CN105457676A - 一种非金属三维宏观结构石墨烯-有机物气溶胶光催化剂 - Google Patents
一种非金属三维宏观结构石墨烯-有机物气溶胶光催化剂 Download PDFInfo
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Abstract
本发明公开了一种非金属三维宏观结构石墨烯-有机物（RGO-EY）气溶胶光催化剂的制备方法和应用。以氧化石墨烯（GO）、有机物曙红（EY，C20H6Br4Na2O）为原料，通过简单的水热处理和冷冻干燥相结合的方式，制备得到了非金属三维宏观结构RGO-EY光催化剂。制备的RGO-EY？具有显著的可见光响应特性和和良好的光催化选择性氢化芳香族硝基化合物至相应的芳香族胺基化合物活性，并且具有可见光催化还原去除污染物Cr(VI)的性能。该催化剂的制备方法简单，原材料来源丰富，成本低廉，对环境友好，并且易于分离回收。
Description
技术领域
本发明属于光催化剂领域，具体涉及一种非金属三维宏观结构石墨烯-有机物气溶胶光催化剂的制备方法及其在可见光下催化加氢芳香族硝基化合物至相应的芳香族胺类化合物和可见光催化去除污染物Cr(VI)的应用。
背景技术
环境污染和能源短缺是当前人类面临的重大挑战，亦是实现人类社会可持续发展必须优先考虑的重大课题。半导体光催化技术作为一项利用太阳能来直接驱动一系列重要化学反应的绿色技术，由于其操作简单、反应条件温和(常温常压)、能耗低、以及适用范围广等特点，被认为是从根本上解决全球能源和环境问题的理想途径之一。然而，传统半导体光催化剂多为金属氧化物或金属硫化物，常常包含稀有昂贵的(如Ti,Nb,Ta,In)、甚至有毒的(如Cd）金属元素，导致催化剂的制备价格昂贵、易造成环境污染等。此外，传统半导体光催化剂的量子效率和太阳能利用率仍然较低，远不能满足实际应用的需求。
有机染料，作为一类重要的具有优良光吸收能力的非金属材料，近年来被广泛应用于太阳能染料敏化电池领域，其具有原材料丰富、成本低等特点，在大面积工业化生产应用中具有较大的优势。在光催化领域，利用有机染料作为光催化剂的研究已有报道，但相比于传统半导体光催化剂在光催化领域的广泛研究和应用，非金属有机染料光催化剂的研究仍处于初步阶段。在目前报道的多数文献中，有机物染料多溶解于反应溶剂，造成非金属有机染料光催化剂与反应物和产物的分离困难，也不利于催化剂的回收利用。因此，积极开发新型有效、成本低廉、环境友好且易于分离回收的非金属光催化剂对促进光催化科学技术在太阳能催化转换及能源环境方面的实际应用具有重要意义。
发明内容
本发明的目的在于提供一种非金属三维宏观结构石墨烯-有机物（RGO-EY）气溶胶光催化剂的制备方法和应用，制备的RGO-EY具有显著的可见光响应特性和良好的光催化选择性氢化芳香族硝基化合物至相应的芳香族胺基化合物活性，并且具有可见光催化还原去除污染物Cr(VI)的性能。该催化剂的制备方法简单，原材料来源丰富，成本低廉，对环境友好，并且易于分离回收。
为实现上述目的，本发明采用如下技术方案：
一种非金属三维宏观结构石墨烯-有机物（RGO-EY）气溶胶光催化剂不包含金属元素，具有三维宏观气溶胶结构。
制备如上所述的RGO-EY气溶胶光催化剂的方法包括以下步骤：
（1）将氧化石墨烯（GO）、水（H2O）、有机物曙红（EY，C20H6Br4Na2O）超声混合均匀，120~200oC水热处理6~48h，得到亲水性的三维石墨烯-有机物（RGO-EY）固体；
（2）将所得的固体冷冻干燥处理，得到非金属三维宏观结构疏水的石墨烯-有机物（RGO-EY）气溶胶光催化剂。
所述的氧化石墨烯、水和有机曙红的质量比为：60:60000:1~4:4000:1；冷冻干燥时间为：12~72h
所述的石墨烯-有机物气溶胶光催化剂用于水相中可见光下选择性氢化芳香族硝基化合物至相应的芳香族胺基化合物。
所述的石墨烯-有机物气溶胶光催化剂用于可见光光催化还原去除污染物六价铬Cr(VI)。
所述的芳香族硝基化合物为下列结构：
中的任意一种。
光催化选择性氢化硝基芳香化合物至相应的胺基芳香化合物具体步骤如下：
