CN106999847A - 改进的空气净化系统和用于除去甲醛的方法 - Google Patents
改进的空气净化系统和用于除去甲醛的方法 Download PDFInfo
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- CN106999847A CN106999847A CN201580048919.0A CN201580048919A CN106999847A CN 106999847 A CN106999847 A CN 106999847A CN 201580048919 A CN201580048919 A CN 201580048919A CN 106999847 A CN106999847 A CN 106999847A
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- oxide
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- aldehyde
- formaldehyde
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Classifications
-
- 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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/54—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/56—Platinum group metals
- B01J23/63—Platinum group metals with rare earths or actinides
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
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Abstract
本发明涉及使用可见光谱的光催化性组合物来分解包括挥发性化合物(VOCs)的污染物的方法。
Description
技术领域
本文公开内容一般而言涉及对空气中污染物的降低。更具体地,本文公开内容涉及使用改进的光催化性组合物来降低空气中的甲醛浓度的元件。
背景技术
光催化剂是降低空气中的甲醛等气体和其它污染物的浓度的有效手段。其是人们所期望的,因为甲醛气体被认为是室内空气综合征(sick-building syndrome)的要因。过去已经利用了多种手段来控制甲醛浓度,包括过滤器、氧化剂、热催化剂和光催化剂。
典型地,已从活性炭或沸石来制备过滤器,其通过物理捕获污染物以将其从空气中除去来发挥作用。采用过滤器的一个问题是随着它们的运转,过滤器必然将发生堵塞,丧失效力,并且必须被更换。
氧化物在其是耗材这点上也存在与过滤器类似的缺点;它们随着运转而消失,并且必须时常更换以保持其效力。
热催化剂在工业环境中用于甲醛的去除。此类催化剂的缺点在于为了有效运作而需要升温至远高于室温(20-25℃)的温度。这点限制了此类催化剂在通常的家庭环境中的实践应用。
上文述及的目前使用的技术的缺点表明人们需要更为有效的可见光谱的光催化剂。
发明内容
本文公开了使用可见光光催化剂、对CeO2和/或MnO2进行照射并且降低空气样品中的甲醛的方法。
一些实施方式包括除去和/或分解污染物(包括但不限于挥发性有机化合物和/或气体)的光催化元件,以及通过除去和/或分解空气中的污染物来净化空气的方法。这些实施方式包括光催化元件,所述光催化元件包含可见光光催化性的、且为吸附性的金属氧化物。在一些实施方式中,光催化元件包含可见光光催化性的、且为吸附性的金属氧化物;和发光元件,所述发光元件与样品和可见光光催化性的、且为吸附性的金属氧化物(例如铈氧化物或锰氧化物)以大约380nm至525nm的光具有光学联系。
所述实施方式包括下述元件,所述元件至少包含配置到基材上的可见光光催化性的、且为吸附性的材料,其用于当所述光催化元件被可见光谱照射且与污染物接触时、通过对污染物加以分解和/或氧化来有效降低空气中的污染物。就除去或分解挥发性有机化合物、无机化合物和/或气体水平(例如甲醛)而言,所述实施方式可以比以往使用的过滤器和组合物更为有效。
