CN108786810A - 一种磁性硅酸铜及其在催化降解亚甲基蓝废水中的应用 - Google Patents

一种磁性硅酸铜及其在催化降解亚甲基蓝废水中的应用 Download PDF

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CN108786810A
CN108786810A CN201810478926.XA CN201810478926A CN108786810A CN 108786810 A CN108786810 A CN 108786810A CN 201810478926 A CN201810478926 A CN 201810478926A CN 108786810 A CN108786810 A CN 108786810A
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methylene blue
waste water
cupric silicate
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黄凯
汪会平
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Southeast University
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    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/70Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/74Iron group metals
    • B01J23/745Iron
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J35/00Catalysts, in general, characterised by their form or physical properties
    • B01J35/30Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
    • B01J35/33Electric or magnetic properties
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J35/00Catalysts, in general, characterised by their form or physical properties
    • B01J35/30Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
    • B01J35/396Distribution of the active metal ingredient
    • B01J35/398Egg yolk like
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J35/00Catalysts, in general, characterised by their form or physical properties
    • B01J35/60Catalysts, in general, characterised by their form or physical properties characterised by their surface properties or porosity
    • B01J35/61Surface area
    • B01J35/615100-500 m2/g
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    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00Treatment of water, waste water, or sewage
    • C02F1/72Treatment of water, waste water, or sewage by oxidation
    • C02F1/722Oxidation by peroxides
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00Treatment of water, waste water, or sewage
    • C02F1/72Treatment of water, waste water, or sewage by oxidation
    • C02F1/725Treatment of water, waste water, or sewage by oxidation by catalytic oxidation
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2101/00Nature of the contaminant
    • C02F2101/30Organic compounds
    • C02F2101/36Organic compounds containing halogen
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2101/00Nature of the contaminant
    • C02F2101/30Organic compounds
    • C02F2101/38Organic compounds containing nitrogen
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2101/00Nature of the contaminant
    • C02F2101/30Organic compounds
    • C02F2101/40Organic compounds containing sulfur

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  • Chemical Kinetics & Catalysis (AREA)
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Abstract

本发明公开了一种磁性硅酸铜及其在催化降解亚甲基蓝废水中的应用,该磁性硅酸铜具有较大的比表面积,用于催化过氧化氢降解亚甲基蓝废水可以加快降解速率和降解效果,在1h以内对亚甲基蓝的降解率可以达到100%,催化剂用量较少,且可以在外加磁场下快速实现固液分离,降低成本。

