CN106946312A - 利用光催化水泥基材料降解饮用水消毒副产物三氯乙酰胺的方法 - Google Patents
利用光催化水泥基材料降解饮用水消毒副产物三氯乙酰胺的方法 Download PDFInfo
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- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
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Abstract
利用光催化水泥基材料降解饮用水消毒副产物三氯乙酰胺的方法,属于建筑材料和水处理技术领域。以钛酸四丁酯为前驱体,通过溶胶‑凝胶法制备二氧化钛溶胶,通过浸润法制备二氧化钛/沸石光催化剂;将二氧化钛/沸石复合物均匀撒布于水泥材料上制成光催化水泥基材料,获得二氧化钛/沸石光催化水泥基材料。配置三氯乙酰胺浓度5000μg/L溶液,搅拌,向其中加入光催化水泥材料;通过紫外光辐照,处理时间为0‑4小时,实现对水中消毒副产物三氯乙酰胺100%的去除。本发明的光催化水泥基材料及水中消毒副产物的降解方法实现了对水中以三氯乙酰胺为代表的氮类消毒副产物的高效,安全去除。
Description
技术领域
本发明属于建筑材料领域和水处理技术领域,更具体的说,涉及一种利用二氧化钛/沸石复合光催化水泥基材料光降解水中消毒副产物三氯乙酰胺的方法。
背景技术
随着水源污染越来严重,饮用水的安全卫生问题也越显重要。江河湖泊等水源容易受到生活、工业废水的污染,饮用水在给水管网中也易受到管中各种的污染,其中,致病微生物可以通过饮用水引起介水传染病。为了减少介水性流行病的传播,一般要消毒杀菌,即采取物理或化学等方法杀死水中的致病微生物,使饮用水的安全卫生满足健康的需求。
目前,我国大部分城市的水厂采用液氯对饮用水进行消毒。但是,液氯在杀灭水中的细菌和病毒的同时,会与一些天然有机物(NOM)或者无机物发生化学反应,生成一些具有“三致”(致癌、致畸、致突变)作用的含碳消毒副产物(Carbon-disinfection by-products,简写为C-DBPs)。为了满足饮用水安全卫生需求,减少消毒后水中C-DBPs的浓度,大多数净水厂将消毒方式转换为以氯胺或者臭氧的消毒方式。然而,消毒方式的改变导致新型的高风险含氮消毒副产物(N-DBPs)在饮用水中频繁检出,N-DBPs所可能引发的潜在健康风险
远远大于C-DBPs。国外学者最先发现N-DBPs,他们对N-DBPs的毒理学、生成过程和控制方法等有一定研究。国内学者关于氮类消毒副产物的生成规律研究较多,其它各个方面研究都较少,而关于对于饮用水中N-DBPs的去除,特别是胺类N-DBPs的去除的研究报道很少。因此,研究饮用水中N-DBPs,特别是胺类N-DBPs的去除,对于保障饮用水的安全可靠和人类的健康具有重要意义。三氯乙酰胺属于一种典型的氮类消毒副产物。
目前主要从三个方面对消毒副产物进行控制:源头控制,过程控制和终端控制。国内外学者对于过程控制研究较多,而对于源头和终端控制研究较少。
1源头控制
源头控制主要是指控制DBPs的前体物,前体物大多为源水中有机物质、腐殖酸和一些小分子有机物等。由于环境的污染,水体受到不同程度的污染,大多数源水中有机物质的含量增加,从而使饮用水中DBPs的含量也增加了。因此,进行源头控制减少源水中的有机物是降低DBPs含量的一种重要方法。源头控制法主要包括强化混凝技术,生物预处理技术,膜技术和吸附法等。
2过程控制
消毒副产物是消毒剂(主要是氯离子、溴离子等)和有机物进行加成、取代反应等从而产生的,过程控制就是指通过改变消毒剂、改变消毒剂的投加方式等,从而改变消毒副产物的生成过程中消毒剂的含量和种类,达到降低饮用水中DBPs的含量。过程控制包括消毒剂的改变和改进消毒工艺。
3终端控制
终端控制是指去除已产生的消毒副产物。终端控制主要包括膜分离技术,曝气法和吸附法等。
目前,国内外学者对于N-DBPs的细胞和遗传毒性研究较多[1],对于通过改变消毒剂或消毒方式,探讨各种N-DBPs的生成潜能的报道也比较多[2],而关于如何去除已生成的N-DBPs研究在国内很少见报道。
[1]杨帆,楚文海,张永吉等.饮用水有机类消毒副产物毒理学研究方法进展[J].生态毒理学报,2012,07(1):35-43.
[2]陈忠林,范洁,杨荣华等.饮用水加氯消毒副产物及其控制技术的发展[J].哈尔滨建筑大学学报,2000(6):35-39.