如本文中所述,在一些实施方式中,提供了用于除去或分解醛(例如甲醛)的方法。在其它一些实施方式中,所述方法可包括将样品与包含可见光光催化性的、且为吸附性的金属氧化物接触;以及将样品暴露给380nm至大约525nm之间的光。在一些实施方式中,光催化性的、且为吸附性的金属氧化物可选自铈氧化物和锰氧化物。在一些实施方式中,所述组合物包含催化性的、且为吸附性的金属氧化物,并且可以为至少70%的金属氧化物。
一些实施方式包括用于除去甲醛的方法,所述方法包括:将样品与包含下述可见光光催化剂的组合物接触;和将样品暴露给大约380nm至大约525nm之间的光,所述可见光光催化剂包含醛吸附性的金属氧化物,并且其中所述金属氧化物的金属具有23至80的原子序数。
一些实施方式包括用于从样品中除去甲醛的元件,所述元件包含:光催化元件和发光元件,所述光催化元件包含可见光光催化剂,所述可见光光催化剂包含醛吸附性的金属氧化物,其中所述金属氧化物的金属具有23至80的原子序数,其中所述发光元件与样品和铈氧化物以大约380nm至525nm的光具有光学联系。
一些实施方式包括用于从空气中除去醛的设备,所述设备包括与含有待除去的醛的空气以流体形式接触的光催化元件。
本文公开的实施方式中用于分解甲醛的元件可通过将光催化性组合物配置到基材上来形成。在一些实施方式中,光催化元件/组合物包含光催化剂,其中所述光催化剂可以是CeO2。光催化剂包括作为暴露给光(例如紫外光或可见光)的结果而可活化或改变化学反应速率的任何材料。
附图简述
图1是光催化涂层的一种实施方式的示意图。
图2是实施例1的光催化剂组合物的甲醛分解的图。
图3是包含CeO2的光催化剂组合物在18小时期间的CO2生成/甲醛分解情况的图。
图4是在暴露给包含CeO2的光催化剂组合物60分钟后的CO2生成/甲醛分解情况的图。
具体实施方式
光催化剂可与紫外或可见光照联用。一些光催化系统包括与金属氧化物组合的TiO2或WO3。不含UV的室内光照的增加导致对在可见光谱中有效的光催化剂的需求增加。
用于除去和/或分解醛的一些方法包括将样品与包含下述可见光光催化剂的组合物接触;以及将样品暴露给大约380nm至大约525nm、或大约447nm至大约457nm之间的光,所述可见光光催化剂包含具有醛吸附性的吸附性金属氧化物。在一些实施方式中,金属氧化物可以是铈氧化物和/或锰氧化物。在一些实施方式中,组合物可以是至少70%的金属氧化物。
在一些实施方式中,用于从样品中分解和/或除去醛(例如甲醛)的元件可包含光催化性的、且为吸附性的金属氧化物;和发光元件,所述发光元件与样品和金属氧化物具有光学联系,或者所述发光元件可发射出与样品和金属氧化物二者接触的光,所述发光元件发射出大约380nm至大约525nm之间的光、或大约447nm至大约457nm之间的光。
光催化剂包括作为暴露给光的结果而可活化或改变化学反应的任何材料。传统上,光催化剂仅可被UV范围中的光(即,具有低于约380nm的波长)活化。这是因为大多数半导体具有宽的能带间隙(>3eV)。然而,通过合适地选择材料或对既有光催化剂进行改良,已可合成了可见光光催化剂。可见光光催化剂包括被可见光(例如人的肉眼能够正常目视检测到的光,例如波长至少约380nm)活化的光催化剂。除了可见波长外,可见光光催化剂还可以被波长低于380nm的UV光活化。一些可见光光催化剂可具有对应于可见范围内的光的能带间隙,例如大于约1.5eV、小于约3.2eV、约1.5eV至约3.2eV、约1.7eV至约3.2eV、或者约1.77eV或约1.8eV至约3.2eV的能带间隙。
在一些实施方式中,光催化剂材料可以是吸收可见光的无机固体,例如固体无机半导体。与标准氢电极进行比较的情况下,此类光催化剂可具有约1eV至约0eV、约0eV至约-1eV、或约-1eV至约-2eV的能量导带。与标准氢电极进行比较的情况下,一些光催化剂可具有约3eV至约3.5eV、约2.5eV至约3eV、或者约2eV至约3.5eV、或者约3.5eV至约5.0eV的能量价带。
