CN110252307A - 一种脱除挥发性有机废气的平板式催化剂及其制备方法 - Google Patents
一种脱除挥发性有机废气的平板式催化剂及其制备方法 Download PDFInfo
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- CN110252307A CN110252307A CN201910513292.1A CN201910513292A CN110252307A CN 110252307 A CN110252307 A CN 110252307A CN 201910513292 A CN201910513292 A CN 201910513292A CN 110252307 A CN110252307 A CN 110252307A
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- MIVBAHRSNUNMPP-UHFFFAOYSA-N manganese(2+);dinitrate Chemical compound [Mn+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O MIVBAHRSNUNMPP-UHFFFAOYSA-N 0.000 description 1
- SQQMAOCOWKFBNP-UHFFFAOYSA-L manganese(II) sulfate Chemical compound [Mn+2].[O-]S([O-])(=O)=O SQQMAOCOWKFBNP-UHFFFAOYSA-L 0.000 description 1
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Classifications
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- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
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- B01D53/864—Removing carbon monoxide or hydrocarbons
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- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
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- B01J23/83—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with rare earths or actinides
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- B01J23/84—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/889—Manganese, technetium or rhenium
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- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2229/00—Aspects of molecular sieve catalysts not covered by B01J29/00
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- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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Abstract
本发明涉及一种脱除挥发性有机废气的平板式催化剂及其制备方法，属于环保技术与VOCs治理领域，该催化剂由活性组分、玻璃纤维、粘结剂、分散剂、载体等混合作为催化剂泥料，采用辊压涂覆制得平板式VOCs催化燃烧催化剂。其中催化剂中载体、不锈钢网、玻璃纤维、活性组分组成，质量比为100:(50～150):(1～8):(10～25)。本方法制备的催化剂具有机械强度高、化学稳定性好、原料成本低、制备工艺简单等特点，对低浓度有机废气具有良好的净化效果，适用于含尘等复杂恶劣有机废气的处理。
Description
技术领域
