CN113289600A - 杂原子掺杂碳点光催化降解工业废气 - Google Patents
杂原子掺杂碳点光催化降解工业废气 Download PDFInfo
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- 239000007789 gas Substances 0.000 title claims abstract description 71
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 19
- 238000013033 photocatalytic degradation reaction Methods 0.000 title claims abstract description 10
- 125000005842 heteroatom Chemical group 0.000 title claims description 6
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims abstract description 8
- 230000001590 oxidative effect Effects 0.000 claims abstract description 6
- 238000000034 method Methods 0.000 claims description 12
- 229910002091 carbon monoxide Inorganic materials 0.000 claims description 10
- 238000001027 hydrothermal synthesis Methods 0.000 claims description 5
- 150000003254 radicals Chemical class 0.000 claims description 5
- 238000000197 pyrolysis Methods 0.000 claims description 4
- 229910052801 chlorine Inorganic materials 0.000 claims description 3
- 229910052688 Gadolinium Inorganic materials 0.000 claims description 2
- 229910052782 aluminium Inorganic materials 0.000 claims description 2
- 229910052796 boron Inorganic materials 0.000 claims description 2
- 229910052794 bromium Inorganic materials 0.000 claims description 2
- 229910052804 chromium Inorganic materials 0.000 claims description 2
- 229910052802 copper Inorganic materials 0.000 claims description 2
- 229910052731 fluorine Inorganic materials 0.000 claims description 2
- 229910052740 iodine Inorganic materials 0.000 claims description 2
- 229910052742 iron Inorganic materials 0.000 claims description 2
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- 238000010189 synthetic method Methods 0.000 claims 1
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 description 33
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- KKEYFWRCBNTPAC-UHFFFAOYSA-N Terephthalic acid Chemical compound OC(=O)C1=CC=C(C(O)=O)C=C1 KKEYFWRCBNTPAC-UHFFFAOYSA-N 0.000 description 16
- 238000000502 dialysis Methods 0.000 description 15
- 239000002243 precursor Substances 0.000 description 15
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- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 10
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 8