在一些实施方式中,可见光光催化剂可包含金属氧化物,例如原子序数为23-80、25-60、23-75、23-40、23、24、25、26、27、28、29、30、31、32、33、34、35、36、37、38、39、40、41、42、43、44、45、46、47、48、49、50、51、52、53、54、55、56、57、58、59、60、61、62、63、64、65、66、67、68、69、70、71、72、73、74、75、76、77、78、79、80或以这些数值为界的范围内的任何原子序数的金属的金属氧化物。在一些实施方式中,金属氧化物可以是ZnO、ZrO2、SnO2、CeO2、SrTiO3、BaTiO3、InO3、CuxO、Fe2O3、ZnS、Bi2O3、WO3、Bi2WO6、BiFeO3、MnyOx、TiO2、CoxO、V2O5或BiVO4。关于CuxO、MnyOx或CoxO,在一些实施方式中,x可以是1、2或3,以及,y可以是1、2或3。在一些实施方式中,金属氧化物可以是单独存在或与其它金属氧化物组合存在的稀土氧化物,例如铈氧化物(例如CeO2)。在一些实施方式中,金属氧化物可包含锰氧化物(例如MnO2)或由其组成。在一些实施方式中,第一光催化剂基本上不含TiO2和/或WO3。在一些实施方式中,光催化剂包含少于约40%、30%、25%、20%、10%、5%、2.5%或1%的TiO2和/或WO3。
在一些实施方式中,组合物还可包含非光催化性的金属氧化物。在一些实施方式中,组合物还包含贵金属,例如基于金属氧化物中金属原子总量而言的约0.01%至约10%、约0.2%至约5%、或约0.5%至约2%的贵金属。在一些实施方式中,贵金属可以是铂、钯、金、银、铱、钌和/或铑。在一些实施方式中,贵金属是铂。
在一些实施方式中,金属氧化物可以是对目标挥发性有机化合物具有吸附性的材料,例如CeO2和/或MnO2。例如,金属氧化物可吸收至少0.001mM、0.01mM、0.1mM、0.5mM、0.75mM或1.0mM的目标挥发性有机化合物。用于测定吸附量的合适方法可以是通过恒定体积可变压力分析来进行的。在另一方法中,可通过收集增加的CO2的量、并从甲醛量中减去CO2的量来测量消失的甲醛的量,从而提供对甲醛吸附量的估计。在一些实施方式中,相对每克可见光光催化性材料(例如CeO2)而言,光催化材料可吸附至少0.1mg、0.5mg、1.0mg、2.0mg和/或至少3.0mg的醛(例如甲醛)。在一种实施方式中,相对于每克CeO2而言,光催化性材料可吸附至少2.1mg的甲醛。在一种实施方式中,相对于每克CeO2而言,光催化性材料可吸附至少4.2mg的甲醛。在一些实施方式中,CeO2吸附甲醛使得甲醛向CO2和水的氧化/转化增加。
一些实施方式包括氧化物半导体,例如CeO2、MnO2及其变化形式。光催化剂可由本领域技术人员通过多种方法(包括固相反应、燃烧、溶剂热合成、火焰热解、等离子体合成、化学气相沉积、物理气相沉积、球磨和高能球磨(high energy grinding))来合成。在一些实施方式中,光催化剂可以是至少70%、75%、80%、85%、90%、95%、99%或100%的第一光催化剂。在一些实施方式中,光催化性组合物(composite)包含约1%至约99%的如前文所述的可见光光催化性材料,例如,CeO2和/或MnO2,以及相应地,约99%至约1%的非光催化性材料。在一些实施方式中,非光催化性材料可以是光催化活性为低于CeO2和/或MnO2活性的10%、5%、1%和/或0.5%的氧化物。在一些实施方式中,非光催化性材料可以是Al2O3。
在一些实施方式中,光催化剂还包含至少一种天然存在的元素,例如非惰性气体(non-noble gas)元素。在一些实施方式中,光催化剂材料可包括至少一种天然存在的元素(例如非惰性气体元素)或被至少一种天然存在的元素(例如非惰性气体元素)掺杂或负载。被掺杂的元素可作为通常在合成期间添加的前体而被提供。
在一些实施方式中,光催化剂还包含至少一种金属。在一些实施方式中,光催化剂可负载至少一种金属。光催化剂可通过合成后方法,例如,浸渍、光还原和溅射而负载金属。作为一种优选的实施方式,在光催化剂上负载金属可按照美国专利公开文本No.2008/0241542(其整体通过参考并入本文)中所述来进行。在一些实施方式中,光催化剂上负载的元素可以是贵重元素(noble element)。在一些实施方式中,负载到光催化剂上的元素可以是至少一种贵重元素、氧化物和/或氢氧化物。在一些实施方式中,贵重元素可以是铂、钯、金、银、铱、钌、铑或它们的氧化物和/或其氢氧化物。在一些实施方式中,负载到光催化剂上的元素可包含过渡金属,或其氧化物和/或氢氧化物。在一些实施方式中,负载到光催化剂上的元素可选自铁、铜、镍或它们的氧化物和/或其氢氧化物。在一些实施方式中,负载到光催化剂上的元素可选自不同的元素的组(包括至少一种过渡金属和至少一种贵金属或它们各自的氧化物和/或氢氧化物)。
