black carbon. 2) Adding the prepared black carbon and the water solution of the water organic pollutants into a photoreactor to form a reaction system, and stirring the reaction system under the irradiation of simulated sunlight to realize the degradation of the water organic pollutants. Compared with the prior art, the method has the main advantages that: the preparation of the black carbon is cheap and simple, the photodegradation reaction condition is mild, the reaction operation is simple, the universality is wide, and the black carbon can degrade various water organic pollutants in water and has very important environmental significance.
Description
Technical Field
The invention belongs to the technical field of water pollution degradation, and particularly relates to a method for degrading organic pollutants in a water body by using black carbon light.
Background
Along with the continuous improvement of the living standard of people, the pollution condition of water bodies is intensified worldwide along with the great development of industry. Especially, the discharge of organic matters in various large mining plants causes the pollution of the organic matters in the water body. Drinking polluted water for a long time can cause tumors, cancers, cardiovascular and cerebrovascular diseases, stones, teratogenesis and the like. Therefore, the degradation of organic pollutants in the water body has very important environmental significance. In recent years, the photodegradation of organic matters is widely concerned by people due to the characteristics of environmental protection and the like.
A commonly used photodegradation catalyst is TiO2And CdS and ZnO are not good photocatalysts for degrading pollutants in water because the chemical properties of CdS and ZnO are unstable, so that photodissolution can be carried out while photocatalysis is carried out, and dissolved metal ions have certain biotoxicity. TiO 22The catalyst is used for photocatalytic decomposition of water to produce hydrogen and photocatalyst degradation of organic matters, but the problems of high cost, low catalytic efficiency under sunlight and the like caused by the need of using noble metal load in the photocatalytic degradation are solved.
Disclosure of Invention
In order to overcome the defects of the prior art, the invention provides a method for degrading organic pollutants in a water body by using black carbon light, which comprises the following steps:
1) burning C under the condition of controllable combustion-oxygen ratio6-C20Hydrocarbon compounds to prepare black carbon;
2) adding the black carbon prepared in the step 1) and the aqueous solution containing the organic pollutants into a photoreactor to form a reaction system, and stirring the reaction system under the irradiation of simulated sunlight at a controlled temperature to realize the degradation of the organic pollutants in the water body.
According to an embodiment of the present invention, wherein in step 1: the combustion-oxygen ratio is C6-C20A molar ratio of hydrocarbon compound to oxygen of 0.05 to 0.2:1, such as 0.1 to 0.19:1, such as 0.10 to 0.18:1, such as 0.10:1, 0.11:1, 0.12:1, 0.13:1, 0.14:1, 0.15:1, 0.16:1, 0.17:1 or 0.18: 1. The black carbon which can be used for photodegrading organic pollutants in water cannot be prepared by adopting a fuel-oxygen ratio of 0.05-0.2: 1.
According to an embodiment of the present invention, wherein in step 1: said C6-C20The hydrocarbon compound is selected from C6-C20Alkyl of (C)6-C20Alkenyl of, C6-C20Alkynyl of (A), C6-C20Aryl of (a); for example selected from C6-C10Alkyl of (C)6-C10Alkenyl of, C6-C10Alkynyl of (A), C6-C10Aryl group of (1).
Illustratively, said C6-C20The hydrocarbon compound is at least one selected from n-hexane, n-heptane, n-octane, n-nonane, n-decane, hexene, heptene, octene, nonene, decene, hexyne, heptyne, octyne, nonyne, decyne, benzene, toluene, xylene, etc. Preferably, said C6-C20The hydrocarbon compound is at least one selected from n-hexane, n-decane and toluene.
According to an embodiment of the present invention, step 1 specifically is:
c is to be6-C20Is filled into the fuel pool and ignited by a wick extending into the fuel pool6-C20By controlling the introduction of N into the combustion chamber2And O2Content control of (C)6-C20The combustion oxygen ratio of the hydrocarbon compound in the combustion process, and collecting black carbon generated by combustion.
