Maryam Mirasgari, Seyed Mehdi Alavi, Mehran Rezaei
{"title":"制备和评估用于甲烷全氧化的 LaCu1-xNixO3(x = 0、0.1、0.3、0.5 和 0.7)过氧化物催化剂","authors":"Maryam Mirasgari, Seyed Mehdi Alavi, Mehran Rezaei","doi":"10.1007/s11164-024-05377-4","DOIUrl":null,"url":null,"abstract":"<div><p>A series of Ni-substituted LaCu<sub>1-x</sub>Ni<sub>x</sub>O<sub>3</sub> (x = 0, 0.1, 0.3, 0.5 and 0.7) catalysts were prepared by a mechanochemical synthesis method and the prepared samples were used in catalytic combustion of methane. The catalytic results indicated that the partial substitution of Ni affected the catalytic performance and the increase in nickel content increased the catalytic activity and among the prepared catalysts the LaCu<sub>0.5</sub>Ni<sub>0.5</sub>O<sub>3</sub> sample possessed the highest catalytic activity and thermal stability. The results showed that methane conversion reached from 7.8 to 73.8% at 500 °C with the substitution of Ni in the amount of x = 0.5. Also, the addition of Ni instead of Cu in the LaCu<sub>1-x</sub>Ni<sub>x</sub>O<sub>3</sub> led to an increase in total pore volume and specific surface area and a decrease in average crystalline size. According to O<sub>2</sub>-TPD profiles of the LaCu<sub>1-x</sub>Ni<sub>x</sub>O<sub>3</sub> catalysts, mobility of lattice oxygen (O<sup>2−</sup>) has a crucial role in determining the performance of these catalysts. The H<sub>2</sub>-TPR results indicated that the addition of Ni slightly improved the reducibility of catalysts. Furthermore, a decrease in calcination temperature of LaCu<sub>0.5</sub>Ni<sub>0.5</sub>O<sub>3</sub> catalyst resulted in an increase in the catalytic activity due to the enhancement in the concentration of oxygen vacancy and specific surface area. Also, the results revealed that the increase in feed ratio (CH<sub>4</sub>/O<sub>2</sub>) leads to an increment in methane conversion.</p></div>","PeriodicalId":753,"journal":{"name":"Research on Chemical Intermediates","volume":"50 10","pages":"4835 - 4854"},"PeriodicalIF":2.8000,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Preparation and evaluation of the LaCu1-xNixO3 (x = 0, 0.1, 0.3, 0.5 and 0.7) perovskite catalysts for total oxidation of methane\",\"authors\":\"Maryam Mirasgari, Seyed Mehdi Alavi, Mehran Rezaei\",\"doi\":\"10.1007/s11164-024-05377-4\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>A series of Ni-substituted LaCu<sub>1-x</sub>Ni<sub>x</sub>O<sub>3</sub> (x = 0, 0.1, 0.3, 0.5 and 0.7) catalysts were prepared by a mechanochemical synthesis method and the prepared samples were used in catalytic combustion of methane. The catalytic results indicated that the partial substitution of Ni affected the catalytic performance and the increase in nickel content increased the catalytic activity and among the prepared catalysts the LaCu<sub>0.5</sub>Ni<sub>0.5</sub>O<sub>3</sub> sample possessed the highest catalytic activity and thermal stability. The results showed that methane conversion reached from 7.8 to 73.8% at 500 °C with the substitution of Ni in the amount of x = 0.5. Also, the addition of Ni instead of Cu in the LaCu<sub>1-x</sub>Ni<sub>x</sub>O<sub>3</sub> led to an increase in total pore volume and specific surface area and a decrease in average crystalline size. According to O<sub>2</sub>-TPD profiles of the LaCu<sub>1-x</sub>Ni<sub>x</sub>O<sub>3</sub> catalysts, mobility of lattice oxygen (O<sup>2−</sup>) has a crucial role in determining the performance of these catalysts. The H<sub>2</sub>-TPR results indicated that the addition of Ni slightly improved the reducibility of catalysts. Furthermore, a decrease in calcination temperature of LaCu<sub>0.5</sub>Ni<sub>0.5</sub>O<sub>3</sub> catalyst resulted in an increase in the catalytic activity due to the enhancement in the concentration of oxygen vacancy and specific surface area. Also, the results revealed that the increase in feed ratio (CH<sub>4</sub>/O<sub>2</sub>) leads to an increment in methane conversion.