用于分解醛(例如甲醛)的方法可包括将醛(例如甲醛)与包含金属氧化物的可见光光催化剂组合物接触。对一些材料而言,光催化性可能是在光催化剂表面上从电子-空穴对形成的反应性物种(能够进行还原和氧化)导致的,其中电子-空穴对是通过吸收电磁辐射而在光催化剂主体中产生的。
待被除去/分解的醛不受特别限制,其可包括例如甲醛(包括多聚甲醛)、乙醛(包括多聚乙醛)、丙醛、丁醛、戊醛、己醛、庚醛、2-乙基己醛、环己醛、糠醛、乙二醛、戊二醛、苯甲醛、2-甲基苯甲醛、3-甲基苯甲醛、4-甲基苯甲醛、对羟基苯甲醛、间羟基苯甲醛、苯乙醛和β-苯基丙醛。可将这些醛单独除去,或者还可联合除去两种或更多种。在一种实施方式中,可除去甲醛。
在一中实施方式中,对醛的除去/分解可包括对醛进行氧化,例如对甲醛进行氧化。在一些实施方式中,可将醛氧化,以形成二氧化碳和水。在一些实施方式中,醛可被基本上完全氧化为二氧化碳和水。在一些实施方式中,醛中至少70%、75%、80%、85%、90%、95%、97%或99%被转化为二氧化碳和水。
图1是根据本文所述的一些实施方式的光催化元件10的示意图。在一些实施方式中,光催化元件10可被提供为包括与醛8接触的光催化剂12。在一些实施方式中,如箭头16所示,可提供光源14以照射同时与醛8(例如甲醛)接触着的光催化剂12。在一些实施方式中,光催化元件10可被提供为包括基材(未示出)和光催化性组合物,所述组合物包括至少一种光催化剂材料12。在一些实施方式中,光催化剂组合物以使得光催化剂组合物可与光和待分解的物质(例如甲醛)接触的方式被涂布到基材上。
在一些实施方式中,源14可以是包括光致发光(磷光或荧光)材料、白炽材料、电致发光或化学发光或声致发光或机械发光或热发光材料中至少一种的透明光催化性组合物。磷光材料可包括ZnS和硅酸铝,而荧光材料可以包含磷光体,例如YAG-Ce(掺杂Ce的YAG)、Y2O3-Eu(掺杂Eu的氧化钇)、多种有机染料等。白炽材料可包含碳和钨,而电致发光材料可包括ZnS、InP、GaN等。很多类型的发光机理可用于提供能量以引发光催化,例如,太阳光、荧光灯、白炽灯、基于发光二极管(LED)的照明、钠蒸气灯、卤素灯、汞蒸气灯、惰性气体放电和火焰。在一些实施方式中,光源发出的以及与光催化性材料和/或醛(例如醛8)发生光学联系的光照可自大约380nm、大约390nm、大约400nm、大约410nm、大约420nm、或大约430nm起;以及直至大约475nm、大约495nm、大约525nm,或上述发射波长的任何组合。在一种实施方式中,光照可在大约447nm至大约457nm之间。
在一些实施方式中,光催化剂与醛的接触可在大约90℃、大约80℃、大约70℃、大约65℃、大约50℃、大约45℃、大约40℃、和/或大约35℃的最大值以下。
在一些实施方式中,光催化性组合物可被配置到基材上。在一些实施方式中,通过配置到基材上,光催化性组合物可以是在配置到基材上之前单独形成的层。在另一实施方式中,光催化性组合物可在基材表面上形成,例如通过气相沉积诸如化学气相沉积(CVD)或物理气相沉积(PVD);层压;挤压;轧制;浸泡;熔融;粘合;溶胶-凝胶沉积;旋涂;浸涂;棒式涂布;狭缝(slot)涂布;刷涂;溅射;热喷涂,包括火焰喷涂、等离子体喷涂(DC或RF);高速氧燃料喷涂(HVOF);原子层沉积(ALD);冷喷涂或气溶胶沉积来形成。在另一实施方式中,光催化性组合物可被掺入进基材的表面中,例如至少部分地嵌入到表面内。
在一些实施方式中,光催化剂组合物基本上覆盖基材。在一些实施方式中,光催化剂组合物接触或覆盖基材表面的至少约10%、至少约25%、至少约35%、至少约40%、至少约50%、至少约60%、至少约75%、至少约85%、或至少约95%。
更大的表面积可意味着更高的光催化活性。在一些实施方式中,光催化剂的Brunner Emmett Teller(BET)比表面积为约在0.1-500m2/g或10-50m2/g。