Exemplarily, step 1 specifically includes:
the method comprises the steps of filling chromatographic pure normal hexane into a fuel pool, igniting the normal hexane to generate flame through a wick extending into the fuel pool, and accurately controlling N to enter a combustion chamber2And O2The oxygen-fuel ratio of the normal hexane combustion process is controlled, black carbon is collected by a quartz plate with the thickness of 10 cm x 10 cm at a position 4 cm above the flame, the collected black carbon is scraped off, and the black carbon is placed in a sealed reagent bottle for standby.
According to the embodiment of the invention, after the black carbon prepared in the step 1) and the aqueous solution containing the organic pollutants are added into a photoreactor to form a reaction system, the reaction system in the photoreactor is subjected to ultrasonic treatment and stirring, so that the organic pollutants and the black carbon are uniformly dispersed; then stirring under the condition of simulating sunlight irradiation and controlling the temperature to realize the degradation of organic pollutants in the water body;
according to an embodiment of the present invention, wherein in step 2:
the concentration of black carbon in the reaction system is 0.01-12mg/ml, for example 0.05-8mg/ml, for example 0.1-6mg/ml, such as 0.1mg/ml, 0.18mg/ml, 0.2mg/ml, 0.3mg/ml, 0.33mg/ml, 0.5mg/ml, 0.8mg/ml, 1mg/ml, 2mg/ml, 3mg/ml, 4mg/ml, 5mg/ml or 6 mg/ml;
the organic pollutant in the reaction system is selected from organic dye, phenolic compound, alcohol compound, acid compound and aldehyde compound. For example, the organic dye may be selected from methyl orange, rhodamine B, eosin; the phenolic compound may be selected from: phenol, 2, 4-dichlorophenol, bisphenol a; the alcohol compound may be selected from: methanol, ethanol, tert-butanol, benzyl alcohol, furfuryl alcohol; the acid compound may be selected from: benzoic acid, phenylacetic acid, parahydroxybenzoic acid, parahydroxyacetic acid; the aldehyde compound may be selected from: formaldehyde, acetaldehyde, benzaldehyde, phenylacetaldehyde;
the initial concentration of the organic pollutants in the reaction system is 10-6M～10-3M, e.g. 10-6M、10-5M、2*10-5M、3*10-5M、5*10-5M、10-4M or 10-3M; the initial concentration refers to the concentration of organic pollutants in a reaction system before the photocatalytic reaction starts.
The photoreactor is a reactor which can be transparent to a light source, such as a transparent reactor;
the simulated sunlight is a xenon lamp light source, the wavelength range of the simulated sunlight is 300nm-700nm, and the power of the simulated sunlight is 300W;
the temperature of the reaction may be from 5 to 80 deg.C, for example from 10 to 60 deg.C, for example from 20 to 30 deg.C;
the illumination time may be 0.5 hours or more, for example 1 to 40 hours, such as 1 to 12 hours, the illumination being carried out with stirring;
the reaction is carried out under actual atmospheric conditions.
Advantageous effects
The invention uses black carbon to realize photodegradation of organic pollutants in water body, and the technical core is combustion C6-C20Preparation of hydrocarbon compound ofThe prepared black carbon can degrade organic pollutants in water under the irradiation of simulated sunlight. The black carbon is cheap and simple to prepare, mild in photodegradation reaction conditions, free of any catalyst, simple in reaction operation, wide in universality, and capable of degrading various organic pollutants in water, and has very important environmental significance.
Drawings
FIG. 1 is a graph showing the degradation kinetics of 2, 4-dichlorophenol (2,4-DCP) in example 1 and comparative example 1;
FIG. 2 is a graph showing the degradation kinetics of Methyl Orange (MO) in example 2 and comparative example 2.
