{"title":"通过掺杂 Sm 的 Co3O4 来削弱 Co-O 键,从而提高 SmyCoOx 对甲苯和邻二甲苯氧化的催化活性","authors":"","doi":"10.1016/j.seppur.2024.129911","DOIUrl":null,"url":null,"abstract":"<div><div>Cobalt-based catalysts are the most promising catalysts for the catalytic oxidation of volatile organic compounds (VOCs). Metal doping is considered to be a valuable strategy to improve the catalytic activity of metal oxide catalysts. Here, a small amount of Sm doped Sm<sub>y</sub>CoO<sub>x</sub> spinel oxides with walnut-like shape were successfully prepared by solvothermal method and applied for oxidation of toluene and o-xylene. Their physiochemical properties were studied by various characterization, DFT calculation and in situ DRIFIS tests. Sm<sub>0.09</sub>CoO<sub>x</sub> substituted by Sm at six-coordination cobalt shows the best oxidation ability on toluene (T<sub>90</sub> = 228 °C) and o-xylene (T<sub>90</sub> = 268 °C). This is because doping Sm in Co<sub>3</sub>O<sub>4</sub> causes the lattice distortion, and generates Sm-O-Co bonds to weaken the bond energy of Co-O bonds, thus inducing the generation of active oxygen by improving the mobility of lattice oxygen. These results are of great significance for constructing metal–oxygen bonds through metal-doped cobalt oxide catalysts to improve catalytic performance.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1000,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Promoting the catalytic activity of SmyCoOx on oxidation of toluene and o-xylene by Sm doped Co3O4 to weaken the Co–O bonds\",\"authors\":\"\",\"doi\":\"10.1016/j.seppur.2024.129911\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Cobalt-based catalysts are the most promising catalysts for the catalytic oxidation of volatile organic compounds (VOCs). Metal doping is considered to be a valuable strategy to improve the catalytic activity of metal oxide catalysts. Here, a small amount of Sm doped Sm<sub>y</sub>CoO<sub>x</sub> spinel oxides with walnut-like shape were successfully prepared by solvothermal method and applied for oxidation of toluene and o-xylene. Their physiochemical properties were studied by various characterization, DFT calculation and in situ DRIFIS tests. Sm<sub>0.09</sub>CoO<sub>x</sub> substituted by Sm at six-coordination cobalt shows the best oxidation ability on toluene (T<sub>90</sub> = 228 °C) and o-xylene (T<sub>90</sub> = 268 °C). This is because doping Sm in Co<sub>3</sub>O<sub>4</sub> causes the lattice distortion, and generates Sm-O-Co bonds to weaken the bond energy of Co-O bonds, thus inducing the generation of active oxygen by improving the mobility of lattice oxygen. These results are of great significance for constructing metal–oxygen bonds through metal-doped cobalt oxide catalysts to improve catalytic performance.</div></div>\",\"PeriodicalId\":427,\"journal\":{\"name\":\"Separation and Purification Technology\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":8.1000,\"publicationDate\":\"2024-09-27\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Separation and Purification Technology\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1383586624036505\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Separation and Purification Technology","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1383586624036505","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
摘要
钴基催化剂是催化氧化挥发性有机化合物 (VOC) 的最有前途的催化剂。金属掺杂被认为是提高金属氧化物催化剂催化活性的重要策略。本文采用溶热法成功制备了少量掺杂 Sm 的核桃状 SmyCoOx 尖晶石氧化物,并将其用于甲苯和邻二甲苯的氧化。通过各种表征、DFT 计算和原位 DRIFIS 试验研究了它们的理化性质。由 Sm 取代六配位钴的 Sm0.09CoOx 对甲苯(T90 = 228 ℃)和邻二甲苯(T90 = 268 ℃)的氧化能力最佳。这是因为在 Co3O4 中掺杂 Sm 会导致晶格畸变,并生成 Sm-O-Co 键,削弱 Co-O 键的键能,从而通过提高晶格氧的流动性来诱导活性氧的生成。这些结果对于通过金属掺杂氧化钴催化剂构建金属氧键以提高催化性能具有重要意义。
Promoting the catalytic activity of SmyCoOx on oxidation of toluene and o-xylene by Sm doped Co3O4 to weaken the Co–O bonds
Cobalt-based catalysts are the most promising catalysts for the catalytic oxidation of volatile organic compounds (VOCs). Metal doping is considered to be a valuable strategy to improve the catalytic activity of metal oxide catalysts. Here, a small amount of Sm doped SmyCoOx spinel oxides with walnut-like shape were successfully prepared by solvothermal method and applied for oxidation of toluene and o-xylene. Their physiochemical properties were studied by various characterization, DFT calculation and in situ DRIFIS tests. Sm0.09CoOx substituted by Sm at six-coordination cobalt shows the best oxidation ability on toluene (T90 = 228 °C) and o-xylene (T90 = 268 °C). This is because doping Sm in Co3O4 causes the lattice distortion, and generates Sm-O-Co bonds to weaken the bond energy of Co-O bonds, thus inducing the generation of active oxygen by improving the mobility of lattice oxygen. These results are of great significance for constructing metal–oxygen bonds through metal-doped cobalt oxide catalysts to improve catalytic performance.
期刊介绍:
Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.