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Fe、Mn、Cu及其复合负载γ-Al2O3纳米颗粒的制备、表征和催化降解PVA性能

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苏扬帆, 李梦娟, 葛明桥. Fe、Mn、Cu及其复合负载γ-Al2O3纳米颗粒的制备、表征和催化降解PVA性能[J]. 环境化学, 2018, 37(6): 1272-1281. doi: 10.7524/j.issn.0254-6108.2017091802
引用本文: 苏扬帆, 李梦娟, 葛明桥. Fe、Mn、Cu及其复合负载γ-Al2O3纳米颗粒的制备、表征和催化降解PVA性能[J]. 环境化学, 2018, 37(6): 1272-1281. doi: 10.7524/j.issn.0254-6108.2017091802
shu
SU Yangfan, LI Mengjuan, GE Mingqiao. Preparation, characterization and catalytic performance of Fe, Mn,Cu and complex metallic oxides supported on γ-Al2O3[J]. Environmental Chemistry, 2018, 37(6): 1272-1281. doi: 10.7524/j.issn.0254-6108.2017091802
Citation: SU Yangfan, LI Mengjuan, GE Mingqiao. Preparation, characterization and catalytic performance of Fe, Mn,Cu and complex metallic oxides supported on γ-Al2O3[J]. Environmental Chemistry, 2018, 37(6): 1272-1281. doi: 10.7524/j.issn.0254-6108.2017091802
shu

Fe、Mn、Cu及其复合负载γ-Al2O3纳米颗粒的制备、表征和催化降解PVA性能

  • 1.

    江南大学纺织服装学院, 无锡, 214122;

  • 2.

    生态纺织教育部重点实验室, 江南大学, 无锡, 214122

  • 基金项目:

    国家高技术研究发展计划（2016YFB0302901-3）和中央高校基本科研业务费专项资金（JUSRP51723B）资助.

Preparation, characterization and catalytic performance of Fe, Mn,Cu and complex metallic oxides supported on γ-Al2O3

  • 1.

    College of Textile & Clothing, Jiangnan University, Wuxi, 214122, China;

  • 2.

    Key Laboratory of Eco-Textiles(Jiangnan University), Ministry of Education, Wuxi, 214122, China

  • Fund Project: Supported by the National High-tech R&D Program of China (2016YFB0302901-3) and the Fundamental Research Funds for the Central University(JUSRP51723B).