</p></div>\",\"PeriodicalId\":753,\"journal\":{\"name\":\"Research on Chemical Intermediates\",\"volume\":\"50 10\",\"pages\":\"4835 - 4854\"},\"PeriodicalIF\":2.8000,\"publicationDate\":\"2024-08-29\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Research on Chemical Intermediates\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s11164-024-05377-4\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Research on Chemical Intermediates","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s11164-024-05377-4","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
采用机械化学合成法制备了一系列镍取代的 LaCu1-xNixO3 (x = 0、0.1、0.3、0.5 和 0.7)催化剂,并将制备的样品用于甲烷的催化燃烧。催化结果表明,镍的部分取代影响了催化性能,镍含量的增加提高了催化活性,在制备的催化剂中,LaCu0.5Ni0.5O3 样品具有最高的催化活性和热稳定性。结果表明,镍的取代量为 x = 0.5 时,甲烷转化率在 500 °C 时从 7.8% 提高到 73.8%。此外,在 LaCu1-xNixO3 中添加 Ni 而不是 Cu 会导致总孔体积和比表面积的增加以及平均结晶尺寸的减小。根据 LaCu1-xNixO3 催化剂的 O2-TPD 曲线,晶格氧(O2-)的流动性对这些催化剂的性能起着至关重要的作用。H2-TPR 结果表明,镍的添加略微改善了催化剂的还原性。此外,降低 LaCu0.5Ni0.5O3 催化剂的煅烧温度可提高催化活性,这是因为氧空位浓度和比表面积增加了。研究结果还显示,进料比(CH4/O2)的增加会提高甲烷的转化率。
Preparation and evaluation of the LaCu1-xNixO3 (x = 0, 0.1, 0.3, 0.5 and 0.7) perovskite catalysts for total oxidation of methane
A series of Ni-substituted LaCu1-xNixO3 (x = 0, 0.1, 0.3, 0.5 and 0.7) catalysts were prepared by a mechanochemical synthesis method and the prepared samples were used in catalytic combustion of methane. The catalytic results indicated that the partial substitution of Ni affected the catalytic performance and the increase in nickel content increased the catalytic activity and among the prepared catalysts the LaCu0.5Ni0.5O3 sample possessed the highest catalytic activity and thermal stability. The results showed that methane conversion reached from 7.8 to 73.8% at 500 °C with the substitution of Ni in the amount of x = 0.5. Also, the addition of Ni instead of Cu in the LaCu1-xNixO3 led to an increase in total pore volume and specific surface area and a decrease in average crystalline size. According to O2-TPD profiles of the LaCu1-xNixO3 catalysts, mobility of lattice oxygen (O2−) has a crucial role in determining the performance of these catalysts. The H2-TPR results indicated that the addition of Ni slightly improved the reducibility of catalysts. Furthermore, a decrease in calcination temperature of LaCu0.5Ni0.5O3 catalyst resulted in an increase in the catalytic activity due to the enhancement in the concentration of oxygen vacancy and specific surface area. Also, the results revealed that the increase in feed ratio (CH4/O2) leads to an increment in methane conversion.
期刊介绍:
Research on Chemical Intermediates publishes current research articles and concise dynamic reviews on the properties, structures and reactivities of intermediate species in all the various domains of chemistry.
The journal also contains articles in related disciplines such as spectroscopy, molecular biology and biochemistry, atmospheric and environmental sciences, catalysis, photochemistry and photophysics. In addition, special issues dedicated to specific topics in the field are regularly published.