CN106902857A - 一种膨胀g‑C3N4光催化剂及其制备方法 - Google Patents
一种膨胀g‑C3N4光催化剂及其制备方法 Download PDFInfo
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Abstract
本发明公开了一种膨胀g‑C3N4光催化剂及其制备方法，属于材料制备及光催化技术领域。该催化剂仅仅使用尿素或三聚氰胺为前驱体，在空气中直接两步热处理得到g‑C3N4粉末，然后在真空加热条件下，利用乙醇快速气化过程对其膨胀，得到一种高活性的膨胀g‑C3N4光催化材料。本发明所得膨胀g‑C3N4光催化材料具有很强的吸附能力、优异的可见光降解和产氢能力。本发明的显著优点在于：成本低廉，过程简单，条件温和且稳定，效果显著，易于放大生产。
Description
技术领域
本发明属于物理化学领域，具体涉及一种光催化剂及其制备方法。
背景技术
目前，能源短缺和环境污染问题日益突出，光催化技术被认为是一种低成本、环境友好的绿色能源和环境治理技术。制备高性能、宽响应范围、低成本的光催化材料是光催化技术需要解决的主要问题。
类石墨型氮化碳(g-C3N4)具有类似石墨的层状结构，层间含有C3N3环或C6N7环，环之间通过末端的N原子相连而形成一层无限扩展的平面，属于非金属化合物半导体。它的带隙为2.7eV，对可见光具有吸收能力(λ>420nm)，在水溶液中具有高稳定性和无毒、易制备等特点。作为新型光催化剂可广泛应用于各种催化反应中，包括降解有机染料、光解水制氢、有机反应等。目前合成g-C3N4的方法主要有缩聚法、模板法。通过传统缩聚法可制备g-C3N4粉末颗粒；软模板法主要使用表面活性剂为模板，以含氮前驱物为源，经水热反应制备具有介孔结构的g-C3N4体相材料；使用硬模板法制备的多孔g-C3N4虽然具有很大的比表面积和良好的光催化性能，但是合成过程必须使用强酸去除模板剂，方法繁琐且很不环保。
由于上述层状g-C3N4体相材料存在光生电子-空穴对复合率较高、量子效率低、比表面积小等缺点，将其膨胀后剥离成单层或少层的二维材料，可有效提高比表面积，能够达到高效、快速、广谱降解环境有机污染物、光解水产氢的目的。
发明内容
本发明所要解决的技术问题是关于层状g-C3N4体相光催化材料的有效剥离。通过膨胀剥离过程提高g-C3N4的比表面积、改善其光催化活性。为了解决这一技术问题，本发明提出利用真空膨胀法对两步热处理所得层状结构g-C3N4粉末进行有效剥离。
本发明所采用的技术方案是以简单、易得的尿素或三聚氰胺为原料，先通过两步热处理法合成层状结构g-C3N4粉末，再将g-C3N4通过真空膨胀法进行剥离，得到膨胀g-C3N4光催化材料。
本发明的目的在于提供一种用真空膨胀法得到的膨胀g-C3N4光催化材料及其制备方法。该方法主要利用真空加热条件下乙醇沸点降低，饱和蒸气压增大，乙醇溶液在管状容器中剧烈气化体积膨胀过程，将分散在其中的二维层状g-C3N4晶格间距急剧拉大，导致膨胀剥离。真空膨胀法具有加热温度低，工艺设备简单、操作方便、成本低廉，效果显著，所得g-C3N4光催化剂具有高效吸附性和可见光光催化能力。
本发明的制备方法如下：
1.将一定量的尿素或三聚氰胺倒入坩埚中，然后置于炉子中进行两步热处理。热处理过程为：由室温升至500℃后恒温热处理2h，继续升温至550℃再恒温热处理2h，之后自然降温冷却至室温，得到浅黄色g-C3N4粉末。