  • 摘要: 采用浸渍-煅烧法制备了Fe、Mn、Cu及其复合负载的γ-Al2O3纳米颗粒，采用了SEM-EDS、BET以及XRD等方法对制备得到的MnxOy/γ-Al2O3、CuxOy/γ-Al2O3、FexOy/γ-Al2O3以及FexCuyMnzOw/γ-Al2O3纳米颗粒进行了表征.结果表明，通过浸渍-煅烧法得到的四种纳米颗粒催化剂均可以和双氧水形成非均相类Fenton反应体系，产生大量羟基自由基，从而有效降解PVA大分子，降低废水中的PVA浓度.另外还通过Box-Behnken Design响应面分析法分别确定了MnxOy/γ-Al2O3、CuxOy/γ-Al2O3、FexOy/γ-Al2O3以及FexCuyMnzOw/γ-Al2O3纳米颗粒催化双氧水降解处理PVA的最佳工艺参数.利用GPC和GC-MS分析进一步表征PVA在不同催化剂条件下得到的降解产物后，分析结果表明：Fe、Mn、Cu复合负载的FexCuyMnzOw/γ-Al2O3纳米颗粒催化双氧水降解PVA的催化效果相对较好.当PVA初始反应浓度为1%，反应温度为60℃，催化剂投加量为0.5 g·L-1，双氧水投加量为60 mL·L-1时，PVA的浓度下降率可以达到95%以上，降解产物粘均分子量达到1395，分子量下降率达到99%，降解小分子产物主要包括丁酮、苯甲醛、己醛以及乙酸等不饱和小分子.
    Abstract: MnxOy/γ-Al2O3, CuxOy/γ-Al2O3, FexOy/γ-Al2O3 and FexCuyMnzOw/γ-Al2O3 nano particles were prepared by a wet impregnation-calcination method and characterized by SEM-EDS, BET and XRD. Results revealed that the prepared MnxOy/γ-Al2O3, CuxOy/γ-Al2O3, FexOy/γ-Al2O3 and FexCuyMnzOw/γ-Al2O3 nano particles rapidly reacted with H2O2 and produced large quantity of hydroxyl radicals. With the oxidation by hydroxyl radicals in heterogeneous Fenton-like process, PVA macromolecules in solution was effectively degraded and hence removed in aqueous solution. The Box-Behnken response surface analysis method was employed to investigate the optimum degradation parameters of PVA using MnxOy/γ-Al2O3, CuxOy/γ-Al2O3, FexOy/γ-Al2O3 and FexCuyMnzOw/γ-Al2O3 particles. Gel permeation chromatography (GPC) and gas chromatography-mass spectrometry (GC-MS) were also used to further identify the products of PVA under different catalyst conditions. It demonstrated that the catalytic performance of FexCuyMnzOw/γ-Al2O3 particles was better than other three catalysts. The PVA removal efficiency was above 95% while the reaction temperature was 60℃, initial concentration of PVA was 1%, H2O2 dosage was 60 min·L-1 and FexCuyMnzOw/γ-Al2O3 dosage was 0.5 g·L-1 respectively. Besides, the GPC detection also confirmed that PVA was effectively oxidized with a decreasing rate of about 99%, for the molecular weight from 100773 to 1395. Based on GC-MS analysis, it turned out that the degradation products of PVA mainly included several unsaturated compounds of lower molecular weight, such as butanone, benzaldehyde, hexanal and acetic acid, etc.
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  • 收稿日期:  2017-09-18
  • 刊出日期:  2018-06-15
苏扬帆, 李梦娟, 葛明桥. Fe、Mn、Cu及其复合负载γ-Al2O3纳米颗粒的制备、表征和催化降解PVA性能[J]. 环境化学, 2018, 37(6): 1272-1281. doi: 10.7524/j.issn.0254-6108.2017091802
引用本文: 苏扬帆, 李梦娟, 葛明桥. Fe、Mn、Cu及其复合负载γ-Al2O3纳米颗粒的制备、表征和催化降解PVA性能[J]. 环境化学, 2018, 37(6): 1272-1281. doi: 10.7524/j.issn.0254-6108.2017091802
shu
SU Yangfan, LI Mengjuan, GE Mingqiao. Preparation, characterization and catalytic performance of Fe, Mn,Cu and complex metallic oxides supported on γ-Al2O3[J]. Environmental Chemistry, 2018, 37(6): 1272-1281. doi: 10.7524/j.issn.0254-6108.2017091802
Citation: SU Yangfan, LI Mengjuan, GE Mingqiao. Preparation, characterization and catalytic performance of Fe, Mn,Cu and complex metallic oxides supported on γ-Al2O3[J]. Environmental Chemistry, 2018, 37(6): 1272-1281. doi: 10.7524/j.issn.0254-6108.2017091802
shu

Fe、Mn、Cu及其复合负载γ-Al2O3纳米颗粒的制备、表征和催化降解PVA性能

  • 1.  江南大学纺织服装学院, 无锡, 214122;
  • 2.  生态纺织教育部重点实验室, 江南大学, 无锡, 214122
  • 收稿日期:  2017-09-18
基金项目:

国家高技术研究发展计划（2016YFB0302901-3）和中央高校基本科研业务费专项资金（JUSRP51723B）资助.

摘要: 采用浸渍-煅烧法制备了Fe、Mn、Cu及其复合负载的γ-Al2O3纳米颗粒，采用了SEM-EDS、BET以及XRD等方法对制备得到的MnxOy/γ-Al2O3、CuxOy/γ-Al2O3、FexOy/γ-Al2O3以及FexCuyMnzOw/γ-Al2O3纳米颗粒进行了表征.结果表明，通过浸渍-煅烧法得到的四种纳米颗粒催化剂均可以和双氧水形成非均相类Fenton反应体系，产生大量羟基自由基，从而有效降解PVA大分子，降低废水中的PVA浓度.另外还通过Box-Behnken Design响应面分析法分别确定了MnxOy/γ-Al2O3、CuxOy/γ-Al2O3、FexOy/γ-Al2O3以及FexCuyMnzOw/γ-Al2O3纳米颗粒催化双氧水降解处理PVA的最佳工艺参数.利用GPC和GC-MS分析进一步表征PVA在不同催化剂条件下得到的降解产物后，分析结果表明：Fe、Mn、Cu复合负载的FexCuyMnzOw/γ-Al2O3纳米颗粒催化双氧水降解PVA的催化效果相对较好.当PVA初始反应浓度为1%，反应温度为60℃，催化剂投加量为0.5 g·L-1，双氧水投加量为60 mL·L-1时，PVA的浓度下降率可以达到95%以上，降解产物粘均分子量达到1395，分子量下降率达到99%，降解小分子产物主要包括丁酮、苯甲醛、己醛以及乙酸等不饱和小分子.

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