本发明涉及一种脱除挥发性有机废气的平板式催化剂及其制备方法，属于环境保护技术领域。
背景技术
化石能源需求随着经济社会的快速发展而的迅速增加，带来严重的空气污染问题。其中，挥发性有机物(VOCs)废气是常见的大气污染物之一，我国年排放量达3000万吨以上。根据世界卫生组织(WHO)定义，挥发性有机化合物(Volatile organic compounds，简称VOCs)废气是熔点低于室温而沸点在50-260°之间的挥发性有机化合物的总称。VOCs主要的大气污染源之一，主要来源于石油化工、涂料、制药、印刷等行业排放的废气，包括非甲烷烃类、含氧有机物、含氮有机物、含硫有机物等。VOCs的大量排放给环境造成了严重的危害，而且能与NO2和SO2通过复杂的大气化学反应形成细颗粒物(PM)和臭氧等污染物，是引起大气光化学烟雾、细颗粒物污染和臭氧层破坏等二次污染问题的重要前体物。此外，VOCs对人体的呼吸系统、生殖系统、免疫系统等有严重的损害作用，部分VOCs甚至有致癌作用。寻求合理有效的治理技术来解决VOCs污染问题，已经迫在眉睫。
挥发性有机废气有多种处理方法，总体可分为两类：回收技术和消除技术。第一类应用的场合是回收高浓度的有机废气(大于5000mg/m3)；第二类是通过化学反应、生物降解等方法将废气中的有机物转化为无毒或低毒物质。其中，针对浓度较低且回收价值不高的VOCs，常采用催化燃烧的方法进行消除。催化燃烧法即在催化剂存在的条件下，VOCs可在较低的起燃温度下进行无焰燃烧，完全分解成二氧化碳和水，并放出热量。具有燃烧温度低，能量消耗少、无二次污染等特点。
催化燃烧法的核心是催化剂，按照活性组分不同可分为贵金属与非贵金属催化剂
两大类。其中Pt、Pd、Rh、Ir等贵金属催化剂已经工业化，具有起燃温度与完全燃烧温度低、应用范围较广等特点，但是由于贵金属储量有限，该类催化剂存在价格昂贵且易中毒等问题。非贵金属价态多变且价格相对较低，通过元素调变制备复合氧化物催化剂具有高催化活性、高稳定性、良好的抗中毒性等优点，因此该类催化剂的制备逐渐引起了工业界的广泛关注。
目前使用的催化燃烧催化剂多为负载型整体式催化剂，如黄琼等(现代化工,2015,35(3):135-138.)制备的工业大尺寸MnCeOx/堇青石整体式催化剂具有较好的处理苯、二甲苯的能力，且抗水抗毒性能优异。目前多使用浸渍法对催化剂进行负载，Deng Lei等(Journal of Rare Earths,2018(3))采用浸渍法制备出一种NiMnO3/Ce0.75Zr0.25O2/堇青石整体式催化剂，对苯、甲苯和二甲苯的混合物催化燃烧表现出较好的催化活性，在275℃时混合VOCs的转化率达到95.6％。然而此法制得的催化剂活性组分容易从堇青石载体表面脱落，从而影响催化剂的稳定性和使用寿命。另外，实际VOCs废气排放条件较为复杂，除挥发性有机化合物外，还存在颗粒物等固体杂质，不仅容易堵塞蜂窝陶瓷整体式催化剂的孔道，而且会造成催化剂磨损和活性组分流失，导致催化剂失活。因此，开发适用于复杂条件特别是含尘废气的VOCs脱除催化剂具有重要意义。
发明内容
本发明的目的是针对整体式催化剂存在的上述缺陷，提出了一种脱除挥发性有机废气的平板式催化剂，本发明的另一目的是提供上述催化剂的制备方法。该催化剂以不锈钢网板为基体，将催化剂泥料双面加压涂覆在不锈钢网板上，干燥锻烧后得到的板式催化剂用于脱除VOCs废气，具有机械强度高、抗堵塞、耐磨损及抗中毒能力强等优点。
本发明的技术方案为：一种脱除挥发性有机废气的平板式催化剂，其特征在于所述平板式催化剂由载体、不锈钢网、玻璃纤维和活性组分组成，其质量比为100:(50～150):(1～8):(10～25)；所述的载体为二氧化钛、三氧化二铝、二氧化硅、二氧化锆或分子筛中的任一种；活性组分为氧化钴、氧化锰、氧化铈、氧化铜、氧化镧或氧化铁中的一种或几种。
本发明还提供了制备上述平板式催化剂的方法，其具体步骤如下：
A.将载体、玻璃纤维、粘结剂和分散剂按质量比100:(1～8):(2～11):(5～10)混合，搅拌均匀，得到混合粉料；
B.将活性组分金属盐混合，加入适量去离子水，搅拌均匀，得到活性组分溶液；
C.将步骤A得到的混合粉料与步骤B得到的活性组分溶液混合，搅拌均匀后在阴暗处陈腐，得到催化剂泥料；其中载体和活性组分金属盐的质量比为100:(40～100)；
D.将步骤C得到的催化剂泥料挤出后置于不锈钢网板上，然后通过辊压进行均匀涂覆、成型，最后经干燥、焙烧制得板式催化剂；其中载体和不锈钢网的质量比为100:(50～150)。
优选上述不锈钢网为304不锈钢网，网厚0.5mm～1.5mm；网眼长2mm～10mm，网眼宽为1mm～7mm，网筋为0.5mm～0.8mm。不锈钢钢网的网眼尺寸是决定板式催化剂质量的重要因素，网眼尺寸过小会降低钢网的产能，同时也会减小催化剂的有效面积，从而影响催化剂性能；而网眼尺寸过大会导致钢网易断裂，影响产品机械强度和质量。