在一些实施方式中,提供光催化层,其包括上文所述的铈氧化物/锰氧化物的组合物。
在一些实施方式中,提供了制造光催化性组合物的方法,所述方法包括:制造包含光催化剂(例如CeO2)和分散介质的分散体系;其中所述分散体系具有大约2至大约50wt%的固体材料;将所述分散体系应用到基材上;以及,以足以将几乎所有分散介质从分散体系蒸发的温度和时间对分散体系和基材进行加热。在一些实施方式中,分散体系被应用以整体或部分覆盖基材,或者应用至基材表面上产生涂层或表面层。
在一些实施方式中,有制造光催化性组合物的下述方法,所述方法包括:混合CeO2的水性分散体系;添加足够的分散介质,例如水,以得到大约10至大约30wt%的固体材料的分散体系;将所述分散体系应用到基材上;以及,以足以将几乎所有水从分散体系蒸发的温度和时间对基材进行加热。在一些实施方式中,CeO2可以是溶胶。
在一些实施方式中,添加的分散介质(例如水)的量足以获得大约2至大约50wt%、大约10至大约30wt%、或大约15至大约25wt%固体材料的分散体系。在一些实施方式中,添加的分散介质(例如水)的量足以获得大约20wt%的固体材料的分散体系。
在一些实施方式中,以足以实质上除去分散介质的足够的温度和/或足够的时间对被混合物覆盖的基材进行加热。在一些实施方式中,分散介质中的至少大约90%、至少大约95%、或至少大约99%被除去。在一些实施方式中,以大约室温至500℃之间的温度对被分散体系覆盖的基材进行加热。在一些实施方式中,被分散体系覆盖的基材被加热至大约90℃和大约150℃之间的温度。在一些实施方式中,被分散体系覆盖的基材被加热至大约120℃的温度。在一些实施方式中,被分散体系覆盖的基材被加热至低于约200℃、低于约300℃、低于约400℃和/或低于约500℃的温度。尽管不希望受任何理论限制,但认为将温度保持在约500℃以下可以减少光催化材料热失活(例如由于光催化材料相变成较低活性的相、掺杂物扩散、掺杂物失活、负载的材料分解或凝结(总活性表面积降低)导致的)的可能性。
在一些实施方式中,被分散体系覆盖的基材被加热大约10秒至大约2小时的时间。在一些实施方式中,被混合物覆盖的基材被加热大约1小时的时间。
本文所述的分散体系可被应用至几乎任何基材。将分散体系应用至基材的其它方法可包括:将分散体狭缝涂/浸涂/旋涂、刷、轧制、浸泡、熔融、粘合或喷涂到基材上。可以使用适当的推进剂(propellant)来将分散体喷涂到基材上。
在一些实施方式中,基材不需要能够透光。例如基材可以是能够将分散体系直接应用于其上的常见工业或家用表面。基材可以包括玻璃(例如窗户)、墙(例如干式墙)、石材(例如花岗岩台面)、砖石(例如砖墙)、金属(例如不锈钢)、木材、塑料(例如用于花的塑料卷膜)、其他聚合物表面、陶瓷等。这些实施方式中的分散体系可以被配制为漆或液体粘合剂。这些实施方式中的分散体系可被应用至带(tape)、壁纸、帷帘(drape)、灯罩、灯盖、桌或台面覆盖物等上。
光催化剂组合物可能够光催化分解有机化合物(例如醛,包括乙醛、甲醛、丙醛等)。光催化性分解可以以固相、液相或气相发生。
在一些实施方式中,基材包括可透过气体的材料。在一些实施方式中,可透过气体的材料可以使得以最小阈值的流速通过基材。在另一实施方式中,气体可透过的材料可以是多孔PTFE(例如HEPA/ULPA过滤器)、无纺或纺织品、折叠型过滤器(例如织物、纸、多孔塑料例如多孔PTFE)、玻璃/石英毛、纤维(例如玻璃石英、塑料)、蜂巢结构的金属或陶瓷材料、或将光催化剂粘附到任何已有的过滤材料上。在一些实施方式中,可透过气体的材料是多孔的,和/或在其中和/或在贯通期间界定有孔。在一些实施方式中,可透过气体的材料可以是陶瓷。陶瓷可包含Al2O3、ZrO2、SiO2或其它已知的陶瓷材料。在一些实施方式中,陶瓷元件包含Al2O3。在一些实施方式中,陶瓷元件包含ZrO2。在一些实施方式中,陶瓷元件包含SiO2。在一些实施方式中,陶瓷包含本领域中已知的其它已知陶瓷材料。
陶瓷基材可具有每英寸约1孔(ppi)至大约50pp、大约5ppi至大约45ppi、大约10ppi至大约40ppi、大约15ppi至大约35ppi、大约20ppi至大约30ppi的范围内、大约30ppi、或上述范围的任何组合的多孔性。