2.取一定量的g-C3N4粉末倒入一端闭口的管状器皿中，加入少量乙醇，然后置于真空干燥箱内，在80-120℃下真空膨胀，得到膨胀g-C3N4可见光光催化材料。
3.最后对膨胀g-C3N4光催化材料性能进行表征，在可见光下进行光催化降解和裂解水产氢。所述的水中降解目标为罗丹明B(RhB)。
附图说明
图1不同温度条件下制备的膨胀g-C3N4光催化剂的XRD图谱，(a)为全谱，(b)为局部放大图谱。
图2不同温度条件下制备的膨胀g-C3N4光催化剂的拉曼图谱
图3不同温度条件下制备的膨胀g-C3N4光催化剂的罗丹明B降解图谱
图4不同温度条件下制备的膨胀g-C3N4光催化剂的产氢率图谱
图5膨胀g-C3N4光催化剂的产氢量随时间的关系图谱
图6不同温度条件下制备的膨胀g-C3N4光催化剂的光致发光图谱
具体实施方式
下面结合具体实例对本发明的产品制备方法作进一步的说明。
具体实施步骤如下：
实施例1：
(1)取10g尿素置于带盖的坩埚内，使尿素处于半封闭状态放入马弗炉内进行两步热处理。以4℃/min的升温速率，将炉子温度升到500℃，热处理2h，再以10℃/min升温到550℃进行第二步热处理，保温2h，之后自然降温到室温，得到淡黄色g-C3N4粉末。
(2)将步骤(1)得到的淡黄色样品倒入敞口离心管中，加入2ml的无水乙醇，再把离心管放在大烧杯内，一起放进真空干燥箱内进行真空膨胀剥离，温度设为80℃，时间为3h，膨胀剥离结束时，反应物会分布在离心管及烧杯内壁上，最终得到膨胀g-C3N4光催化剂。
(3)对膨胀g-C3N4光催化剂进行光催化降解和裂解水产氢表征。
实施例2：
(1)取10g尿素置于带盖的坩埚内，使尿素处于半封闭状态放入马弗炉内进行两步热处理。以4℃/min的升温速率，将炉子温度升到500℃，热处理2h，再以10℃/min升温到550℃进行第二步热处理，保温2h，之后自然降温到室温，得到淡黄色g-C3N4粉末。
(2)将步骤(1)得到的淡黄色样品倒入敞口离心管中，加入3ml的无水乙醇，再把离心管放在大烧杯内，一起放进真空干燥箱内进行真空膨胀剥离，温度设为100℃，时间为2h，膨胀剥离结束时，反应物会分布在离心管及烧杯内壁上，最终得到膨胀g-C3N4光催化剂。
(3)对膨胀g-C3N4光催化剂进行光催化降解和裂解水产氢表征。
实施例3：
(1)取10g三聚氰胺置于带盖的坩埚内，使尿素处于半封闭状态放入马弗炉内进行两步热处理。以4℃/min的升温速率，将炉子温度升到500℃，热处理2h，再以10℃/min升温到550℃进行第二步热处理，保温2h，之后自然降温到室温，得到淡黄色g-C3N4粉末。
(2)将步骤(1)得到的淡黄色样品倒入一端敞口玻璃管中，加入4ml的无水乙醇，再把离心管放在大烧杯内，一起放进真空干燥箱内进行真空膨胀剥离，温度设为120℃，时间为2h，膨胀剥离结束时，反应物会分布在离心管及烧杯内壁上，最终得到膨胀g-C3N4光催化剂。
(3)对膨胀g-C3N4光催化剂进行光催化降解和裂解水产氢表征。
实施例4：
罗丹明B溶液降解性能的测试：