发明内容
1.发明要解决的技术问题
本发明针对目前国内饮用水中消毒副产物三氯乙酰胺控制方法缺乏的技术现状,提出了一种光催化水泥基材料及水中消毒副产物三氯乙酰胺的去除方法。本发明提供的技术方法方案安全、高效、可靠、方便,可用于饮用水处理,从而保障水质安全。
本发明技术方案表征为:
一种光催化水泥基材料,它由以下两种组分按照一定质量复合而成:
A组分(基材料):直径为14cm,高为1cm的水泥浆圆片,水灰比(水泥与水的质量比)控制在0.35-0.4,水泥质量为22g,水质量为7.7g-8.8g;
B组分(光催化剂):1gTiO2/沸石复合材料;其中,B组分由以下2种组分按照一定的质量百分比复合而成:
(1)沸石;
(2)TiO2:占沸石质量比40%;
通过溶胶凝胶法制备TiO2溶胶,通过浸润法制备TiO2/沸石光催化剂,将TiO2/沸石光催化剂均匀洒布于水泥基材料上制备光催化水泥基材料。
制备光催化水泥基材料的方法,其特征在于,具体步骤为:以钛酸四丁酯(Ti(OC4H9)4)为前驱体,将其和乙醇按体积比V(Ti(OC4H9)4):V(C2H5OH)=1:3混合,搅拌10min,用硝酸调节溶液的pH值至4,搅拌3~4h,得到透明略带浅黄色的溶胶;接着分别按TiO2占沸石质量分数比30%、35%、40%、45%的比例将沸石加入TiO2溶胶中,缓慢滴加去离子水使溶胶水解得到灰白色凝胶,将凝胶在100℃下干燥至恒重后研磨;最后将研磨好的粉末在不同的温度(200℃、300℃、400℃、500℃)下锻烧4h,研磨即得到浅黄色粉末。
上述制备获得的光催化水泥基材料应用于水中消毒副产物三氯乙酰胺的光降解方法,其步骤为:
(1)配置三氯乙酰胺浓度为5000μg/L的的溶液1L,加入一片上述步骤中制备的光催化水泥圆片;
(2)通过紫外辐照,处理时间为0-20h,实现水中三氯乙酰胺的100%的去除。
本发明机理:理论上,光催化反应在TiO2表面经由以下几步实现即:(a)用光能大于TiO2带隙的光辐照TiO2产生电子-空位对;(b)TiO2表面捕获被吸附的三氯乙酰胺,使光生电子、空位分离;(c)在电子空位分别与水反应生成强氧化性的羟基自由基和超氧离子,这两种强氧化性物质与表面被吸附的三氯乙酰胺中进行氧化还原反应,使三氯乙酰胺分解成无毒的H2O和CO2;(d)产物的解吸和表面的重构。锐钛矿型TiO2虽然具有优良的光催化活性,但是这种晶型的TiO2的吸附能力不好,特别是对非极性分子,这限制了它的进一步应用。而沸石由于其多孔结正好具有良好的吸附性能。如两者结合起来,从而产生协同效应,能很好地提高Ti02的光催化性能。插入沸石孔洞内和负载在沸石表面上的TiO2粒子在紫光的照射下产生空穴-电子对,因为沸石孔洞内具有很强的电场强度,其表面也有电子富集,可以起到抑制电子-空穴复合的作用,从而使得沸石吸附的有机物可以很容易的获得紫外光激发TiO2而与水和氧生成的活性基团,从而提高沸石负载TiO2光催化剂的光催化活性。将TiO2-沸石复合物均匀洒布在水泥基材料表面,通过水泥浆的粘性使其粘附于水泥基材料表面,并且均匀洒布于表面可以使TiO2-沸石复合物具有更大的光接触面,有利于光催化反应的发生。
2.有益效果
采用本发明提供的技术方案,与已有的技术对比,具有如下显著效果:
(1)本发明提供了一种光催化水泥基材料,该材料由二氧化钛/沸石复合光催化剂与水泥圆片组成,在紫外光辐照下受激发后,通过光催化机理,可以高效的产生高活性、强氧化性的羟基自由基和超氧离子。这些强氧化物质可以与三氯乙酰胺发生氧化还原反应使其变成无毒性的H2O和CO2,实现对其的降解与脱毒,在过程中无毒性副产物生成,安全可靠;且此种光催化水泥基材料的结合。光敏药剂本身不含毒性物质,不引起二次污染,因此该方法高效、安全、可靠;
(2)本发明的一种水中消毒副产物三氯乙酰胺的去除方法,可以实现消毒副产物的高效去除;与现有的处理方法相比,该光催化水泥基材料可以通过调节药剂配方比例,灵活地控制产生对消毒副产物具有特殊选择性和反应活性的特定活性物种,从而灵活而又有选择性地实现了对消毒副产物三氯乙酰胺全部完全高效的降解和脱毒,可以实现对消毒副产物三氯乙酰胺的安全脱毒,且过程中无毒性副产物生成,安全可靠;另外,该光催化复合材料与水泥基材料结合,不会在水体中造成明显残留,无需后续处理,操作方便,运行经济。
附图说明