- RAHZWNYVWXNFOC-UHFFFAOYSA-N Sulphur dioxide Chemical compound O=S=O RAHZWNYVWXNFOC-UHFFFAOYSA-N 0.000 description 8
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 7
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- RWSOTUBLDIXVET-UHFFFAOYSA-N Dihydrogen sulfide Chemical compound S RWSOTUBLDIXVET-UHFFFAOYSA-N 0.000 description 6
- 229910000037 hydrogen sulfide Inorganic materials 0.000 description 6
- 229910021529 ammonia Inorganic materials 0.000 description 5
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 4
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- 229910002092 carbon dioxide Inorganic materials 0.000 description 4
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- NNMXSTWQJRPBJZ-UHFFFAOYSA-K europium(iii) chloride Chemical compound Cl[Eu](Cl)Cl NNMXSTWQJRPBJZ-UHFFFAOYSA-K 0.000 description 2
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- UMGDCJDMYOKAJW-UHFFFAOYSA-N thiourea Chemical compound NC(N)=S UMGDCJDMYOKAJW-UHFFFAOYSA-N 0.000 description 2
- 239000002912 waste gas Substances 0.000 description 2
- JIAARYAFYJHUJI-UHFFFAOYSA-L zinc dichloride Chemical compound [Cl-].[Cl-].[Zn+2] JIAARYAFYJHUJI-UHFFFAOYSA-L 0.000 description 2
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 1
- 229910021555 Chromium Chloride Inorganic materials 0.000 description 1
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- 229910021380 Manganese Chloride Inorganic materials 0.000 description 1
- GLFNIEUTAYBVOC-UHFFFAOYSA-L Manganese chloride Chemical compound Cl[Mn]Cl GLFNIEUTAYBVOC-UHFFFAOYSA-L 0.000 description 1
- 229920000877 Melamine resin Polymers 0.000 description 1
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 description 1
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- 229910000147 aluminium phosphate Inorganic materials 0.000 description 1
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- ATBAMAFKBVZNFJ-UHFFFAOYSA-N beryllium atom Chemical compound [Be] ATBAMAFKBVZNFJ-UHFFFAOYSA-N 0.000 description 1
- QGJOPFRUJISHPQ-NJFSPNSNSA-N carbon disulfide-14c Chemical compound S=[14C]=S QGJOPFRUJISHPQ-NJFSPNSNSA-N 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 239000011651 chromium Substances 0.000 description 1
- QSWDMMVNRMROPK-UHFFFAOYSA-K chromium(3+) trichloride Chemical compound [Cl-].[Cl-].[Cl-].[Cr+3] QSWDMMVNRMROPK-UHFFFAOYSA-K 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 238000009833 condensation Methods 0.000 description 1
