CN113663689B - 一种用于净化空气中甲醛污染物的光热催化炭材料 - Google Patents
一种用于净化空气中甲醛污染物的光热催化炭材料 Download PDFInfo
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- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 title claims abstract description 69
- 230000003197 catalytic effect Effects 0.000 title claims abstract description 33
- 239000003575 carbonaceous material Substances 0.000 title claims abstract description 20
- 239000003344 environmental pollutant Substances 0.000 title claims abstract description 14
- 231100000719 pollutant Toxicity 0.000 title claims abstract description 13
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 33
- 239000003054 catalyst Substances 0.000 claims abstract description 23
- 238000002360 preparation method Methods 0.000 claims abstract description 18
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 12
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- 239000004372 Polyvinyl alcohol Substances 0.000 claims description 15
- 229920002451 polyvinyl alcohol Polymers 0.000 claims description 15
- 238000003756 stirring Methods 0.000 claims description 12
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 12
- NTHWMYGWWRZVTN-UHFFFAOYSA-N sodium silicate Chemical compound [Na+].[Na+].[O-][Si]([O-])=O NTHWMYGWWRZVTN-UHFFFAOYSA-N 0.000 claims description 11
- 229910010413 TiO 2 Inorganic materials 0.000 claims description 10
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 10
- 239000010949 copper Substances 0.000 claims description 10
- 238000001354 calcination Methods 0.000 claims description 9
- QPLDLSVMHZLSFG-UHFFFAOYSA-N Copper oxide Chemical group [Cu]=O QPLDLSVMHZLSFG-UHFFFAOYSA-N 0.000 claims description 8
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims description 8
- 239000004115 Sodium Silicate Substances 0.000 claims description 8
- 239000000047 product Substances 0.000 claims description 8
- 229910052911 sodium silicate Inorganic materials 0.000 claims description 8
- 239000007864 aqueous solution Substances 0.000 claims description 7
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- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 4
- 239000005751 Copper oxide Substances 0.000 claims description 4
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 4
- 239000012298 atmosphere Substances 0.000 claims description 4
- 229910052802 copper Inorganic materials 0.000 claims description 4
- 229910000431 copper oxide Inorganic materials 0.000 claims description 4
- 238000004898 kneading Methods 0.000 claims description 4