（1）取60mL10ppm的芳香族硝基化合物溶液、25mg的RGO-EY光催化剂和80μL空穴捕获剂三乙醇胺于反应瓶中，搅拌均匀，并通入氮气(60mL/min)，在黑暗状态下吸附2h，使芳香族硝基化合物在光催化剂表面达到吸附平衡；
（2）在氮气保护下，对上述体系进行可见光光照（λ>420nm），每隔一定时间后取适量液体，进行紫外-可见吸收光谱分析和液相色谱分析；
光催化还原去除污染物Cr(VI)具体步骤如下：
（1）取60mL10ppm的Cr(VI)溶液、25mg的RGO-EY光催化剂和80μL空穴捕获剂三乙醇胺于反应瓶中，搅拌均匀，并通入氮气(60mL/min)，在黑暗状态下吸附2h，使Cr(VI)化合物在光催化剂表面达到吸附平衡；
（2）在氮气保护下，对上述体系进行可见光光照（λ>420nm），每隔一定时间后取适量液体，进行紫外-可见吸收光谱分析。
本发明的有益效果在于：
（1）本发明首次制备得到了具有非金属特性、三维宏观结构的石墨烯-有机物（RGO-EY）气溶胶光催化剂，所制得的复合光催化材料具有显著的可见光响应特性；
(2）所制备的三维宏观石墨烯-有机物（RGO-EY）气溶胶光催化剂表现出显著优于传统粉末状材料（RGO-EY(Powder)）的导电性能，在光催化过程更有利于促进光生电子-空穴对的快速分离，提高电子迁移能力、从而使复合光催化材料具有更高的光催化性能；
（3）本发明首次将RGO-EY复合型光催化剂应用于可见光下光催化选择性（选择性>99%）氢化芳香族硝基化合物至相应的芳香族胺基化合物和光催化还原去除污染物Cr(VI)；
（4）RGO-EY光催化剂的生产工艺简单、制作成本低、并且环境友好、易于分离回收。
附图说明
图1是非金属RGO-EY气溶胶光催化剂的宏观结构及SEM图；
图2是非金属RGO-EY气溶胶光催化剂的XPS图；
图3是三维宏观结构非金属RGO-EY气溶胶光催化剂与粉末状RGO-EY(Powder)催化剂的压力-电阻率和尼奎斯特阻抗测试图；
图4是非金属RGO-EY气溶胶、RGO-EY(Powder)光催化剂可见光照射下氢化对硝基苯胺(A)、还原去除Cr(VI)(B)以及氢化对硝基苯酚(C)、邻硝基苯酚(D)、邻硝基苯胺(E)、对甲氧基硝基苯(F)等不同取代基芳香族硝基化合物的活性图。
具体实施方式
本发明用下列实施例来进一步说明本发明，但本发明的保护范围并不限于下列实施例。
实施例1
将30mgGO粉末、0.5mgEY粉末以及30g去离子水超声混合均匀，接着120°C水热处理48h，得到亲水性的三维石墨烯-有机物（RGO-EY）固体，将所得的固体冷冻干燥处理12h，得到非金属三维宏观结构疏水的石墨烯-有机物（RGO-EY）气溶胶光催化剂。将宏观柱状25mg的RGO-EY催化剂、60mL10ppm的对硝基苯胺溶液以及80μL三乙醇胺混合均匀，以60mL/min的流量向反应液中持续通入氮气，待吸附平衡后，置于可见光(>420nm)下光照60min，对硝基苯胺的转化率为67%，相应的生成对苯二胺产物的选择性达99%以上。
实施例2
将30mgGO粉末、1.5mgEY粉末以及30g去离子水超声混合均匀，接着180°C水热处理12h，得到亲水性的三维石墨烯-有机物（RGO-EY）固体，将所得的固体冷冻干燥处理24h，得到非金属三维宏观结构疏水的石墨烯-有机物（RGO-EY）气溶胶光催化剂。将宏观柱状25mg的RGO-EY催化剂、60mL10ppm的对硝基苯胺溶液以及80μL三乙醇胺混合均匀，以60mL/min的流量向反应液中持续通入氮气，待吸附平衡后，置于可见光(>420nm)下光照30min，对硝基苯胺的转化率为94%，相应的生成对苯二胺产物的选择性达99%以上。
实施例3
将30mgGO粉末、7.5mgEY粉末以及30g去离子水超声混合均匀，接着150°C水热处理24h，得到亲水性的三维石墨烯-有机物（RGO-EY）固体，将所得的固体冷冻干燥处理36h，得到非金属三维宏观结构疏水的石墨烯-有机物（RGO-EY）气溶胶光催化剂。将宏观柱状25mg的RGO-EY催化剂、60mL10ppm的对硝基苯胺溶液以及80μL三乙醇胺混合均匀，以60mL/min的流量向反应液中持续通入氮气，待吸附平衡后，置于可见光(>420nm)下光照3min，对硝基苯胺的转化率为99%，相应的生成对苯二胺产物的选择性达99%以上。
