Experimental study and kinetic model analysis on photothermal catalysis of formaldehyde by manganese and cerium based catalytic materials.

IF 2.1 4区 环境科学与生态学 Q3 ENGINEERING, ENVIRONMENTAL Journal of the Air & Waste Management Association Pub Date : 2023-05-01 DOI:10.1080/10962247.2023.2179685
Zhiqiang Wang, Wei Xiao, Fangzhu Zhang, Shimin Zhang, Wufeng Jin
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The results showed that the higher the temperature in the experimental box (56.7 ± 0.2°C, 62.6 ± 0.2°C, 68.2 ± 0.2°C), the better the formaldehyde degradation by catalytic effect (formaldehyde degradation percentage: 76.2<math><mrow><mrow><mi>%</mi></mrow></mrow></math>, 78.3<math><mrow><mrow><mi>%</mi></mrow></mrow></math>, 82.1<math><mrow><mrow><mi>%</mi></mrow></mrow></math>). With increase of the initial formaldehyde concentration (200 <math><mrow><mi>p</mi><mi>p</mi><mi>b</mi></mrow></math>, 500 <math><mrow><mi>p</mi><mi>p</mi><mi>b</mi></mrow></math>, 1000 <math><mrow><mi>p</mi><mi>p</mi><mi>b</mi></mrow></math>), the catalytic effect first increased and then decreased (formaldehyde degradation percentage: 63<math><mrow><mrow><mi>%</mi></mrow></mrow></math>, 78.3<math><mrow><mrow><mi>%</mi></mrow></mrow></math>, 70.6<math><mrow><mrow><mi>%</mi></mrow></mrow></math>). The catalytic effect risen gradually with the increase of load ratio (10<math><mi>g</mi><mrow><mo>/</mo></mrow><mrow><msup><mi>m</mi><mn>2</mn></msup></mrow></math>, 20<math><mi>g</mi><mrow><mo>/</mo></mrow><mrow><msup><mi>m</mi><mn>2</mn></msup></mrow></math>, and 40<math><mi>g</mi><mrow><mo>/</mo></mrow><mrow><msup><mi>m</mi><mn>2</mn></msup></mrow></math>), and the formaldehyde degradation percentages were 62.8<math><mrow><mrow><mi>%</mi></mrow></mrow></math>, 78.3<math><mrow><mrow><mi>%</mi></mrow></mrow></math>, and 81.1<math><mrow><mrow><mi>%</mi></mrow></mrow></math>, respectively. According to the expressions of the Eley-Rideal (ER) model, the Langmuir-Hinshelwood (LH) model, and the Mars-Van Krevelen (MVK) model, the experimental results were fitted and verified, and it was found that the ER model had a high degree of fit. It is more suitable to explain the catalytic mechanism of formaldehyde by MnO<sub>x</sub>-CeO<sub>2</sub> catalyst in the experimental cabin, where formaldehyde is in the adsorption state and oxygen is in the gas phase.<i>Implications</i>: Judging from the current research status, vehicles have become an indispensable mode of travel for people, and the air quality in the vehicle is not optimistic. Most vehicles generally have the phenomenon of excessive formaldehyde. The characteristic of formaldehyde in the car is the continuous release, especially in the hot summer, the temperature inside the car rises sharply under the sun radiation. At this time, the formaldehyde concentration exceeds the standard by 4 to 5 times, which can cause great damage to the health of the passengers. In order to improve the air quality in the car, it is necessary to adopt the correct purification technology to degrade formaldehyde. The problem brought by this situation is how to effectively use solar radiation and high temperature in the car to degrade formaldehyde in the car. Therefore, this study uses the thermal catalytic oxidation technology to catalyze the degradation of formaldehyde in the high temperature environment of the car in summer. The selected catalyst is MnO<sub>x</sub>-CeO<sub>2</sub>, mainly because manganese oxide (MnO<sub>x</sub>) itself is the most effective catalyst for volatile organic compounds (TCO) among transition metal oxides, and CeO<sub>2</sub> has excellent oxygen storage and release capacity and Oxidation activity, which helps to improve the activity of MnO<sub>x</sub>. Finally, the effects of temperature, initial concentration of formaldehyde and catalyst loading on the experiment were explored, and the kinetic model of thermal catalytic oxidation of formaldehyde with MnO<sub>x</sub>-CeO<sub>2</sub> catalyst was analyzed to provide technical support for the future application of this research in practice.</p>","PeriodicalId":49171,"journal":{"name":"Journal of the Air & Waste Management Association","volume":null,"pages":null},"PeriodicalIF":2.1000,"publicationDate":"2023-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the Air & Waste Management Association","FirstCategoryId":"93","ListUrlMain":"https://doi.org/10.1080/10962247.2023.2179685","RegionNum":4,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
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Abstract