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- 238000001514 detection method Methods 0.000 description 1
- 238000012851 eutrophication Methods 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 229960002089 ferrous chloride Drugs 0.000 description 1
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- MEANOSLIBWSCIT-UHFFFAOYSA-K gadolinium trichloride Chemical compound Cl[Gd](Cl)Cl MEANOSLIBWSCIT-UHFFFAOYSA-K 0.000 description 1
- 238000005286 illumination Methods 0.000 description 1
- 238000001727 in vivo Methods 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- NMCUIPGRVMDVDB-UHFFFAOYSA-L iron dichloride Chemical compound Cl[Fe]Cl NMCUIPGRVMDVDB-UHFFFAOYSA-L 0.000 description 1
- RBTARNINKXHZNM-UHFFFAOYSA-K iron trichloride Chemical compound Cl[Fe](Cl)Cl RBTARNINKXHZNM-UHFFFAOYSA-K 0.000 description 1
- 239000011777 magnesium Substances 0.000 description 1
- 239000011572 manganese Substances 0.000 description 1
- 235000002867 manganese chloride Nutrition 0.000 description 1
- 239000011565 manganese chloride Substances 0.000 description 1
- 229940099607 manganese chloride Drugs 0.000 description 1
- JDSHMPZPIAZGSV-UHFFFAOYSA-N melamine Chemical compound NC1=NC(N)=NC(N)=N1 JDSHMPZPIAZGSV-UHFFFAOYSA-N 0.000 description 1
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 description 1
- 229910052753 mercury Inorganic materials 0.000 description 1
- 238000001000 micrograph Methods 0.000 description 1
- 229910000069 nitrogen hydride Inorganic materials 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 239000013618 particulate matter Substances 0.000 description 1
- 229920001223 polyethylene glycol Polymers 0.000 description 1
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- 239000011701 zinc Substances 0.000 description 1
- 235000005074 zinc chloride Nutrition 0.000 description 1
- 239000011592 zinc chloride Substances 0.000 description 1
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Abstract
本发明描述了一种杂原子掺杂碳点光催化降解工业废气,合成能产生大量具有强氧化性自由基的杂原子掺杂碳点X‑CDs,在光照射下,即可与工业废气中的还原性气体发生反应,杂原子掺杂碳点X‑CDs具有廉价,易制备,高光稳定性,催化效率高等优势,具有绿色环保,简单迅速,成本低廉,性质稳定,适合进行大规模工业废气的有效处理。
Description
技术领域
本发明涉及废气处理技术领域,具体涉及杂原子掺杂碳点(X-CDs)光催化降解工业废气的绿色高效处理方法。
背景技术