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- NDVLTYZPCACLMA-UHFFFAOYSA-N silver oxide Substances [O-2].[Ag+].[Ag+] NDVLTYZPCACLMA-UHFFFAOYSA-N 0.000 claims description 4
- 239000004408 titanium dioxide Substances 0.000 claims description 4
- 239000003638 chemical reducing agent Substances 0.000 claims description 2
- 229910000365 copper sulfate Inorganic materials 0.000 claims description 2
- ARUVKPQLZAKDPS-UHFFFAOYSA-L copper(II) sulfate Chemical compound [Cu+2].[O-][S+2]([O-])([O-])[O-] ARUVKPQLZAKDPS-UHFFFAOYSA-L 0.000 claims description 2
- 238000001035 drying Methods 0.000 claims description 2
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- CQLFBEKRDQMJLZ-UHFFFAOYSA-M silver acetate Chemical compound [Ag+].CC([O-])=O CQLFBEKRDQMJLZ-UHFFFAOYSA-M 0.000 claims description 2
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- 239000012279 sodium borohydride Substances 0.000 claims description 2
- 229910000033 sodium borohydride Inorganic materials 0.000 claims description 2
- 239000001509 sodium citrate Substances 0.000 claims description 2
- NLJMYIDDQXHKNR-UHFFFAOYSA-K sodium citrate Chemical compound O.O.[Na+].[Na+].[Na+].[O-]C(=O)CC(O)(CC([O-])=O)C([O-])=O NLJMYIDDQXHKNR-UHFFFAOYSA-K 0.000 claims description 2
- JBJWASZNUJCEKT-UHFFFAOYSA-M sodium;hydroxide;hydrate Chemical compound O.[OH-].[Na+] JBJWASZNUJCEKT-UHFFFAOYSA-M 0.000 claims description 2
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- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims 1
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- 229910052797 bismuth Inorganic materials 0.000 description 9
- JCXGWMGPZLAOME-UHFFFAOYSA-N bismuth atom Chemical compound [Bi] JCXGWMGPZLAOME-UHFFFAOYSA-N 0.000 description 9
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- 229910002115 bismuth titanate Inorganic materials 0.000 description 5
- QGLKJKCYBOYXKC-UHFFFAOYSA-N nonaoxidotritungsten Chemical compound O=[W]1(=O)O[W](=O)(=O)O[W](=O)(=O)O1 QGLKJKCYBOYXKC-UHFFFAOYSA-N 0.000 description 5
- 229910001930 tungsten oxide Inorganic materials 0.000 description 5
- 229910052688 Gadolinium Inorganic materials 0.000 description 4
- ZCDOYSPFYFSLEW-UHFFFAOYSA-N chromate(2-) Chemical compound [O-][Cr]([O-])(=O)=O ZCDOYSPFYFSLEW-UHFFFAOYSA-N 0.000 description 4
- UIWYJDYFSGRHKR-UHFFFAOYSA-N gadolinium atom Chemical compound [Gd] UIWYJDYFSGRHKR-UHFFFAOYSA-N 0.000 description 4
- LSGOVYNHVSXFFJ-UHFFFAOYSA-N vanadate(3-) Chemical compound [O-][V]([O-])([O-])=O LSGOVYNHVSXFFJ-UHFFFAOYSA-N 0.000 description 4