Modern people spend more and more time in cars in their daily lives, and the pollution of formaldehyde in the car may directly affect people's health. Thermal catalytic oxidation technology by solar light is a potential way to purify formaldehyde in cars. MnOx-CeO2 was prepared by the modified co-precipitation method as the main catalyst, and the basic characteristic (SEM, N2 adsorption, H2-TPR, UV-visible absorbance) were also analyzed in detail. The experimental study was set up to simulate the solar photothermal catalysis of formaldehyde in-car environment. The results showed that the higher the temperature in the experimental box (56.7 ± 0.2°C, 62.6 ± 0.2°C, 68.2 ± 0.2°C), the better the formaldehyde degradation by catalytic effect (formaldehyde degradation percentage: 76.2%, 78.3%, 82.1%). With increase of the initial formaldehyde concentration (200 ppb, 500 ppb, 1000 ppb), the catalytic effect first increased and then decreased (formaldehyde degradation percentage: 63%, 78.3%, 70.6%). The catalytic effect risen gradually with the increase of load ratio (10g/m2, 20g/m2, and 40g/m2), and the formaldehyde degradation percentages were 62.8%, 78.3%, and 81.1%, respectively. According to the expressions of the Eley-Rideal (ER) model, the Langmuir-Hinshelwood (LH) model, and the Mars-Van Krevelen (MVK) model, the experimental results were fitted and verified, and it was found that the ER model had a high degree of fit. It is more suitable to explain the catalytic mechanism of formaldehyde by MnOx-CeO2 catalyst in the experimental cabin, where formaldehyde is in the adsorption state and oxygen is in the gas phase.Implications: Judging from the current research status, vehicles have become an indispensable mode of travel for people, and the air quality in the vehicle is not optimistic. Most vehicles generally have the phenomenon of excessive formaldehyde. The characteristic of formaldehyde in the car is the continuous release, especially in the hot summer, the temperature inside the car rises sharply under the sun radiation. At this time, the formaldehyde concentration exceeds the standard by 4 to 5 times, which can cause great damage to the health of the passengers. In order to improve the air quality in the car, it is necessary to adopt the correct purification technology to degrade formaldehyde. The problem brought by this situation is how to effectively use solar radiation and high temperature in the car to degrade formaldehyde in the car. Therefore, this study uses the thermal catalytic oxidation technology to catalyze the degradation of formaldehyde in the high temperature environment of the car in summer. The selected catalyst is MnOx-CeO2, mainly because manganese oxide (MnOx) itself is the most effective catalyst for volatile organic compounds (TCO) among transition metal oxides, and CeO2 has excellent oxygen storage and release capacity and Oxidation activity, which helps to improve the activity of MnOx. Finally, the effects of temperature, initial concentration of formaldehyde and catalyst loading on the experiment were explored, and the kinetic model of thermal catalytic oxidation of formaldehyde with MnOx-CeO2 catalyst was analyzed to provide technical support for the future application of this research in practice.

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锰、铈基催化材料光热催化甲醛的实验研究及动力学模型分析。
现代人在日常生活中花在汽车上的时间越来越多,而车内甲醛的污染可能直接影响到人们的健康。太阳能光热催化氧化技术是一种有潜力的净化车内甲醛的方法。以改性共沉淀法为主催化剂制备了MnOx-CeO2,并对其基本特性(SEM、N2吸附、H2-TPR、紫外可见吸光度)进行了详细分析。建立了模拟甲醛车内环境的太阳光热催化实验研究。结果表明,实验箱内温度越高(56.7±0.2°C、62.6±0.2°C、68.2±0.2°C),催化降解甲醛效果越好(甲醛降解率分别为76.2%、78.3%、82.1%)。随着甲醛初始浓度(200 ppb、500 ppb、1000 ppb)的增加,催化效果先升高后降低(甲醛降解率分别为63%、78.3%、70.6%)。随着负载比(10g/m2、20g/m2和40g/m2)的增加,催化效果逐渐提高,甲醛降解率分别为62.8%、78.3%和81.1%。根据Eley-Rideal (ER)模型、Langmuir-Hinshelwood (LH)模型和Mars-Van Krevelen (MVK)模型的表达式,对实验结果进行了拟合和验证,发现ER模型具有较高的拟合度。在甲醛处于吸附状态、氧气处于气相的实验舱内,用MnOx-CeO2催化剂来解释甲醛的催化机理更为合适。启示:从目前的研究现状来看,车辆已经成为人们不可缺少的出行方式,车内空气质量不容乐观。大多数车辆普遍存在甲醛超标的现象。车内甲醛的特点是不断释放,特别是在炎热的夏天,车内温度在太阳辐射下急剧上升。此时,甲醛浓度超标4 ~ 5倍,会对乘客的健康造成极大损害。为了改善车内空气质量,必须采用正确的净化技术来降解甲醛。这种情况带来的问题是如何有效地利用太阳辐射和车内高温来降解车内甲醛。因此,本研究采用热催化氧化技术,在夏季汽车高温环境下催化降解甲醛。催化剂选择MnOx-CeO2,主要是因为在过渡金属氧化物中,氧化锰(MnOx)本身是挥发性有机化合物(TCO)最有效的催化剂,而CeO2具有优异的储放氧能力和氧化活性,有助于提高MnOx的活性。最后,探讨了温度、甲醛初始浓度和催化剂负载对实验的影响,并分析了MnOx-CeO2催化剂热催化氧化甲醛的动力学模型,为本研究未来在实践中的应用提供技术支持。
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来源期刊
Journal of the Air & Waste Management Association
Journal of the Air & Waste Management Association ENGINEERING, ENVIRONMENTAL-ENVIRONMENTAL SCIENCES
CiteScore
5.00
自引率
3.70%
发文量
95
审稿时长
3 months
期刊介绍: The Journal of the Air & Waste Management Association (J&AWMA) is one of the oldest continuously published, peer-reviewed, technical environmental journals in the world. First published in 1951 under the name Air Repair, J&AWMA is intended to serve those occupationally involved in air pollution control and waste management through the publication of timely and reliable information.
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