Detailed Description
The invention will be further illustrated with reference to the following specific examples. It should be understood that these examples are only for illustrating the present invention and are not intended to limit the scope of the present invention. In addition, it should be understood that various changes or modifications can be made by those skilled in the art after reading the disclosure of the present invention, and such equivalents also fall within the scope of the invention.
The experimental methods used in the following examples are all conventional methods unless otherwise specified; reagents, materials and the like used in the following examples are commercially available unless otherwise specified; the wavelength range of the 300W xenon lamp used in the examples described below was 300nm to 700 nm.
Example 1
The method comprises the steps of filling chromatographic pure normal hexane into a fuel pool, igniting the normal hexane to generate flame through a wick extending into the fuel pool, and accurately controlling N to enter a combustion chamber2And O2The content of the (C) in the (C) is controlled to be the fuel-oxygen ratio in the normal hexane combustion process, and the fuel-oxygen ratio is controlled to be 0.18 in the experiment. The black carbon was collected 4 cm above the flame using a 10 cm by 10 cm quartz plate, scraped off, and placed in a sealed reagent bottle for use.
The black carbon prepared above is added into a temperature-controlled transparent photochemical reactor containing 2, 4-dichlorophenol aqueous solution. Wherein the black carbon concentration is 0.33mg/ml, and the initial concentration of 2, 4-dichlorophenol is 5 x 10-5M, then the photoreactor was sonicated for 5 minutes to suspendThe liquids are mixed evenly. After the ultrasound was completed, the reactor was stirred (20 rpm) for 30 minutes under an open temperature control (25 ℃) so that the 2, 4-dichlorophenol and black carbon samples were uniformly dispersed. Then, the mixture was irradiated with a 300W xenon lamp for 12 hours under temperature control and stirring, and samples were taken after 0, 2,4, 6, 8, 10, and 12 hours of irradiation. Detecting the concentration of 2, 4-chlorophenol in the reaction solution at different reaction times by high performance liquid chromatography, as shown in figure 1, the concentration in figure 10I.e. the initial concentration. From the chromatographic results: with the progress of the illumination reaction, the concentration of the 2, 4-chlorophenol is gradually reduced, and the degradation rate of the 2, 4-chlorophenol reaches more than 70 percent after 12 hours of illumination.
Example 2
The method comprises the steps of filling chromatographic pure normal hexane into a fuel pool, igniting the normal hexane to generate flame through a wick extending into the fuel pool, and accurately controlling N to enter a combustion chamber2And O2The content of the (C) in the (C) is controlled to be the fuel-oxygen ratio in the normal hexane combustion process, and the fuel-oxygen ratio is controlled to be 0.18 in the experiment. The black carbon was collected 4 cm above the flame using a 10 cm by 10 cm quartz plate, scraped off, and placed in a sealed reagent bottle for use.
The black carbon prepared above is added into a temperature-controlled transparent photochemical reactor containing methyl orange aqueous solution. Wherein the black carbon concentration is 0.33mg/ml, and the initial concentration of methyl orange is 4 x 10-5M, then the photoreactor was sonicated for 5 minutes to mix the suspension uniformly. After the ultrasound was completed, the reactor was stirred (20 rpm) for 30 minutes under open temperature control (25 ℃) so that the methyl orange and black carbon samples were uniformly dispersed. Then, the mixture was irradiated with a 300W xenon lamp for 12 hours under temperature control and stirring, and samples were taken after 0, 3, 6, 9, and 12 hours of irradiation. The concentration of methyl orange in the reaction solution at different reaction times was measured by UV-visible absorption spectroscopy, as shown in FIG. 2, the concentration in FIG. 20I.e. the initial concentration. From the uv-vis absorption spectrum results: with the progress of the illumination reaction, the concentration of the methyl orange is gradually reduced, and the degradation rate of the methyl orange reaches more than 70 percent after 12 hours of illumination.