陶瓷基材的厚度可在大约1mm至大约50mm之间,可为大约1mm厚至大约5mm厚;大约5mm厚至大约10mm厚;大约10mm厚至大约15mm厚;大约15mm厚至大约20mm厚;大约20mm厚至大约25mm厚;大约25mm厚至大约30mm厚;大约30mm厚至大约35mm厚;大约35mm厚至大约40mm厚;大约40mm厚至大约45mm厚、大约45mm厚至大约50mm厚;或以上述中的任何值为边界的范围内的厚度。
在一些实施方式中,当在光照下甲醛气体与光催化性组合物接触时,甲醛氧化元件的有效性提高。可选择多孔性和厚度的合适组合,以优化气流速度,从而实现期望水平的甲醛浓度。
在一些实施方式中,光催化性组合物通过浸涂而配置到多孔陶瓷基材上。在一些实施方式中,浸渍和干燥后,于大约400℃对元件退火大约12小时。退火提高组合物与陶瓷基材的粘附,并且增加元件的效能。退火工艺后,光催化性组合物形成穿过陶瓷基质配置的颗粒层。
在一些实施方式中,基材包含薄膜。此外,膜可以是(但不必须是)透明的。膜可以由低密度聚乙烯(LDPE)、高密度聚乙烯(HDPE)、聚丙烯(PP)、聚氯乙烯(PVC)、聚对苯二甲酸乙二醇酯(PET)、改性的聚对苯二甲酸乙二醇酯(PETG)、尼龙6、离聚物、由丙烯腈/丙烯酸甲酯共聚物改性的腈橡胶(nitrile rubber modified acrylonitrile-methyl acrylatecopolymer)或纤维素乙酸酯。
在一些实施方式中,薄膜具有大约10μm至大约250μm、大约10μm至大约30μm、大约30μm至大约50μm、大约50μm至大约70μm、大约70μm至大约90μm、大约90μm至大约110μm、大约110μm至大约130μm、大约130μm至大约150μm、大约150μm至大约170μm、大约170μm至大约190μm、大约190μm至大约210μm、大约210μm至大约230μm、大约230μm至大约250μm的厚度、或以上述中的任何值为边界的范围内的厚度。
光催化性组合物可通过本领域中已知的多种沉积方法配置在薄膜基材上,非限制性的例子包括浸渍、气相沉积、液相沉积等。
在一些实施方式中,基材包括玻璃。基材可以是硅酸盐或聚碳酸盐玻璃、或者典型地用于窗和显示器的其它玻璃。
在一些实施方式中,利用下述方法,其中,受污染的空气被暴露给光和光催化剂材料、组合物或分散体系(如上文所述),由此从空气中除去醛。
在一些实施方式中,光和光催化剂材料、组合物或分散体系可从空气中除去大约50%、大约60%、大约70%、大约80%、大约90%、大约95%、大约99%或更多的醛(包括甲醛)。
在一些实施方式中,光和光催化剂材料、组合物或分散体系可将大约50%、大约60%、大约70%、大约80%、大约90%、大约95%、大约99%或更多的醛(包括甲醛)转变为二氧化碳。
样品制备
除非另有指明,所有材料不经进一步纯化而使用。除非另有指明,所有材料均购自Sigma Aldrich(St.Louis,MO,USA)。
实施例1:样品制备
将粗制粉状CeO2(100mg)(Nanostructured&Amorphous Materials,Inc.,Houston,TX,USA)与去离子H2O(1至1.5mL)混合,制造分散体系。使用超声均质仪对得到的分散体系均质5分钟,然后涂布到使用电晕处理器与处理过的培养皿(直径60mm)的底上。将培养皿在加热板上于90-100℃加热,直到所有液体都蒸发。
通过同时从Xe灯(灯输出功率300W)进行光照以及在120℃热处理60分钟来清洁得到的培养皿。冷却至室温后,将培养皿密封于5L的袋中。
以与上文实施例1所述类似的方式准备另一个袋(甲醛对照和CO2对照),但在密封之前不向其中放入培养皿。
实施例2:光催化活性测量
向实施例1中记载的封有培养皿/未封有培养皿的袋中注入1.2L含有100ppm甲醛(HCHO)氮(N2)气和1.8L压缩空气(21%O2、78%N2、0.9%Ar),以制造初始甲醛(HCHO)浓度为每百万分之40±4份的3L气体混合物。在用外界蓝光照射各培养皿之前将袋在黑暗中放置大约30分钟。在黑暗期的开始和结束时以及在启动蓝光后的不同时间间隔对HCHO和二氧化碳(CO2)的浓度加以测量。使用检测管(No.91L),通过采样100mL气体来测定HCHO的浓度。使用CO2监控仪,通过采样10mL气体来测定CO2的浓度。通过定制蓝色LED阵列提供外界蓝光,其被设置为在培养皿的中心处提供25mW/cm2的光强。采样进行至18小时。18小时后,对袋进行冲洗,重新装入100ppm(HCHO)/1.8L的压缩空气(如上文所述),在与前述参数相同的参数下再次进行测量。结果示于图2和图3。图2和图3中显示了较之对照组中的甲醛和/或CO2水平而言甲醛随时间的降低的存在([实线]FA)以及CO2随时间的增加的存在([虚线]CO2)。