实施例4
将30mgGO粉末、0.5mgEY粉末以及30g去离子水超声混合均匀，接着200°C水热处理6h，得到亲水性的三维石墨烯-有机物（RGO-EY）固体，将所得的固体冷冻干燥处理72h，得到非金属三维宏观结构疏水的石墨烯-有机物（RGO-EY）气溶胶光催化剂。将宏观柱状的25mgRGO-EY催化剂、60mL10ppm的Cr(VI)以及80μL三乙醇胺混合均匀，以60mL/min的流量向反应液中持续通入氮气，待吸附平衡后，置于可见光(>420nm)下光照60min，RGO-EY对Cr(VI)的光催化去除率达到40%。
实施例5
将30mgGO粉末、1.5mgEY粉末以及30g去离子水超声混合均匀，接着180°C水热处理12h，得到亲水性的三维石墨烯-有机物（RGO-EY）固体，将所得的固体冷冻干燥处理24h，得到非金属三维宏观结构疏水的石墨烯-有机物（RGO-EY）气溶胶光催化剂。将宏观柱状的25mgRGO-EY催化剂、60mL10ppm的Cr(VI)以及80μL三乙醇胺混合均匀，以60mL/min的流量向反应液中持续通入氮气，待吸附平衡后，置于可见光(>420nm)下光照40min，RGO-EY对Cr(VI)的光催化去除率达到99%。
实施例6
将30mgGO粉末、7.5mgEY粉末以及30g去离子水超声混合均匀，接着180°C水热处理12h，得到亲水性的三维石墨烯-有机物（RGO-EY）固体，将所得的固体冷冻干燥处理24h，得到非金属三维宏观结构疏水的石墨烯-有机物（RGO-EY）气溶胶光催化剂。将宏观柱状的25mgRGO-EY催化剂、60mL10ppm的Cr(VI)以及80μL三乙醇胺混合均匀，以60mL/min的流量向反应液中持续通入氮气，待吸附平衡后，置于可见光(>420nm)下光照3min，RGO-EY对Cr(VI)的光催化去除率达到100%。
从图3可以看出，相比于粉末状RGO-EY(Powder)复合材料，所制备的三维宏观结构非金属RGO-EY气溶胶光催化剂表现出更优良的导电性能和更高的电荷分离迁移效率，从而促使其表现出更加显著的可见光氢化芳香族硝基化合物至相应的芳香族胺基化合物和还原去除污染物六价铬Cr(VI)的活性(如图4所示)。
以上所述仅为本发明的较佳实施例，凡依本发明申请专利范围所做的均等变化与修饰，皆应属本发明的涵盖范围。
Claims (5)
1.一种非金属三维宏观结构石墨烯-有机物气溶胶光催化剂的制备方法，其特征在于：包括以下步骤：
（1）将氧化石墨烯、水和有机物曙红超声混合均匀，120~200oC水热处理6~48h，得到亲水性的三维石墨烯-有机物固体；
（2）将所得的固体冷冻干燥处理，得到非金属三维宏观结构疏水的石墨烯-有机物气溶胶光催化剂。
2.根据权利1所述的方法，其特征在于：所述的氧化石墨烯、水和有机曙红的质量比为：60:60000:1~4:4000:1；冷冻干燥时间为：12~72h。
3.一种如权利要求1所述的制备方法制得的非金属三维宏观结构石墨烯-有机物气溶胶光催化剂的应用，其特征在于：所述的石墨烯-有机物气溶胶光催化剂用于水相中可见光下选择性氢化芳香族硝基化合物至相应的芳香族胺基化合物。
4.一种如权利要求1所述的制备方法制得的非金属三维宏观结构石墨烯-有机物气溶胶光催化剂的应用，其特征在于：所述的石墨烯-有机物气溶胶光催化剂用于可见光光催化还原去除污染物六价铬。
5.根据权利要求3所述的非金属三维宏观结构石墨烯-有机物气溶胶光催化剂的应用，其特征在于：所述的芳香族硝基化合物为下列结构：
中的任意一种。
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| CN108499612A (zh) * | 2018-05-16 | 2018-09-07 | 福州大学 | 以石墨烯为支撑骨架的三维碳化钛/署红水凝胶光催化复合材料及其制备方法与应用 |
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