本具体实施方式中，所用罗丹明B溶液的浓度为10mg/L，所用可见光源为300W氙灯(通过滤波片滤去小于420nm波长光)，取80ml罗丹明B溶液和50mg膨胀g-C3N4光催化剂混合，先在无光照条件下搅拌60min，使溶液混合均匀吸附。然后开灯光照，进行光催化反应。在光照过程中每隔一段时间抽取5ml左右的反应液，经高速离心后，取上清液在分光光度计上进行光吸收测试，罗丹明B溶液的降解率计算公式为：降解率＝(C0－C)/C0×100％，式中C0为初始罗丹明B溶液在554nm波长处的吸光度值，C为光照后罗丹明B溶液的吸光度值。
光催化产氢性能测试：
本测试在泊菲莱光催化产氢系统上实施。先称取50mg膨胀g-C3N4光催化剂倒入反应装置中，加入90ml水、10ml抗坏血酸、2ul的氯铂酸。连接好反应装置进行测试。所用可见光源为300W氙灯(通过滤波片滤去小于420nm波长光)。
附图分析:
从X射线衍射图谱(XRD)可以看出(图1)，与未真空膨胀的g-C3N4粉末相比，真空膨胀的g-C3N4光催化剂对应的(002)衍射峰都明显向小角度方向移动，表明g-C3N4的层间距被拉大，体现了膨胀效果。
由膨胀g-C3N4降解罗丹明B图谱(图3)可以看出，膨胀g-C3N4光催化剂的吸附性明显增强，从未真空膨胀前吸附能力20％增加到～50％，光催化降解速率也明显增加，从未真空膨胀前的50min缩短到26min，效率显著。膨胀g-C3N4的光催化产氢结果也说明其光催化活性大大增加，产氢率提高了近1倍，而且不同时间内产氢量基本呈现线性增长趋势。
这些实验结果都表明利用本发明提出的真空膨胀法，能够成功得到膨胀g-C3N4粉末光催化材料，该材料表现出了优异的吸附性和光催化活性。
最后应说明的是：以上所述仅为本发明的优选实施例而已，并不用于限制本发明，尽管参照前述实施例对本发明进行了详细的说明，对于本领域的技术人员来说，其依然可以对前述各实施例所记载的技术方案进行修改，或者对其中部分技术特征进行等同替换。凡在本发明的精神和原则之内，所作的任何修改、等同替换、改进等，均应包含在本发明的保护范围之内。
Claims (6)
1.一种膨胀g-C3N4光催化剂及其制备方法，其特征在于，取尿素或三聚氰胺为原料，先通过热处理法合成层状结构g-C3N4粉末，再将g-C3N4通过真空膨胀法进行剥离，得到膨胀g-C3N4光催化材料。
2.根据权利要求1所述的一种膨胀g-C3N4光催化剂及其制备方法，其特征在于真空膨胀过程中所用一端闭口的管状器皿为塑料材质或玻璃材质。
3.根据权利要求1所述的一种膨胀g-C3N4光催化剂及其制备方法，其步骤为：
一、将尿素或三聚氰胺倒入坩埚中，然后置于炉子中进行两步热处理；热处理过程为：由室温升至500℃后恒温热处理2h，继续升温至550℃再恒温热处理2h，之后自然降温冷却至室温，得到浅黄色g-C3N4粉末；
二、取g-C3N4粉末倒入一端闭口的管状器皿中，加入少量乙醇，然后置于真空干燥箱内，在80-120℃下真空膨胀，得到膨胀g-C3N4可见光光催化材料；
三、最后对膨胀g-C3N4光催化材料性能进行表征，在可见光下进行光催化降解和裂解水产氢。
4.根据权利要求3所述的一种膨胀g-C3N4光催化剂制备方法，其特征在于，g-C3N4在乙醇溶液中的分散摩尔浓度为1.3-2.7mol/L。
5.根据权利要求3所述的一种膨胀g-C3N4光催化剂制备方法，其特征在于，真空膨胀温度为80℃。
6.根据权利要求3所述的一种膨胀g-C3N4光催化剂制备方法，其特征在于，真空膨胀时间为2-3h。
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