Description

一种磁性硅酸铜及其在催化降解亚甲基蓝废水中的应用
技术领域
本发明属于废水处理技术领域,具体涉及一种磁性硅酸铜及其在催化降解亚甲基蓝废水中的应用。
背景技术
在我国纺织业、印染业快速发展的浪潮中,产生的有机染料废水年排放量已经达到了数亿吨。当这种废水处理不彻底或者被偷排到河流等水体中之后,由于染料分子自身带有的颜色加重水环境的色度阻碍阳光的入射,将会影响动植物的正常生命活动。同时,有机染料分子很难通过生物自然降解的途径被分解,加上它本身就有的毒性,如果不采取措施治理,那么将会对生态平衡造成长期消极的影响。目前催化湿式过氧化法因为能够产生具有极强氧化能力的HO·,能够几乎将所有有机物进行完全地氧化分解,而在该方法中催化剂的选择十分关键,高效的、稳定的、损耗低的催化剂一直是研究的重点。非均相磁性催化剂作为固体催化剂并且本身具有磁性,在使用过后,仅仅使用外加磁场就可以方便的将催化剂从废水中分离出来,有利于回收循环使用,不仅节约了能源,而且操作起来非常方便。以磁性物质作为内核的yolk-shell结构的材料一方面磁性分布非常均匀,每个单分散的微粒子都具有磁性,同时具有yolk-shell结构的特性,即有较大的比表面积、较低的密度,在催化领域中已有不俗的表现。另外,因为很多研究表明铜基催化剂在催化降解废水领域中催化活性很高,而磁性的yolk-shell结构的硅酸铜材料之前从未有研究用于降解有机废水。
发明内容
本发明的目的是提供一种磁性硅酸铜及其在催化降解亚甲基蓝废水中的应用,该磁性硅酸铜具有较大的比表面积,对亚甲基蓝的降解效果好。
一种磁性硅酸铜,具有yolk-shell结构,核心为四氧化三铁,壳为硅酸铜,比表面积在399m2/g。
上述磁性硅酸铜在催化降解亚甲基蓝废水中的应用。
所述应用是将磁性硅酸铜和过氧化氢加至亚甲基蓝废水进行催化氧化反应。
进一步地,亚甲基蓝废水中亚甲基蓝的浓度为20mg/L~2000mg/L。
进一步地,催化氧化反应的温度为25~80℃,pH为2~12。
进一步地,磁性硅酸铜的用量为0.4g/L。
进一步地,过氧化氢的浓度为30wt.%,用量为10mL/L~80mL/L。
本发明所用的磁性硅酸铜具有较大的比表面积,可以加快降解速率和降解效果,在1h以内对亚甲基蓝的降解率可以达到100%,催化剂用量较少,且可以在外加磁场下快速实现固液分离,降低成本。
具体实施方式
下面通过实施例对本发明技术方案作进一步详细说明。
本发明所采用的磁性硅酸铜参照文献Liu J, Cheng J, Che R, et al.Synthesis and Microwave Absorption Properties of Yolk–Shell Microspheres withMagnetic Iron Oxide Cores and Hierarchical Copper Silicate Shells [J]. AcsApplied Materials & Interfaces, 2013, 5(7): 2503-9. 和Zhang X B, Tong H W,Liu S M, et al. An improved Stöber method towards uniform and monodisperseFe3O4@C nanospheres [J]. Journal of Materials Chemistry A, 2013, 1(25): 7488-7493.方法制成,比表面积为399m2/g。
实施例1
按照现有技术制备的磁性硅酸铜,即为目标催化剂。量取100 mL 30 mg/L pH为2.21的亚甲基蓝溶液于规格为250 mL的三颈烧瓶中,并称取40mg的催化剂加入其中,然后置于30℃水浴中进行机械搅拌,使其分散均匀。在催化剂搅拌分散均匀后,加入0.1mL质量浓度为30%的过氧化氢作为氧化剂,30min后亚甲基蓝降解率即达到100%。
实施例2
按照现有技术制备的磁性硅酸铜,即为目标催化剂。量取100 mL 200mg/L pH为6.78的亚甲基蓝溶液于规格为250 mL的三颈烧瓶中,并称取40mg的催化剂加入其中,然后置于50℃水浴中进行机械搅拌,使其分散均匀。在催化剂搅拌分散均匀后,加入0.3mL质量浓度为30%的过氧化氢作为氧化剂,15min后亚甲基蓝降解率即达到100%。
实施例3
按照现有技术制备的磁性硅酸铜,即为目标催化剂。量取100 mL800mg/L pH为9.53的亚甲基蓝溶液于规格为250 mL的三颈烧瓶中,并称取40mg的催化剂加入其中,然后置于79℃水浴中进行机械搅拌,使其分散均匀。在催化剂搅拌分散均匀后,加入0.7mL质量浓度为30%的过氧化氢作为氧化剂,7min后亚甲基蓝降解率即达到100%。
实施例4
按照现有技术制备的磁性硅酸铜,即为目标催化剂。量取100 mL 1700mg/L pH为11.67的亚甲基蓝溶液于规格为250 mL的三颈烧瓶中,并称取40mg的催化剂加入其中,然后置于79℃水浴中进行机械搅拌,使其分散均匀。在催化剂搅拌分散均匀后,加入0.7mL质量浓度为30%的过氧化氢作为氧化剂,5min后亚甲基蓝降解率即达到100%。
实施例5
按照现有技术制备的磁性硅酸铜,即为目标催化剂。量取500 mL 1000mg/L pH为10.76的亚甲基蓝溶液于规格为1000 mL的三颈烧瓶中,并称取200mg的催化剂加入其中,然后置于67℃水浴中进行机械搅拌,使其分散均匀。在催化剂搅拌分散均匀后,加入2.8mL质量浓度为30%的过氧化氢作为氧化剂,6min后亚甲基蓝降解率即达到100%。
实施例6
为了证明所用催化剂在催化氧化处理废水的应用方面具有更好的性能,将此催化剂与已报道过的催化剂进行了活性对比。催化剂1[Chinese Journal of Catalysis, 2013,34, 2125-2129]、催化剂2[Catalysis Communications, 2015, 72, 1-5]、催化剂3[Nanoscale, 2013, 5,3078-82]、催化剂4[Catalysis Communications, 2014, 46,174–178]对于亚甲基蓝的降解率分别为66%、63%、75%、50%,而在同样的反应条件下,本发明所制备催化剂对应的亚甲基蓝降解率全部达到了100%,因此该对比结果更加说明了这种硅酸铜材料在降解亚甲基蓝废水的应用中具有优异性能,并且为其在污水处理方面的应用开拓了更宽广的道路。