优选所述的粘结剂为聚乙烯醇、羧甲基纤维素或羟丙基甲基纤维素中的一种或两种以上任意组合。
优选所述分散剂为乙醇胺、二乙醇胺、三乙醇胺或甘油中的一种或两种以上任意组合。
优选所述活性组分金属盐为含金属的硝酸盐、醋酸盐、硫酸盐或氯化盐；所述的金属为钴、锰、铈、铜、镧或铁中的一种或几种。
优选步骤C中陈腐时间为2～3天。
优选步骤D中的干燥温度为100～130℃，干燥时间为2～6h，焙烧温度为450～600℃，焙烧时间为4～6h。
本发明中催化剂活性评价在连续流动固定床石英管反应器中进行，原料气有机物浓度为500～2000ppm，反应气流量为50～100mL/min。
有益效果：
(1)本发明的催化剂机械强度高，具有较高的活性和抗毒性能，尤其对高灰运行工况具有很强的适应性，抗堵塞、耐磨损性强。
(2)本发明制备的催化剂原料来源广泛、价格低廉，制备过程操作方便，便于放大生产。
(3)本发明制备的板式催化剂与传统浸渍法涂覆制备的整体式催化剂相比具有较强的耐磨性能，延长了催化剂使用寿命。
具体实施方式
实施例1
取100g二氧化钛、4g玻璃纤维、3g羧甲基纤维素、5g二乙醇胺，混合均匀，得到均匀的干料，取13g醋酸钴，55g硝酸铁，添加74g的去离子水，搅拌均匀后得到钴铁溶液，将干料与钴铁溶液均匀混合，得到催化剂泥料，陈腐2天。将泥料涂覆于不锈钢网上，不锈钢网厚0.5mm，网眼长8mm，网眼宽为3mm，网筋宽为0.5mm，辊压均匀后，然后在100℃温度下干燥2h，再放入马弗炉中进行焙烧，焙烧温度为550℃，焙烧时间为4h，自然冷却后即得到板式催化剂,其中载体、不锈钢网、玻璃纤维和活性组分的质量比为100:100：4:16。
取一定量的板式催化剂置于连续流动固定床石英管反应器中，原料气中甲苯浓度为1000ppm,反应气流量为90mL/min。反应温度在365℃时，甲苯的去除率为99％。催化剂连续运行100h以上，活性未见明显降低。
实施例2
取100g二氧化钛、5g玻璃纤维、10g聚乙烯醇、8g乙醇胺，混合均匀，得到均匀的干料，取10g硝酸钴，60g硝酸铜，添加70g的去离子水，搅拌均匀后得到钴铜溶液，将干料与钴铜溶液均匀混合，得到催化剂泥料，陈腐2天。将泥料涂覆于不锈钢网上，不锈钢网厚1mm，网眼长5mm，网眼宽为4mm，网筋宽为0.6mm，辊压均匀后，然后在100℃温度下干燥4h，再放入马弗炉中进行焙烧，焙烧温度为500℃，焙烧时间为4h，自然冷却后即得到板式催化剂，其中载体、不锈钢网、玻璃纤维和活性组分的质量比为100:60：5:22。
取一定量的板式催化剂置于连续流动固定床石英管反应器中，原料气中甲苯浓度为1000ppm,反应气流量为70mL/min。反应温度在354℃时，甲苯的去除率为99％。催化剂连续运行100h以上，活性未见明显降低。
实施例3
取100g二氧化锆、6g玻璃纤维、8g羧甲基纤维素、3g聚乙烯醇、3g三乙醇胺、4g甘油，混合均匀，得到均匀的干料，取8g氯化钴，45g氯化锰，添加84g的去离子水，搅拌均匀后得到钴锰溶液，将干料与钴锰溶液均匀混合，得到催化剂泥料，陈腐2天。将泥料涂覆于不锈钢网上，不锈钢网厚1.5mm，网眼长6mm，网眼宽为5mm，网筋宽为0.8mm，辊压均匀后，然后在110℃温度下干燥4h，再放入马弗炉中进行焙烧，焙烧温度为450℃，焙烧时间为5h，自然冷却后即得到板式催化剂，其中载体、不锈钢网、玻璃纤维和活性组分的质量比为100:150：6:23。
取一定量的板式催化剂置于连续流动固定床石英管反应器中，原料气中甲苯浓度为1000ppm,反应气流量为80mL/min。反应温度在362℃时，甲苯的去除率为99％。催化剂连续运行100h以上，活性未见明显降低。
实施例4
取100g分子筛、1g玻璃纤维、2g聚乙烯醇、1g羟丙基甲基纤维素、5g乙醇胺、1g二乙醇胺，混合均匀，得到均匀的干料，取11g硝酸镧，53g硫酸锰，添加80g的去离子水，搅拌均匀后得到镧锰溶液，将干料与镧锰溶液均匀混合，得到催化剂泥料，陈腐3天。将泥料涂覆于不锈钢网上，不锈钢网厚0.5mm，网眼长10mm，网眼宽为4mm，网筋宽为0.7mm，辊压均匀后，然后在110℃温度下干燥6h，再放入马弗炉中进行煅烧，焙烧温度为500℃，焙烧时间为6h，自然冷却后即得到板式催化剂，其中载体、不锈钢网、玻璃纤维和活性组分的质量比为100:120：1:23。
取一定量的板式催化剂置于连续流动固定床石英管反应器中，原料气中甲苯浓度为1000ppm,反应气流量为60mL/min。反应温度在359℃时，甲苯的去除率为99％。催化剂连续运行100h以上，活性未见明显降低。
实施例5