Example 3
Filling chromatographic pure n-hexane into a fuel pool, and igniting the n-hexane by a wick extending into the fuel pool to generateFlame, by precise control of N into the combustion chamber2And O2The content of the (C) in the (C) is controlled to be the fuel-oxygen ratio in the normal hexane combustion process, and the fuel-oxygen ratio is controlled to be 0.18 in the experiment. The black carbon was collected 4 cm above the flame using a 10 cm by 10 cm quartz plate, scraped off, and placed in a sealed reagent bottle for use.
The black carbon prepared above is added into a temperature-controlled transparent photochemical reactor containing bisphenol A aqueous solution. Wherein the black carbon concentration is 0.33mg/ml, and the initial concentration of bisphenol A is 2 x 10-5M, then the photoreactor was sonicated for 5 minutes to mix the suspension uniformly. After the ultrasound was completed, the reactor was stirred (20 rpm) for 30 minutes under open temperature control (25 ℃) so that the bisphenol A and black carbon samples were uniformly dispersed. Then, the mixture was irradiated with a 300W xenon lamp for 12 hours under temperature control and stirring, and samples were taken after 0, 2,4, 6, 8, 10, and 12 hours of irradiation. The concentration of bisphenol A in the reaction solution was measured by high performance liquid chromatography for different reaction times. With the progress of the illumination reaction, the concentration of the bisphenol A is gradually reduced, and the degradation rate of the bisphenol A reaches more than 70 percent after 12 hours of illumination.
Example 4
The procedure of example 4 was the same as that of example 1 except that toluene was used in place of n-hexane in example 1, the fuel/oxygen ratio was 0.10, and tert-butanol was used in place of 2, 4-chlorophenol in example 1, and it was found that the concentration of tert-butanol was gradually decreased as the photoreaction proceeded, and that the degradation rate of tert-butanol reached 70% or more when the photoreaction was performed for 12 hours.
Example 5
The procedure of example 5 was the same as that of example 1 except that decane was used in place of n-hexane in example 1, the fuel/oxygen ratio was 0.13, and benzoic acid was used in place of 2, 4-chlorophenol in example 1, and it was found that the tert-butanol concentration gradually decreased as the photoreaction proceeded, and that the degradation rate of benzoic acid reached 70% or more in 12 hours of light irradiation.
Example 6
The procedure of example 5 was the same as that of example 1 except that 2, 4-chlorophenol in example 1 was replaced with formaldehyde, and the results showed that the formaldehyde concentration gradually decreased as the light reaction proceeded, and that the degradation rate of formaldehyde reached 70% or more after 12 hours of light irradiation.
Comparative example 1
The method comprises the steps of filling chromatographic pure normal hexane into a fuel pool, igniting the normal hexane to generate flame through a wick extending into the fuel pool, and accurately controlling N to enter a combustion chamber2And O2The content of the (C) in the (C) is controlled to be the fuel-oxygen ratio in the normal hexane combustion process, and the fuel-oxygen ratio is controlled to be 0.18 in the experiment. The black carbon was collected 4 cm above the flame using a 10 cm by 10 cm quartz plate, scraped off, and placed in a sealed reagent bottle for use.
The black carbon prepared above is added into a temperature-controlled transparent photochemical reactor containing 2, 4-dichlorophenol aqueous solution. Wherein the black carbon concentration is 0.33mg/ml, and the initial concentration of 2, 4-dichlorophenol is 5 x 10-5M, then the photoreactor was sonicated for 5 minutes to mix the suspension uniformly. After the ultrasound was completed, the reactor was stirred (20 rpm) for 30 minutes under an open temperature control (25 ℃) so that the 2, 4-dichlorophenol and black carbon samples were uniformly dispersed. Stirring was carried out under a controlled temperature for 12 hours in the dark, and samples were taken after stirring for 0, 2,4, 6, 8, 10, and 12 hours, respectively. The concentration of 2, 4-chlorophenol in the reaction solution was measured by HPLC at different reaction times, as shown in FIG. 1. From the chromatographic results: stirring under dark condition, and keeping the concentration of 2, 4-chlorophenol basically unchanged.