实施例3:甲醛的光催化转化
按照与上文所述的实施例1和2的记载相似的方式来制备实施例3并进行测试。其在图4中示为“CO2,在FA中,具有CeO2”。此外,以与实施例1和2中的记载相似的方式来进行实施例3的测试,但在两种情况下不向袋中装入甲醛(第1和第2对照轮)。这些在图4中示为“CO2,第一和第二对照轮”。与40ppm甲醛的情况相比较,CO2的量以慢得多的速率增加。该差异显然是来自甲醛向CO2的光催化分解。图4显示了向CeO2暴露60分钟后CO2的量增加,这被认为是来自光催化性的甲醛分解。这样的活性等于每小时每100mg CeO2大约2.1μmol甲醛。
实施例4:铂的负载(预示性)
铂的负载将通过浸透法来进行。Pt与CeO2的重量比将被设置为1比100。将硝酸四氨合铂(II)(Pt(NH3)4(NO3)2)(4.5mg)与去离子H2O(8mL)在管状反应器中混合,制造溶液。向溶液中加入粗制CeO2(0.2g)(Nanostructured&Amorphous Materials,Inc.,Houston,TX,USA)之后,在硅酮油浴中于90℃伴随剧烈搅拌将管状反应器加热1小时。然后向管状反应器中的反应混合物中加入含有NaOH(25mg)和葡萄糖(125mg)的水性溶液(2mL)。将反应混合物硅酮油浴中再保持1小时。冷却至室温后,将混合物滤经0.05μm的膜,用50至100mL去离子H2O洗,在空气炉中于110℃干燥过夜(16至18小时),最后在马弗炉中于400℃退火1小时。预计负载有Pt的CeO2也将展示出甲醛分解活性。
实施方案
涉及下述实施方案:
实施方案1.一种用于除去甲醛的方法,所述方法包括:
将样品与包含可见光光催化剂的组合物接触,所述可见光光催化剂包含醛吸附性的金属氧化物,并且,其中,所述金属氧化物的金属具有23至80的原子序数;和
将所述样品暴露给大约380nm至大约525nm的光。
实施方案2.实施方案1的方法,其中所述金属氧化物是ZnO、ZrO2、SnO2、CeO2、SrTiO3、BaTiO3、In2O3、CuxO、Fe2O3、ZnS、WO3、MnyOx、TiO2、CoxO或V2O5,其中x为1、2或3,并且y为1、2或3。
实施方案3.实施方案1的方法,其中所述金属氧化物是铈氧化物或锰氧化物。
实施方案4..实施方案1、2或3的方法,其中所述组合物还包含贵金属。
实施方案5.实施方案4的方法,其中所述贵金属是铂、钯、金、银、铱、钌或铑。
实施方案6.实施方案4的方法,其中所述贵金属是铂。
实施方案7.一种用于从样品中除去甲醛的元件,所述元件包含:
光催化元件,其包含可见光光催化剂,所述可见光光催化剂包含醛吸附性的金属氧化物,其中所述金属氧化物的金属具有23至80的原子序数;和
发光元件,其中所述发光元件与样品和铈氧化物以大约380nm至525nm的光具有光学联系。
实施方案8.实施方案7的元件,其中所述光催化性的、且为吸附性的金属氧化物是ZnO、ZrO2、SnO2、CeO2、SrTiO3、BaTiO3、In2O3、CuxO、Fe2O3、ZnS、WO3、MnyOx、TiO2、CoxO或V2O5,其中x为1、2或3,并且y为1、2或3。
实施方案9.实施方案7的元件,其中所述光催化性的、且为吸附性的金属氧化物是铈氧化物或锰氧化物。
实施方案10.实施方案7、8或9的元件,其中所述组合物还包含贵金属。
实施方案11.实施方案10的元件,其中所述贵金属是铂、钯、金、银、铱、钌或铑。
实施方案12.实施方案10的元件,其中所述贵金属是铂。
实施方案13.一种用于从空气中除去醛的设备,所述设备包含:实施方案7、8、9、10或11的元件;其中所述光催化元件与含有待除去的醛的空气以流体形式接触。
实施方案14.实施方案13的设备,其中还包含吸附到光催化元件上的醛。