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- OFNHMKFJXLGYNW-UHFFFAOYSA-N dioxido(dioxo)chromium gadolinium(3+) Chemical compound [Cr](=O)(=O)([O-])[O-].[Gd+3].[Cr](=O)(=O)([O-])[O-].[Cr](=O)(=O)([O-])[O-].[Gd+3] OFNHMKFJXLGYNW-UHFFFAOYSA-N 0.000 description 3
- 239000012299 nitrogen atmosphere Substances 0.000 description 3
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- FJOLTQXXWSRAIX-UHFFFAOYSA-K silver phosphate Chemical compound [Ag+].[Ag+].[Ag+].[O-]P([O-])([O-])=O FJOLTQXXWSRAIX-UHFFFAOYSA-K 0.000 description 3
- 229940019931 silver phosphate Drugs 0.000 description 3
- 229910000161 silver phosphate Inorganic materials 0.000 description 3
- 239000010936 titanium Substances 0.000 description 3
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- ADZWSOLPGZMUMY-UHFFFAOYSA-M silver bromide Chemical compound [Ag]Br ADZWSOLPGZMUMY-UHFFFAOYSA-M 0.000 description 1
- 229910052712 strontium Inorganic materials 0.000 description 1
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 description 1
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Abstract
本发明公开了一种用于净化空气中甲醛的光热催化炭材料，由具有光热协同催化功能的催化剂和活性炭载体组成。该光热催化炭材料将活性炭的吸附净化性能与催化剂的光热催化净化性能相结合，实现吸附与光热催化协同高效净化甲醛气体污染物。该光热催化炭材料制备工艺简单、成本较低、适合宏量制备和推广应用于室内空气净化相关领域。
Description
技术领域
本发明属于大气污染治理技术领域，具体涉及一种用于净化空气中甲醛污染物的光热催化炭材料的制备及其应用。
背景技术
室内装修、家具、装饰品等所释放的以甲醛为代表的挥发性有机化合物（VOCs）是重要的室内环境污染物，危害人体健康。如何有效净化VOCs既是全社会关心的民生问题，也是环境污染治理领域的重点研究内容。基于活性炭的吸附技术是目前应用最为广泛的室内VOCs净化技术，常用于净化大风量、低浓度的有机废气。然而活性炭对VOCs的吸附量受温度与湿度的影响，且在高温下易脱附造成二次污染。
光热协同催化氧化技术是一种能在相对温和条件下将VOCs催化转化成CO2、H2O等无毒气体的新型催化净化技术。例如，溴化银/银/钛酸锶- TiO2纳米管阵列(TiNT)（ZL201810417799.2）、钛酸铋/铋/钒酸铋（CN110368924A）、铬酸钆/银/磷酸银（CN110237853A）、氧化钨/铋/铬酸钆（CN111659392A）等光热催化材料都被报道有较好的光热协同净化VOCs的性能。然而，光热催化剂催化净化VOCs效率不仅受其本征活性影响，还受污染物气体的传质影响。因此，在净化低浓度的室内甲醛等VOCs时，单一光热催化技术的使用仍难以满足实际工况需求。
发明内容
针对上述室内空气低浓度甲醛净化技术所面临的难题，本发明公开了一种将吸附技术与光热协同催化技术相耦合的技术和用于净化空气中甲醛污染物的光热催化炭材料，通过两种技术的优势互补和协同作用，实现甲醛气体污染物的高效净化。
为了实现上述发明目的，本发明采用的技术方案如下：
一种用于净化空气中甲醛污染物的光热催化炭材料，由具有光热协同催化功能的催化剂和活性炭载体组成，其中，催化剂与活性炭的质量比为0.01~0.2。
上述的光热催化炭材料组成中的催化剂为氧化铜/银/二氧化钛、钛酸铋/铋/钒酸铋、铬酸钆/银/磷酸银、氧化钨/银/铬酸钆等具有光热协同催化功能的催化剂。
上述的光热催化炭材料由以下步骤制备而成：
(1) 按比例将催化剂与活性炭粉末混合均匀,加入胶黏剂后搅拌捏合;
(2) 挤条成型、风干后，在惰性气氛中煅烧制得光热催化炭材料。
上述的制备方法中的催化剂的制备方法为已有技术或采用经典的沉积沉淀法制得，所属领域的技术人员可以根据现有技术中所公开的各种制备方法得到上述光热催化剂，示例性方法包括但不限于专利中介绍的方法，例如，钛酸铋/铋/钒酸铋（CN110368924A）、铬酸钆/银/磷酸银（CN110237853A）、氧化钨/铋/铬酸钆（CN111659392A），这些专利引入本发明作为参考。
上述的制备方法中的胶黏剂由聚乙烯醇树脂（PVA）和硅酸钠以质量比1~10，在pH为3~7和温度为60~100oC的水溶液条件下混合调制而成。
上述的制备方法中胶黏剂与活性炭质量比例为0.5~2，煅烧温度为100~400℃，煅烧时间1 ~12 h。
上述的光热催化炭在去除室内空气中甲醛气体污染物中的应用。
与现有技术相比，本发明具有如下有益效果:
除室内甲醛气体污染物效率高，适用温度、湿度和甲醛浓度范围广，适用于车内、家居和工厂车间等室内甲醛的净化；易于再生和循环利用，在加热和光照等条件下均可实现吸附污染物的脱除和催化炭的再生，并可有效避免污染物的转移；制备工艺简单、成本较低、适合宏量制备和推广应用。