工业废气,是指企业厂区内燃料燃烧和生产工艺过程中产生的各种排入空气的含有污染物气体的总称。工业废气包括:二氧化碳、二硫化碳、硫化氢、氟化物、氮氧化物、氯、氯化氢、一氧化碳、硫酸、铅汞、铍化物、烟尘及生产性粉尘,排入大气,会污染空气,这些物质通过不同的途径经过呼吸道进入人的体内,有的直接产生危害,有的还有蓄积作用,会更加严重的危害人的健康,不同物质会有不同影响。另外会造成多种环境影响,包括氮氧化物的污染、臭氧污染、酸沉降、颗粒物污染、富营养化等问题。
工业废气的处理技术有吸收法、吸附法、热破坏法、生物处理法、冷凝法和低温离子技术,但目前都存在一定的缺点,如成本高,效率低,造成二次污染。
发明内容
本发明要解决的技术问题是提供一种在经济绿色的条件下利用X-CDs光催化大规模快速处理工业废气污染物。
本发明的目的可以通过以下技术方案来实现:
一种杂原子掺杂碳点光催化降解工业废气,合成能产生大量具有强氧化性自由基的杂原子掺杂碳点X-CDs,在光照射下,即可与工业废气中的还原性气体发生反应。
进一步地,所述杂原子掺杂碳点X-CDs的杂原子包括非金属元素N,S,F,O,P,Cl,Br,I,B;金属元素Fe,Cu,Al,Mn,Mo,Eu,Gd,Ru,Ti,Mg,Cr,Zn等中的一种或几种。
进一步地,所述杂原子掺杂碳点X-CDs的合成方法包括微波法,水热法,超声法以及热解法等。
进一步地,所述的具有强氧化性自由基包括·OH,O·-,1O2,·C或·N。
进一步地,所述的光为波长范围在250~800nm的紫外和可见光。
进一步地,所述的还原性工业废气包括H2S,SO2,NH3,CO2,NO2,NO,CO,HCl,CS2等中的一种或几种。
与现有技术相比,本发明取得了以下效果:
(1)杂原子掺杂碳点X-CDs具有廉价,易合成,高催化性能,绿色环保等优点,适合于进行大规模工业废气的处理;
(2)合成在光照下产生自由基的杂原子掺杂碳点X-CDs,强氧化性的杂原子掺杂碳点X-CDs与具有还原性的工业废气反应,实现低成本高选择性的处理。
(3)与其他工业废气处理的方法相比,杂原子掺杂碳点X-CDs净化率达到99%以上,而且处理效率高,适合大规模推广应用。
附图说明
图1为实施例中使用杂原子掺杂碳点S-CDs的透射电子显微镜示意图;
图2为实施例中使用杂原子掺杂碳点S-CDs对不同工业废气中一氧化碳气体的选择性示意图;
图3为实施例中使用Fe-CDs对工业废气中硫化氢的反应动力学曲线图;
图4为实施例中Cr-CDs对工业废气中二硫化碳气体选择性的示意图;
图5为实施例中使用P-CDs对工业废气中不同气体的选择性示意图。
具体实施方式
下面结合附图和具体实施例对本发明进行详细说明。
实施例1
选择柠檬酸,硫脲为前驱体水热反应180℃,6h,得到的产物通过800)rpm离心10min,用1000Da的透析袋纯化24h,得到纯的杂原子掺杂碳点S-CDs溶液。取部分溶液用对苯二甲酸可检测出·OH的产生。
在白光照射下,工业废气中的一氧化碳经过装有10mg S-CDs的进气管道,使其充分接触反应,最终从排气管道排出的气体检测合格后通入空气中。
图1为合成的S-CDs的透射电镜图,由图可见,合成的S-CDs粒径小于10nm,从图2对工业废气中混合气体的实验可得,对一氧化碳有很高的净化效率和选择性。
实施例2
选择邻苯二胺,柠檬酸,氯化铜为前驱体,在220℃下热解反应4h,得到的产物通过8000rpm离心10min,用1000Da的透析袋纯化24h,得到纯的Cu-CDs溶液。取部分溶液用对苯二甲酸可检测出·OH的产生。
在白光照射下,工业废气中的氨气经过装有10mg Cu-CDs的进气管道,使其充分接触反应,最终从排气管道排出的气体检测合格后通入空气中。
实施例3
选择邻苯二胺,氯化铁为前驱体水热反应180℃,4h,得到的产物通过8000rpm离心10min,用1000Da的透析袋纯化24h,得到纯的Fe-CDs溶液。取部分溶液用对苯二甲酸可检测出·OH的产生。
在白光照射下,工业废气中的硫化氢经过装有10mg Fe-CDs的进气管道,使其充分接触反应,最终从排气管道排出的气体检测合格后通入空气中,如图3所示,在15min可实现对废气中硫化氢的绝大部分净化。
实施例4
选择柠檬酸,硫酸为前驱体在500w下微波反应30min,得到的产物通过8000rpm离心10min,用1000Da的透析袋纯化24h,得到纯的杂原子掺杂碳点S-CDs溶液。取部分溶液用对苯二甲酸可检测出·OH的产生。
在模拟太阳光照射下,工业废气中的一氧化碳经过装有10mg S-CDs的进气管道,使其充分接触反应,最终从排气管道排出的气体检测合格后通入空气中。
实施例5
选择柠檬酸,氯化铕为前驱体,在500w条件下,超声处理20min,得到的产物通过8000rpm离心10min,用1000Da的透析袋纯化24h,得到纯的Eu-CDs溶液。取部分溶液用对苯二甲酸可检测出·OH的产生。
在白光照射下,工业废气中的二氧化碳经过装有10mg Eu-CDs的进气管道,使其充分接触反应,最终从排气管道排出的气体检测合格后通入空气中。
实施例6
选择柠檬酸,氯化铕为前驱体,在500w条件下,超声处理20min,得到的产物通过8000rpm离心10min,用1000Da的透析袋纯化24h,得到纯的Eu-CDs溶液。取部分溶液用对苯二甲酸可检测出·OH的产生。
在白光照射下,工业废气中的二氧化硫经过装有10mg Eu-CDs的进气管道,使其充分接触反应,最终从排气管道排出的气体检测合格后通入空气中。
实施例7