As can be seen from the above example 1 and comparative example 1, the decrease in the concentration of 2, 4-chlorophenol in example 1 is due to photochemical degradation rather than adsorption on black carbon.
Comparative example 2
The method comprises the steps of filling chromatographic pure normal hexane into a fuel pool, igniting the normal hexane to generate flame through a wick extending into the fuel pool, and accurately controlling N to enter a combustion chamber2And O2The content of the (C) in the (C) is controlled to be the fuel-oxygen ratio in the normal hexane combustion process, and the fuel-oxygen ratio is controlled to be 0.18 in the experiment. The black carbon was collected 4 cm above the flame using a 10 cm by 10 cm quartz plate, scraped off, and placed in a sealed reagent bottle for use.
The black carbon prepared above is added into a temperature-controlled transparent photochemical reactor containing methyl orange aqueous solution. Wherein is blackThe carbon concentration was 0.33mg/ml and the initial concentration of methyl orange was 4 x 10-5M, then the photoreactor was sonicated for 5 minutes to mix the suspension uniformly. After the ultrasound was completed, the reactor was stirred (20 rpm) for 30 minutes under open temperature control (25 ℃) so that the methyl orange and black carbon samples were uniformly dispersed. Stirring was carried out under a controlled temperature for 12 hours in the dark, and samples were taken after stirring for 0, 3, 6, 9, and 12 hours, respectively. The concentration of methyl orange in the reaction solution was measured by UV-Vis spectroscopy at different reaction times as shown in FIG. 2. From the uv-vis spectra results: the mixture was stirred under dark conditions, and the methyl orange concentration remained essentially unchanged.
As can be seen from the above example 2 and comparative example 2, the reduction of the methyl orange concentration in example 2 is photochemical degradation, excluding the adsorption of methyl orange on the black carbon surface.
Comparative example 3
The initial concentration is 5 x 10-5M2, 4-dichlorophenol aqueous solution is added into a temperature-controlled transparent open photochemical reactor, and then irradiated with a 300W xenon lamp under temperature control (25 ℃) and stirring for 12 hours, and samples are taken after 0, 2,4, 6, 8, 10 and 12 hours of light irradiation. The concentration of 2, 4-chlorophenol in the reaction solution of different reaction times is detected by high performance liquid chromatography, and the concentration of 2, 4-chlorophenol is basically kept unchanged along with the progress of the light reaction, which shows that 2, 4-chlorophenol does not undergo photodegradation per se, and the photodegradation of 2, 4-chlorophenol in example 1 is caused by the action of black carbon.
As can be seen from the above examples 1-3 and comparative examples 1-3, the method of the present application can effectively remove organic substances in the water body. The organic pollutants in the water body are difficult to degrade under the illumination, and the organic pollutants in the water body are effectively degraded under the action of black carbon.
Claims (17)
1. A method for degrading organic pollutants in a water body by using black carbon light comprises the following steps:
1) burning C under the condition of controllable combustion-oxygen ratio6-C20Hydrocarbon compounds to prepare black carbon;
2) mixing the black carbon prepared in the step 1) with a mixture containingAdding the aqueous solution of the organic pollutants into a photoreactor to form a reaction system, and stirring the reaction system under the irradiation of simulated sunlight at a controlled temperature to realize the degradation of the organic pollutants in the water body; the combustion-oxygen ratio is C6-C20The molar ratio of the hydrocarbon compound to the oxygen is 0.05-0.2: 1;
said C6-C20The hydrocarbon compound is selected from C6-C20Alkyl of (C)6-C20Alkenyl of, C6-C20Alkynyl of (A), C6-C20Aryl group of (1).
2. The method according to claim 1, wherein in step 1): the molar ratio is 0.1-0.2: 1.
3. The method according to claim 2, wherein in step 1): the molar ratio is 0.10-0.18: 1.
4. The method according to claim 1, wherein in step 1): said C6-C20The hydrocarbon compound is selected from C6-C10Alkyl of (C)6-C10Alkenyl of, C6-C10Alkynyl of (A), C6-C10Aryl group of (1).