附图说明
图1是实施例1制备的催化炭材料的示意图。
具体实施方式
本发明的实施方法灵活可变，不仅仅限于此例所述的具体操作方式，为更好地说明本发明，便于理解本发明的技术方案，下面结合具体的实施例对本发明作进一步详细的叙述。
实施例1
光热催化剂氧化铜/银/二氧化钛（或CuOx/Ag/TiO2）的制备：取0.5 g锐钛矿型TiO2粉末超声分散于去离子水中，在剧烈搅拌下，按目标产物中银的负载量为1 wt.%计，逐滴加入适量的醋酸银的水溶液，然后按还原剂的添加量与Ag的摩尔比为20的量，加入硼氢化钠水溶液，继续搅拌，离心分离后分别用去离子水和无水乙醇多次洗涤固体产物，80 °C烘箱中干燥后得到固体产物Ag/TiO2。将Ag/TiO2粉末与按目标产物中Cu的负载量为3wt.%计所需将一定量的硫酸铜加入到60 mL 的0.2 mol/L 的NaOH水溶中，搅拌0.5 h，然后按目标产物里铜的氧化物中Cu+/Cu2+的摩尔比例为~0.5的需求逐滴加入一定量的0.1 mol/L 柠檬酸钠水溶液调控铜元素价态。搅拌0.5 h后，离心分离收集产物，并分别用去离子水和无水乙醇洗涤固体产物，在100 °C的N2的氛围下干燥，得到光热催化材料CuOx/Ag/TiO2。
胶黏剂的制备：将聚乙烯醇树脂（PVA）先溶于热水中，然后按PVA与硅酸钠的质量比为2的比例加入饱和硅酸钠溶液，调节pH到5，然后在90 ℃恒温水浴锅中反应2 h后，冷却至室温制取胶黏剂。
光热催化炭的制备：按CuOx/Ag/TiO2催化剂与活性炭的质量比为0.1的比例加入催化剂和活性炭，并混合均匀，然后按胶黏剂与活性炭质量比例为1的量加入PVA/硅酸钠复合胶黏剂，搅拌捏合、利用挤条机挤出成型、风干后，在氮气气氛和200 ℃下煅烧1 h后得到催化炭材料，如图1所示。
实施例2
光热催化剂钛酸铋/铋/钒酸铋（或Bi4Ti3O12/Bi/BiVO4）的制备：参照专利CN110368924A中介绍的方法合成Bi4Ti3O12/Bi/BiVO4，以催化剂的重量为100 %，单质铋的质量分数为4.4 %，钛酸铋的质量分数为5.6 %。
胶黏剂的制备：将聚乙烯醇树脂（PVA）先溶于热水中，然后按PVA与硅酸钠的质量比为5的比例加入饱和硅酸钠溶液，调节pH到6，然后在100 ℃恒温水浴锅中反应2 h后，冷却至室温制取胶黏剂。
光热催化炭的制备：按Bi4Ti3O12/Bi/BiVO4催化剂与活性炭的质量比为0.05的比例加入催化剂和活性炭，并混合均匀，然后按胶黏剂与活性炭质量比例为1.5的量加入PVA/硅酸钠复合胶黏剂，搅拌捏合、利用挤条机挤出成型、风干后，在氮气气氛和300 ℃下煅烧6 h后得到催化炭材料。
实施例3
光热催化剂氧化钨/铋/铬酸钆（或WO3/Bi/GdCrO3）的制备：参照专利CN111659392A中介绍的方法合成WO3/Bi/GdCrO3，以催化剂的重量为100 %，单质铋的质量分数为4.6 %，氧化钨的质量分数为47.7 %。
胶黏剂的制备：将聚乙烯醇树脂（PVA）先溶于热水中，然后按PVA与硅酸钠的质量比为8的比例加入饱和硅酸钠溶液，调节pH到4，然后在80 ℃恒温水浴锅中反应2 h后，冷却至室温制取胶黏剂。
光热催化炭的制备：按WO3/Bi/GdCrO3催化剂与活性炭的质量比为0.15的比例加入催化剂和活性炭，并混合均匀，然后按胶黏剂与活性炭质量比例为0.8的量加入PVA/硅酸钠复合胶黏剂，搅拌捏合、利用挤条机挤出成型、风干后，在氮气气氛和400 ℃下煅烧1 h后得到催化炭材料。
分别取上述催化炭材料或参比样品活性炭材料0.05g进行不同条件下甲醛净化性能的测试。采用动态实验方法，将材料压片、破碎和过筛后（60~80目），装入内径为5mm的固定床中，以干燥空气作为载气，总进气流量为90mL/min，进气甲醛浓度为~10mg/m3，通过测量不同床层条件下，如室温、加热或光照，床层出口甲醛浓度随时间的变化曲线（或称作甲醛穿透曲线），计算各样品在不同条件下的甲醛平衡净化量，结果如表1所示。
表1各材料净化甲醛性能对比
Claims (4)
1.一种用于净化空气中甲醛污染物的光热催化炭材料，其特征在于，该光热催化炭材料由具有光热协同催化功能的催化剂和活性炭载体组成，其中，催化剂与活性炭的质量比为0.01～0.2；
催化剂为氧化铜/银/二氧化钛；
光热催化剂氧化铜/银/二氧化钛的制备方法为：
取0.5g锐钛矿型TiO2粉末超声分散于去离子水中，在剧烈搅拌下，按目标产物中银的负载量为1wt.％计，逐滴加入适量的醋酸银的水溶液，然后按还原剂的添加量与Ag的摩尔比为20的量，加入硼氢化钠水溶液，继续搅拌，离心分离后分别用去离子水和无水乙醇多次洗涤固体产物，80℃烘箱中干燥后得到固体产物Ag/TiO2；
将Ag/TiO2粉末与按目标产物中Cu的负载量为3wt.％计所需将硫酸铜加入到60mL的0.2mol/L的NaOH水溶中，搅拌0.5h，然后按目标产物里铜的氧化物中Cu+/Cu2+的摩尔比例为0.5的需求逐滴加入0.1mol/L柠檬酸钠水溶液调控铜元素价态，搅拌0.5h后，离心分离收集产物，并分别用去离子水和无水乙醇洗涤固体产物，在100℃的N2的氛围下干燥，得到光热催化材料CuOx/Ag/TiO2。
2.如权利要求1所述的光热催化炭材料，其特征在于，所述的光热催化炭材料由以下步骤制备而成：
(1)按比例将催化剂与活性炭粉末混合均匀,加入胶黏剂后搅拌捏合；
(2)挤条成型、风干后，在惰性气氛中煅烧制得光热催化炭材料。
3.如权利要求2所述的光热催化炭材料，其特征在于，所述胶黏剂由聚乙烯醇树脂和硅酸钠以质量比1～10，在pH为3～7和温度为60～100℃的水溶液条件下混合调制而成；所述胶黏剂与活性炭质量比例为0.5～2；成型后的煅烧温度为100～400℃，煅烧时间1～12h。
4.权利要求1-3任一项所述的光热催化炭材料在去除空气中甲醛污染物的应用。
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