选择柠檬酸,氯化锰为前驱体,在750w条件下,超声处理10min,得到的产物通过8000rpm离心10min,用1000Da的透析袋纯化24h,得到纯的Mn-CDs溶液。取部分溶液用SOSG检测出1O2的产生。
在白光照射下,工业废气中的一氧化氮经过装有10mg Mn-CDs的进气管道,使其充分接触反应,最终从排气管道排出的气体检测合格后通入空气中。
实施例8
选择柠檬酸,聚噻吩为前驱体,在750w条件下,超声处理10min,得到的产物通过8000rpm离心10min,用1000Da的透析袋纯化24h,得到纯的S-CDs溶液。取部分溶液用ESR检测出O2·-的产生。
在白光照射下,工业废气中的氯化氢经过装有10mg S-CDs的进气管道,使其充分接触反应,最终从排气管道排出的气体检测合格后通入空气中。
实施例9
选择邻苯二胺,氯化亚铁为前驱体,在750w条件下,微波处理20min,得到的产物通过8000rpm离心10min,用1000Da的透析袋纯化24h,得到纯的Fe-CDs溶液。取部分溶液用ESR检测出·C的产生。
在白光照射下,工业废气中的二氧化硫经过装有10mg Fe-CDs的进气管道,使其充分接触反应,最终从排气管道排出的气体检测合格后通入空气中。
实施例10
选择苯酚,氯化锌为前驱体,在750w条件下,超声处理10min,得到的产物通过8000rpm离心10min,用1000Da的透析袋纯化24h,得到纯的Zn-CDs溶液。取部分溶液用SOSG检测出1O2的产生。
在白光照射下,工业废气中的一氧化碳经过装有10mg Zn-CDs的进气管道,使其充分接触反应,最终从排气管道排出的气体检测合格后通入空气中。
实施例11
选择柠檬酸,氯化铬为前驱体,在550w条件下,微波处理10min,得到的产物通过8000rpm离心10min,用1000Da的透析袋纯化24h,得到纯的Cr-CDs溶液。取部分溶液用ESR检测出O2·-的产生。
在白光照射下,工业废气中的二硫化碳经过装有10mg Cr-CDs的进气管道,使其充分接触反应,最终从排气管道排出的气体检测合格后通入空气中,如图4所示,对二硫化碳具有很高的选择性。
实施例12
选择三聚氰胺,柠檬酸为前驱体,在220℃下,热解处理1.5h,得到的产物通过8000rpm离心10min,用1000Da的透析袋纯化24h,得到纯的N-CDs溶液。取部分溶液用ESR检测出·N的产生。
在白光照射下,工业废气中的二氧化碳经过装有8mg N-CDs的进气管道,使其充分接触反应,最终从排气管道排出的气体检测合格后通入空气中。
实施例13
选择柠檬酸,氯化钆为前驱体,在750w条件下,超声处理10min,得到的产物通过8000rpm离心10min,用1000Da的透析袋纯化24h,得到纯的Gd-CDs溶液。取部分溶液用对苯二甲酸检测出·OH的产生。
在白光照射下,工业废气中的一氧化碳经过装有10mg Gd-CDs的进气管道,使其充分接触反应,最终从排气管道排出的气体检测合格后通入空气中。
实施例14
选择橘子皮,磷酸为前驱体,水热反应180℃,4h,得到的产物通过8000rpm离心10min,用1000Da的透析袋纯化24h,得到纯的P-CDs溶液。取部分溶液用SOSG检测出1O2的产生。
在白光照射下,工业废气中的氨气经过装有10mg P-CDs的进气管道,使其充分接触反应,最终从排气管道排出的气体检测合格后通入空气中,如图5所示,对氨气具有很高的选择性。
实施例15
选择聚乙二醇,柠檬酸,氯化铜为前驱体,在750w条件下,超声处理10min,得到的产物通过8000rpm离心10min,用1000Da的透析袋纯化24h,得到纯的Cu-CDs溶液。取部分溶液用对苯二甲酸检测出·OH的产生。
在白光照射下,工业废气中的二硫化碳经过装有10mg Cu-CDs的进气管道,使其充分接触反应,最终从排气管道排出的气体检测合格后通入空气中。
本发明的上述实施例仅仅是为清楚地说明本发明所作的举例,而并非是对本发明的实施方式的限定。对于所属领域的普通技术人员来说,在上述说明的基础上还可以做出其它不同形式的变化或变动。这里无法对所有的实施方式予以全部列出。凡是属于本发明的技术方案所引伸出的显而易见的变化或变动仍处于本发明的保护范围之列。
Claims (6)
1.一种杂原子掺杂碳点光催化降解工业废气,其特征在于,合成产生大量具有强氧化性自由基的杂原子掺杂碳点X-CDs,在光照射下,即可与工业废气中的还原性气体发生反应。
2.根据权利要求1所述的杂原子掺杂碳点光催化降解工业废气,其特征在于:所述杂原子掺杂碳点X-CDs的杂原子包括非金属元素N,S,F,O,P,Cl,Br,I,B;金属元素Fe,Cu,Al,Mn,Mo,Eu,Gd,Ru,Ti,Mg,Cr,Zn等中的一种或几种。
3.根据权利要求1所述的杂原子掺杂碳点光催化降解工业废气,其特征在于:所述杂原子掺杂碳点X-CDs的合成方法包括微波法,水热法,超声法以及热解法等。
4.根据权利要求1所述的杂原子掺杂碳点光催化降解工业废气,其特征在于:所述的具有强氧化性自由基包括·OH,O·-,1O2,·C或·N。
5.根据权利要求1所述的杂原子掺杂碳点光催化降解工业废气,其特征在于:所述的光为波长范围在250~800nm的紫外和可见光。
6.根据权利要求1所述的杂原子掺杂碳点光催化降解工业废气,其特征在于:所述还原性工业废气包括H2S,SO2,NH3,CO2,NO2,NO,CO,HCl,CS2等中的一种或几种。
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