Claims (7)

1.一种磁性硅酸铜,具有yolk-shell结构,核心为四氧化三铁,壳为硅酸铜,比表面积为399m2/g。
2.权利要求1所述的磁性硅酸铜在催化降解亚甲基蓝废水中的应用。
3.根据权利要求2所述的磁性硅酸铜在催化降解亚甲基蓝废水中的应用,其特征在于:将磁性硅酸铜和过氧化氢加至亚甲基蓝废水进行催化氧化反应。
4.根据权利要求3所述的磁性硅酸铜在催化降解亚甲基蓝废水中的应用,其特征在于:亚甲基蓝废水中亚甲基蓝的浓度为20mg/L~2000mg/L。
5.根据权利要求3所述的磁性硅酸铜在催化降解亚甲基蓝废水中的应用,其特征在于:催化氧化反应的温度为25~80℃,pH为2~12。
6.根据权利要求3所述的磁性硅酸铜在催化降解亚甲基蓝废水中的应用,其特征在于:磁性硅酸铜的用量为0.4g/L。
7.根据权利要求3所述的磁性硅酸铜在催化降解亚甲基蓝废水中的应用,其特征在于:过氧化氢的浓度为30wt.%,用量为10mL/L~80mL/L。
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CN108404856A (zh) * 2018-05-17 2018-08-17 南京信息工程大学 用稻壳灰制备磁性硅酸铜吸附剂及其制备方法
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CN110482675A (zh) * 2019-08-25 2019-11-22 山东理工大学 一种用硅酸锰处理亚甲基蓝废水的方法
CN116618056A (zh) * 2023-04-20 2023-08-22 陕西科技大学 可见光响应的层状硅酸铁光芬顿催化剂、制备方法和应用

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CN108404856A (zh) * 2018-05-17 2018-08-17 南京信息工程大学 用稻壳灰制备磁性硅酸铜吸附剂及其制备方法
CN108404856B (zh) * 2018-05-17 2021-04-30 南京信息工程大学 用稻壳灰制备磁性硅酸铜吸附剂及其制备方法
CN110482676A (zh) * 2019-08-25 2019-11-22 山东理工大学 一种处理亚甲基蓝废水的方法
CN110482675A (zh) * 2019-08-25 2019-11-22 山东理工大学 一种用硅酸锰处理亚甲基蓝废水的方法
CN116618056A (zh) * 2023-04-20 2023-08-22 陕西科技大学 可见光响应的层状硅酸铁光芬顿催化剂、制备方法和应用
CN116618056B (zh) * 2023-04-20 2023-12-29 陕西科技大学 可见光响应的层状硅酸铁光芬顿催化剂、制备方法和应用

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