图1是实施例1中光催化水泥基材料在紫外光辐照下降解三氯乙酰胺浓度为5000μg/L的溶液效果图。
具体实施方式
为了进一步了解本发明的内容,结合附图和实施例对本发明作详细描述。
实施例1
光催化水泥基材料,它由以下两种组分按照一定质量复合而成:
本实施例配方设置:
A组分(基材料):直径为14cm,高为1cm的水泥浆圆片,水灰比(水泥与水的质量比)控制在0.35-0.4,水泥质量为22g,水质量为7.7g-8.8g;
B组分(光催化剂):1gTiO2/沸石复合材料;其中,B组分由以下2种组分按照一定的质量百分比复合而成:
(3)沸石;
(4)TiO2:占沸石质量比40%;
通过溶胶凝胶法制备TiO2溶胶,通过浸润法制备TiO2/沸石光催化剂,将TiO2/沸石光催化剂均匀洒布于水泥基材料上制备光催化水泥基材料。
具体步骤为:以钛酸四丁酯(Ti(OC4H9)4)为前驱体,将其和乙醇按体积比V(Ti(OC4H9)4):V(C2H5OH)=1:3混合,恒速剧烈搅拌10min,用硝酸调节溶液的pH值至4,恒速剧烈搅拌3~4h,得到透明略带浅黄色的溶胶。接着分别按TiO2占沸石质量分数比30%、35%、40%、45%的比例将沸石加入TiO2溶胶中,缓慢滴加去离子水使溶胶水解得到灰白色凝胶,将凝胶在100℃下干燥至恒重后研磨。最后将研磨好的粉末置于马弗炉中,在不同的温度(200℃、300℃、400℃、500℃)下锻烧4h,研磨即得到浅黄色粉末待用。
最后,应用于水中消毒副产物三氯乙酰胺的光降解方法,其步骤为:(1)配置三氯乙酰胺浓度为5000μg/L的的溶液1L,加入一片上述步骤制备的光催化水泥圆片;(2)通过紫外辐照,处理时间为0-20h,实现水中三氯乙酰胺的100%的去除。
本实施例中光催化水泥圆片对三氯乙酰胺的光降解效果如图1所示,该材料在光照1小时后降解率就达到了79.1%,光照4h降解率达到了100%。本实施例中该材料对污染物的去除安全高效,成本经济,运行稳定,操作简单。且可以根据不同的污染物改变制备过程中的TiO2的占比和煅烧温度来达到最优的降解效果。由此可证明,本发明方法对水中以三氯乙酰胺为代表的氮类消毒副产物的光降解功效。本实施例所用光催化水泥基材料可以根据污染物的种类与性质,通过调节制备过程中的二氧化钛的占比和煅烧温度得到降解效果最优的光催化水泥基材料。
结合附图1,本实施例的一种水中消毒副产物三氯乙酰胺的去除方法,处理对象为自来水中的以三氯乙酰胺为代表的氮类消毒副产物,可适用于农村供水“最后一公里”水处理,市政公共用水,小区集中供水等。
Claims (3)
1.一种光催化水泥基材料,它由以下两种组分按照一定质量复合而成:
A组分(基材料):直径为14cm,高为1cm的水泥浆圆片,水灰比(水泥与水的质量比)控制在0.35-0.4,水泥质量为22g,水质量为7.7g-8.8g;
B组分(光催化剂):1gTiO2/沸石复合材料;其中,B组分由以下2种组分按照一定的质量百分比复合而成:
(1)沸石;
(2)TiO2:占沸石质量比40%;
通过溶胶凝胶法制备TiO2溶胶,通过浸润法制备TiO2/沸石光催化剂,将TiO2/沸石光催化剂均匀洒布于水泥基材料上制备光催化水泥基材料。
2.一种制备权利要求1光催化水泥基材料的方法,其特征在于,具体步骤为:以钛酸四丁酯(Ti(OC4H9)4)为前驱体,将其和乙醇按体积比V(Ti(OC4H9)4):V(C2H5OH)=1:3混合,搅拌10min,用硝酸调节溶液的pH值至4,搅拌3~4h,得到透明略带浅黄色的溶胶;接着分别按TiO2占沸石质量分数比30%、35%、40%、45%的比例将沸石加入TiO2溶胶中,缓慢滴加去离子水使溶胶水解得到灰白色凝胶,将凝胶在100℃下干燥至恒重后研磨;最后将研磨好的粉末在不同的温度(200℃、300℃、400℃、500℃)下锻烧4h,研磨即得到浅黄色粉末。
3.一种由权利要求2制备获得的光催化水泥基材料应用于水中消毒副产物三氯乙酰胺的光降解方法,其步骤为:
(1)配置三氯乙酰胺浓度为5000μg/L的的溶液1L,加入一片权利要求2中制备的光催化水泥圆片;
(2)通过紫外辐照,处理时间为0-20h,实现水中三氯乙酰胺的100%的去除。
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