除非另外指明,本说明书和权利要求书中使用的表示成分的量、性质(例如分子量、反应条件等等)的所有数字均应被理解为在全部情况下均被术语“约”修饰。因此,除非有相反的说明,否则本说明书和所附权利要求书中记载的数值参数均为近似值,其可能取决于想要获得的所期望的性质而有所变化。最起码,并且不试图限制将等同原则应用于权利要求的范围,每个数值参数至少应根据报道的有效数字并应用普通四舍五入法来理解。
除非本文另有指明或与上下文明显矛盾,否则描述本发明的范畴中(尤其在权利要求书的范畴中)使用的术语“一个”、“一种”(“a”、“an”)、“所述”(“the”)以及类似记载应当被理解为既包括单数又包括复数。除非本文另有指明或与上下文明显矛盾,本文中所描述的所有方法可以以任意合适的顺序进行。本文中所提供的任何实施例和所有实施例或示例性的语言(例如“例如”)的使用仅用于更好地阐述本发明,而不对任何权利要求的范围加以限制。说明书中的任何语言均不应被解释为表示任何未在权利要求中限定的要素是本发明的实施所必需的。
本文公开的替换性要素或实施方案的分组不应被理解为限制。每个组成员可被个别地、或以与该组其它成员或本文中记载的其它要素的任何组合而被提及并被要求保护。应理解,为了方便和/或可专利性的理由,组中的一个或多个成员可被包括进一组或从中删除。当任何此类包括或删除发生时,说明书被视为已记载了修改后的组,并因此满足对所附权利要求书中所采用的全部马库什式组的书面记载的要求。
本文中描述了某些实施方案,包括本申请的发明人已知的用于实施本发明的最佳方式。当然,在阅读前述说明书之后,对这些已被描述的实施方案的改变对于本领域普通技术人员来说将是明显的。本申请的发明人预期本领域技术人员能以合适的方式利用此类改变,本申请的发明人预期本发明可以以除了本文中具体描述的方式之外的方式来实现。因此,权利要求在适用的法律允许的范畴内包含权利要求中记载的主题的所有变化形式和等同形式。此外,除非本文另有指明或与上下文明显矛盾,上文描述的要素以其所有可能变化而得到的任何组合均被包括进本发明。
最后,应当理解,本文中公开的实施方案仅为阐述权利要求的宗旨。可以采用的其它变化形式也落在权利要求的范围内。因此,举例而言(但并非限制),可按照本文中的教导来利用各种替代性实施方案。因此,权利要求并不被狭隘地限制为前文中示出的实施方案。
Claims (14)
1.一种用于除去甲醛的方法,所述方法包括:
将样品与包含可见光光催化剂的组合物接触,所述可见光光催化剂包含醛吸附性的金属氧化物,并且,其中,所述金属氧化物的金属具有23至80的原子序数;和
将所述样品暴露给大约380nm至大约525nm的光。
2.权利要求1的方法,其中所述金属氧化物是ZnO、ZrO2、SnO2、CeO2、SrTiO3、BaTiO3、In2O3、CuxO、Fe2O3、ZnS、WO3、MnyOx、TiO2、CoxO或V2O5,其中x为1、2或3,并且y为1、2或3。
3.权利要求1的方法,其中所述金属氧化物是铈氧化物或锰氧化物。
4.权利要求1、2或3的方法,其中所述组合物还包含贵金属。
5.权利要求4的方法,其中所述贵金属是铂、钯、金、银、铱、钌或铑。
6.权利要求4的方法,其中所述贵金属是铂。
7.一种用于从样品中除去甲醛的元件,所述元件包含:
光催化元件,其包含可见光光催化剂,所述可见光光催化剂包含醛吸附性的金属氧化物,其中所述金属氧化物的金属具有23至80的原子序数;和
发光元件,其中所述发光元件与样品和铈氧化物以大约380nm至525nm的光具有光学联系。
8.权利要求7的元件,其中所述光催化性的、且为吸附性的金属氧化物是ZnO、ZrO2、SnO2、CeO2、SrTiO3、BaTiO3、In2O3、CuxO、Fe2O3、ZnS、WO3、MnyOx、TiO2、CoxO或V2O5,其中x为1、2或3,并且y为1、2或3。
9.权利要求7的元件,其中所述光催化性的、且为吸附性的金属氧化物是铈氧化物或锰氧化物。
10.权利要求7、8或9的元件,其中所述组合物还包含贵金属。
11.权利要求10的元件,其中所述贵金属是铂、钯、金、银、铱、钌或铑。
12.权利要求10的元件,其中所述贵金属是铂。
13.一种用于从空气中除去醛的设备,所述设备包含:权利要求7、8、9、10或11的元件;其中所述光催化元件与含有待除去的醛的空气以流体形式接触。
14.权利要求13的设备,其中还包含吸附到光催化元件上的醛。
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