5. The method of claim 4, wherein C is6-C20The hydrocarbon compound is at least one selected from n-hexane, n-heptane, n-octane, n-nonane, n-decane, hexene, heptene, octene, nonene, decene, hexyne, heptyne, octyne, nonyne, decyne, benzene, toluene and xylene.
6. The method of claim 5, wherein C is6-C20The hydrocarbon compound is at least one selected from n-hexane, n-decane and toluene.
7. The method according to claim 1, wherein step 1) is specifically:
c is to be6-C20Is filled into the fuel pool and ignited by a wick extending into the fuel pool6-C20By controlling the introduction of N into the combustion chamber2And O2Content control of (C)6-C20The combustion oxygen ratio of the hydrocarbon compound in the combustion process, and collecting black carbon generated by combustion.
8. The method according to claim 7, wherein step 1) is specifically:
the method comprises the steps of filling chromatographic pure normal hexane into a fuel pool, igniting the normal hexane to generate flame through a wick extending into the fuel pool, and accurately controlling N to enter a combustion chamber2And O2The oxygen-fuel ratio of the normal hexane combustion process is controlled, black carbon is collected by a quartz plate with the thickness of 10 cm x 10 cm at a position 4 cm above the flame, the collected black carbon is scraped off, and the black carbon is placed in a sealed reagent bottle for standby.
9. The method according to claim 1, wherein after the black carbon prepared in step 1) and the aqueous solution containing the organic pollutants are added into the photoreactor to form a reaction system, the reaction system in the photoreactor is stirred after being subjected to ultrasonic treatment, so that the organic pollutants and the black carbon are uniformly dispersed; and then stirring under the condition of simulating sunlight irradiation to realize the degradation of organic pollutants in the water body.
10. The method according to claim 1, wherein in step 2): the concentration of black carbon in the reaction system is 0.01-12 mg/ml.
11. The method of claim 10, wherein in step 2): the concentration of black carbon in the reaction system is 0.05-8 mg/ml.
12. The method of claim 11, wherein in step 2): the concentration of black carbon in the reaction system is 0.1-6 mg/ml.
13. The method as claimed in any one of claims 1 to 12, wherein the organic contaminant in the reaction system is selected from organic dyes, phenolic compounds, alcohol compounds, acid compounds, aldehyde compounds.
14. The method of claim 13, wherein the organic dye is selected from methyl orange, rhodamine B, eosin; the phenolic compound is selected from phenol, 2, 4-dichlorophen and bisphenol A; the alcohol compound is selected from methanol, ethanol, tert-butyl alcohol, benzyl alcohol and furancarbinol; the acid compound is selected from benzoic acid, phenylacetic acid, p-hydroxybenzoic acid and p-hydroxyphenylacetic acid; the aldehyde compound is selected from formaldehyde, acetaldehyde, benzaldehyde and phenylacetaldehyde.
15. The method of claim 1, wherein the initial concentration of the organic contaminant in the reaction system is 10%- 6M～10-3M。
16. The method of claim 1, wherein the simulated sunlight is a xenon lamp light source with a wavelength range of 300nm to 700nm and a power of 300W.
17. The process according to any one of claims 1 to 9, wherein the temperature of the reaction is 5 to 80 ℃;
the illumination time is more than 0.5 hour, and the illumination is carried out under stirring;
the reaction is carried out under actual atmospheric conditions.
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| CN101644446A (en) * | 2009-09-16 | 2010-02-10 | 浙江中控技术股份有限公司 | Control method and system of air volume-fuel ratio in preparing carbon black |
| CN103143377A (en) * | 2013-02-19 | 2013-06-12 | 中国科学院理化技术研究所 | Application of heteroatoms doped aqueous carbon quantum dot in photocatalyst |
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