CN110624556A - 一种A位Sm掺杂LaFeO3光热协同催化剂 - Google Patents
一种A位Sm掺杂LaFeO3光热协同催化剂 Download PDFInfo
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Abstract
本发明属于有机废气降解领域,尤其是一种A位Sm掺杂LaFeO3光热协同催化剂。本发明针对现有降解VOCs催化剂催化反应起始温度高、降解耗能大以及降解途径单一的情况提供一种A位Sm掺杂LaFeO3光热协同催化剂及其制备方法。本发明以Sm元素对LaFeO3进行A位掺杂。借由LaFeO3较小的晶体尺寸获得丰富的催化反应位点。通过掺杂元素Sm提高催化剂对光吸收强度。使催化剂在可见光下能够产生强还原氧化效果的空穴‑电子对,增强氧化还原能力,有效降低反应温度,形成催化性能高、抗积碳性能优异、反应条件温和、耗能低、二次污染少的VOC光热协同催化剂。
Description
技术领域
本发明属于有机废气降解领域,尤其是一种A位Sm掺杂LaFeO3光热协同催化剂。
背景技术
当今,挥发性有机化合物(VOCs)已被公认为严重危害环境和人类健康的空气中的主要环境危害之一。大多数挥发性有机化合物不仅会对环境造成臭氧层损害,更严重的是,通过与其他空气污染物(即氮氧化物和硫氧化物)反应形成光化学烟雾,长时间接触还会威胁人类健康并导致不可逆转的损伤。在VOCs治理的技术方面,催化氧化技术是目前最具发展前景的处理技术之一。由于LaFeO3的晶体尺寸较小,可以获得潜在丰富的催化反应位点,获得高催化活性。同时,LaFeO3是钙钛矿类型的独特结构,显示出相对窄的带隙(2.5eV),从而产生高效的可见光吸收。并且通过掺杂元素Sm可以显著改变LaFeO3的吸收光强度,表现出强光吸收。本发明制备的催化剂具有高的降解VOCs效率和好的CO2选择性除此之外,该催化剂还具备性质稳定,环保无污染、价格经济等优点。制备的整体催化剂可以在200℃达到98%以上的降解效率。本发明的研究对我国的石油化工厂、涂装车间等降解VOCs具有很现实的意义;本发明针对现有VOCs催化剂催化温度高,降解途径单一以及催化剂能耗大的缺点,提供一种A位Sm掺杂LaFeO3光热协同催化剂及其制备方法。本发明以硝酸铁、硝酸镧、硝酸钐、柠檬酸、聚乙二醇为原料,采用溶胶-凝胶法进行制备。通过掺杂元素Sm提高催化剂对光吸收强度。该催化剂在可见光的辅助下能够产生强还原氧化效果的空穴-电子对,增强氧化还原能力,有效降低反应温度,形成催化性能高、抗积碳性能优异、反应条件温和、耗能低、二次污染少的VOC光热协同催化剂。
发明内容
本发明基于上述原因,提供了一种A位Sm掺杂LaFeO3光热协同催化剂,其特征为其主要制备步骤如下:
(1)称取一定比例的硝酸镧和硝酸钐于500mL烧杯中,同时加入一定比例硝酸铁、柠檬酸(络合剂)、聚乙二醇(分散剂),加入乙醇溶解,搅拌0.5h至完全溶解得到黄色澄清溶液;
(2)将步骤(1)中制备的黄色澄清溶液转入85℃恒温水浴中蒸发溶剂,待溶液凝成湿凝胶,置于通风柜中,用电炉上灼烧至没有黑烟后放至马弗炉中700℃焙烧7h成黑色片状物,即为A位Sm掺杂LaFeO3光热协同催化剂。
进一步地,步骤(1)所述的镧盐、钐盐与铁盐的摩尔比为3:1:4,柠檬酸与铁盐的摩尔比为2:1,聚乙二醇的用量是6g,乙醇的用量是120~150mL。
进一步地,步骤(2)中,溶液恒温蒸发溶剂的温度是85℃,恒温蒸发的时间为6~8h。
进一步地,步骤(2)中,焙烧方式为:在马弗炉中700~900℃焙烧6~7h。
本发明的有益效果为:
与单一的LaFeO3作为催化剂活性组分相比,掺杂Sm元素能明显的提高催化剂的在光照条件下的氧化还原能力,与LaFeO3实现优势互补的作用,使催化剂的光热协同催化活性进一步加强,使催化剂的在低温区域显示出更高活性与选择性。
附图说明
下面结合附图对本发明作进一步说明。
图1为实施例1中A位Sm掺杂LaFeO3光热协同催化剂XRD图。
具体实施方式
下面结合实施例和比较例,以具体说明一种A位Sm掺杂LaFeO3光热协同催化剂及其制备方法。以下实施例旨在说明本发明而不是对本发明的进一步限定。
实施例1
(1)在500mL的烧杯中加入0.0075mol硝酸镧,按照摩尔比La:Sm=3:1的比例称取0.0025mol硝酸钐于同一烧杯中,同时加入0.0100mol硝酸铁、0.0200mol柠檬酸(络合剂)、6g聚乙二醇(分散剂),加入150mL乙醇,搅拌0.5h至完全溶解得到黄色澄清溶液。