取100g二氧化钛、2g玻璃纤维、10g聚乙烯醇、8g乙醇胺，混合均匀，得到均匀的干料，取2.5g硝酸铈，10g硝酸钴，85g 50％硝酸锰溶液，添加30g的去离子水，搅拌均匀后得到铈钴锰溶液，将干料与铈钴锰溶液均匀混合，得到催化剂泥料，陈腐2天。将泥料涂覆于不锈钢网上，不锈钢网厚0.6mm，网眼长5mm，网眼宽为5mm，网筋宽为0.7mm，辊压均匀后，然后在110℃温度下干燥4h，再放入马弗炉中进行焙烧，焙烧温度为550℃，焙烧时间为4h，自然冷却后即得到板式催化剂，其中载体、不锈钢网、玻璃纤维和活性组分的质量比为100:80：2:16。
取一定量的板式催化剂置于连续流动固定床石英管反应器中，原料气中甲苯浓度为500ppm,反应气流量为50mL/min。反应温度在336℃时，甲苯的去除率为99％。催化剂连续运行100h以上，活性未见明显降低。
实施例6
取100g二氧化硅、7g玻璃纤维、5g聚乙烯醇、3g三乙醇胺、6g甘油，混合均匀，得到均匀的干料，取10g硝酸钴，58g硫酸铁，添加80g的去离子水，搅拌均匀后得到钴铁溶液，将干料与钴铁溶液均匀混合，得到催化剂泥料，陈腐2天。将泥料涂覆于不锈钢网上，不锈钢网厚0.5mm，网眼长10mm，网眼宽为5mm，网筋宽为0.8mm，辊压均匀后，然后在130℃温度下干燥3h，再放入马弗炉中进行焙烧，焙烧温度为550℃，焙烧时间为5h，自然冷却后即得到板式催化剂，其中载体、不锈钢网、玻璃纤维和活性组分的质量比为100:100：7:10。
取一定量的板式催化剂置于连续流动固定床石英管反应器中，原料气中甲苯浓度为2000ppm,反应气流量为100mL/min。反应温度在384℃时，甲苯的去除率为99％。催化剂连续运行100h以上，活性未见明显降低。
实施例7
取100g三氧化二铝、8g玻璃纤维、5g羟丙基甲基纤维素、5g聚乙烯醇、5g二乙醇胺、5g甘油，混合均匀，得到均匀的干料，取15g硝酸铈，52g硫酸铜，添加75g的去离子水，搅拌均匀后得到铈铜溶液，将干料与铈铜溶液均匀混合，得到催化剂泥料，陈腐3天。将泥料涂覆于不锈钢网上，不锈钢网厚0.5mm，网眼长8mm，网眼宽为3mm，网筋宽为0.6mm，辊压均匀后，然后在120℃温度下干燥6h，再放入马弗炉中进行焙烧，焙烧温度为600℃，焙烧时间为4h，自然冷却后即得到板式催化剂，其中载体、不锈钢网、玻璃纤维和活性组分的质量比为100:150：8:25。
取一定量的板式催化剂置于连续流动固定床石英管反应器中，原料气中甲苯浓度为1000ppm,反应气流量为60mL/min。反应温度在352℃时，甲苯的去除率为99％。催化剂连续运行100h以上，活性未见明显降低。
Claims (8)
1.一种脱除挥发性有机废气的平板式催化剂，其特征在于由载体、不锈钢网、玻璃纤维和活性组分组成，其质量比为100:(50～150):(1～8):
(10～25)；其中载体为二氧化钛、三氧化二铝、二氧化硅、二氧化锆或分子筛中的任一种；活性组分由氧化钴、氧化锰、氧化铈、氧化铜、氧化镧或氧化铁中的一种或几种组成。
2.一种制备如权利要求1所述的平板式催化剂的方法，其具体步骤如下：
A.将载体、玻璃纤维、粘结剂和分散剂按质量比为100:(1～8):(2～11):(5～10)混合，搅拌均匀，得到混合粉料；
B.将活性组分金属盐混合，加入适量去离子水，搅拌均匀，得到活性组分溶液；
C.将步骤A得到的混合粉料与步骤B得到的活性组分溶液混合，搅拌均匀后在阴暗处陈腐，得到催化剂泥料；其中载体和活性组分金属盐的质量比为100:(40～100)；
D.将步骤C得到的催化剂泥料挤出后置于不锈钢网板上，然后通过辊压进行均匀涂覆、成型，最后经干燥、焙烧制得板式催化剂；其中载体和不锈钢网的质量比为100:(50～150)。
3.根据权利要求1所述的方法，其特征在于：所述不锈钢网为304不锈钢网，网厚0.5mm～1.5mm；网眼长2mm～10mm，网眼宽为1mm～7mm，网筋为0.5mm～0.8mm。
4.根据权利要求1所述的方法，其特征在于所述的粘结剂为聚乙烯醇、羧甲基纤维素或羟丙基甲基纤维素中的一种或两种以上任意组合。
5.根据权利要求1所述的方法，其特征在于：所述分散剂为乙醇胺、二乙醇胺、三乙醇胺或甘油中的一种或两种以上任意组合。
6.根据权利要求1所述的方法，其特征在于：所述活性组分金属盐为含金属的硝酸盐、醋酸盐、硫酸盐或氯化盐；所述的金属为钴、锰、铈、铜、镧或铁中的一种或几种。
7.根据权利要求1所述的方法，其特征在于：所述步骤C中陈腐时间为2～3天。
8.根据权利要求1所述的方法，其特征在于：所述步骤D中的干燥温度为100～130℃，干燥时间为2～6h，焙烧温度为450～600℃，焙烧时间为4～6h。
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