(2)将步骤(1)中制备的黄色澄清溶液转入恒温水浴槽中85℃恒温蒸发溶剂,将所得沉淀物放入烘箱85℃干燥6~8h,待溶液凝成湿凝胶,置于通风柜中,用电炉上灼烧至没有黑烟后,放至马弗炉中700℃焙烧7h成黑色片状物。附图1为所制备的A位Sm掺杂LaFeO3光热协同催化剂XRD图,位于23.7°、26.5°、32.6°、40.1°、46.5°、52.3°、57.6°、66.5°处的典型特征衍生峰对应了SmFeO3的(101)、(111)、(121)、(220)、(202)、(311)、(123)、(242)晶面,证实了正交相钙钛矿的形成。
比较例1
(1)在500mL的烧杯中加入0.0100mol硝酸镧,按照摩尔质量比La:Fe=1:1的比例称取0.0100mol硝酸铁,同时加入0.0200mol柠檬酸(络合剂)、6g聚乙二醇(分散剂)、加入150mL乙醇,搅拌0.5h至完全溶解得到黄色澄清溶液。
(2)将步骤(1)中制备的黄色澄清溶液转入恒温水浴槽中85℃恒温蒸发溶剂,将所得沉淀物放入烘箱85℃干燥6~8h,待溶液凝成湿凝胶,置于通风柜中,用电炉上灼烧至没有黑烟后,放至马弗炉中700℃焙烧7h成黑色片状物。
比较例2
(1)在500mL的烧杯中加入0.0100mol硝酸钐于,按照摩尔质量比Sm:Fe=1:1的比例称取0.0100mol硝酸铁,同时加入0.0200mol柠檬酸(络合剂)、6g聚乙二醇(分散剂)、加入150mL乙醇,搅拌0.5h至完全溶解得到黄色澄清溶液。
(2)将步骤(1)中制备的黄色澄清溶液转入恒温水浴槽中85℃恒温蒸发溶剂,将所得沉淀物放入烘箱85℃干燥6~8h,待溶液凝成湿凝胶,置于通风柜中,用电炉上灼烧至没有黑烟后,放至马弗炉中700℃焙烧7h成黑色片状物。
一种A位Sm掺杂LaFeO3光热协同催化剂性能测试
本发明在光热催化两用固定床(湖南华思)上进行。使用内径为1.5 mL的玻璃石英管作为催化剂反应器,并在玻璃管内衬石英砂基材。活性试验中,将约1 mL催化剂置于湖南华思仪器有限公司的固定床石英管反应器,使用高精度质量流量计精确控制入口气体流量。以N2为载气,气体组成为:甲苯为1000 ppm,O 2为20 vol%,气体空速为18000 h -1。试验前将灯连续通风30分钟,使催化剂吸附饱和,从而消除VOC吸附引起的浓度降低。在测试期间,使用光电离子气体传感器获得准确的入口VOC浓度,记录为[VOC]进 。然后,逐渐升高温度并检测出口处的VOC浓度,记录为[VOC]出。以20 ℃的间隔记录出口处的甲苯浓度,使用红外传感器检测出口的CO 2浓度。
由表1可见,本发明是具有光热协同效应的一种A位Sm掺杂LaFeO3光热协同催化剂,由于其具有的优良的光吸收性能和本身所具有的氧化还原能力,在降低了反应起始温度的同时还增强了在低温段的催化剂氧化还原能力,有效降低了传统催化剂能耗大,催化降解方式单一的缺点。
表1催化剂降解VOCs性能评价试验数据
最优甲苯降解率/% | 最高活性温度/(℃) | 活性温度区间/(℃) | |
实施例1 | 100.0 | 200 | 75~250 |
比较例1 | 100.0 | 250 | 125~275 |
比较例2 | 100.0 | 325 | 175~350 |
Claims (4)
1.一种A位Sm掺杂LaFeO3光热协同催化剂,其特征为其主要制备步骤如下:
(1)称取一定比例的硝酸镧和硝酸钐于500mL烧杯中,同时加入一定比例硝酸铁、柠檬酸(络合剂)、聚乙二醇(分散剂),加入乙醇溶解,搅拌0.5h至完全溶解得到黄色澄清溶液;
(2)将步骤(1)中制备的黄色澄清溶液转入85℃恒温水浴中蒸发溶剂,待溶液凝成湿凝胶,置于通风柜中,用电炉上灼烧至没有黑烟后放至马弗炉中700℃焙烧7h成黑色片状物,即为A位Sm掺杂LaFeO3光热协同催化剂。
2.根据权利要求1所述的A位Sm掺杂LaFeO3光热协同催化剂,其特征在于:在权利要求1步骤(1)中,镧盐与钐盐的摩尔比为3:1,钐盐与铁盐的摩尔比为1:4,柠檬酸与铁盐的摩尔比为2:1,聚乙二醇的用量是6g,乙醇的用量是120~150mL。
3.根据权利要求1所述的A位Sm掺杂LaFeO3光热协同催化剂,其特征在于:在权利要求1步骤(2)中,溶液恒温蒸发溶剂的温度是85℃,恒温蒸发的时间为6~8小时。
4.根据权利要求1所述的A位Sm掺杂LaFeO3光热协同催化剂,其特征在于:在权利要求1步骤(2)中,焙烧方式为:在马弗炉中700~900℃焙烧6~7h。
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CN116217216B (zh) * | 2023-02-28 | 2024-05-14 | 上海交通大学 | 可变太阳吸收率铁酸镧陶瓷粉体及其制备方法和应用 |
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