{"title":"有机配体和光活性物质对衍生自 MOFs 的 Co3O4@MnOx 空心球结构在丙酮和 NO 的高效能量传递和光热催化中的影响","authors":"","doi":"10.1016/j.surfin.2024.105135","DOIUrl":null,"url":null,"abstract":"<div><p>A set of MOFs-derived Co<sub>3</sub>O<sub>4</sub>@MnO<sub>x</sub> hollow-sphere were synthesized to develop a catalyst for the photothermal catalytic removal of NO using acetone as a reducing agent. The study systematically investigated the impact of organic ligands and photoactive substances on energy transfer and photothermocatalytic reactions involving acetone and NO under 5 vol % H<sub>2</sub>O with the catalysts. At 240°C, sample C-5/1 (with an organic ligand added and Co/Mn molar ratio of 5/1) demonstrated 75 % NO conversion and 65 % acetone conversion. The highest catalytic performance was observed in the L-Py sample (with photoactive substance was added), achieving 80 % NO and 69 % acetone conversion at 240°C. The catalyst demonstrated low crystallinity, and the introduction structural defects through ligands adjusted the ratio of active components. Meanwhile, enhanced catalytic performance was attributed to light energy scattering in the inner space of microspheres, resulting in the efficient transfer of 2.17 eV energy with the addition of two photoactive substances. The elevated concentration of surface-active oxygen facilitated oxidation, while M<sup>n</sup>/M<sup>n+1</sup> (Mn<sup>3+</sup>/Mn<sup>4+</sup> and Co<sup>2+</sup>/Co<sup>3+</sup>) redox cycling supplied surface oxygen in the photothermal low-temperature response. The proposed mechanism for the simultaneous degradation of acetone and NO was elucidated using Density Functional Theory calculations.</p></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":null,"pages":null},"PeriodicalIF":5.7000,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Effects of organic ligands and photoactive substances on MOFs-derived Co3O4@MnOx hollow-sphere structure for efficient energy transfer and photothermocatalysis of acetone and NO\",\"authors\":\"\",\"doi\":\"10.1016/j.surfin.2024.105135\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>A set of MOFs-derived Co<sub>3</sub>O<sub>4</sub>@MnO<sub>x</sub> hollow-sphere were synthesized to develop a catalyst for the photothermal catalytic removal of NO using acetone as a reducing agent. The study systematically investigated the impact of organic ligands and photoactive substances on energy transfer and photothermocatalytic reactions involving acetone and NO under 5 vol % H<sub>2</sub>O with the catalysts. At 240°C, sample C-5/1 (with an organic ligand added and Co/Mn molar ratio of 5/1) demonstrated 75 % NO conversion and 65 % acetone conversion. The highest catalytic performance was observed in the L-Py sample (with photoactive substance was added), achieving 80 % NO and 69 % acetone conversion at 240°C. The catalyst demonstrated low crystallinity, and the introduction structural defects through ligands adjusted the ratio of active components. Meanwhile, enhanced catalytic performance was attributed to light energy scattering in the inner space of microspheres, resulting in the efficient transfer of 2.17 eV energy with the addition of two photoactive substances. The elevated concentration of surface-active oxygen facilitated oxidation, while M<sup>n</sup>/M<sup>n+1</sup> (Mn<sup>3+</sup>/Mn<sup>4+</sup> and Co<sup>2+</sup>/Co<sup>3+</sup>) redox cycling supplied surface oxygen in the photothermal low-temperature response. The proposed mechanism for the simultaneous degradation of acetone and NO was elucidated using Density Functional Theory calculations.</p></div>\",\"PeriodicalId\":22081,\"journal\":{\"name\":\"Surfaces and Interfaces\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.7000,\"publicationDate\":\"2024-09-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Surfaces and Interfaces\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2468023024012914\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Surfaces and Interfaces","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2468023024012914","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
研究人员合成了一组由 MOFs 衍生的 Co3O4@MnOx 空心球,用于开发一种以丙酮为还原剂光热催化去除 NO 的催化剂。研究系统地考察了有机配体和光活性物质对能量传递的影响,以及催化剂在 5 vol % H2O 条件下与丙酮和 NO 发生的光热催化反应。240°C 时,样品 C-5/1(添加了有机配体,Co/Mn 摩尔比为 5/1)的 NO 转化率为 75%,丙酮转化率为 65%。催化性能最高的是 L-Py 样品(添加了光活性物质),在 240°C 时实现了 80% 的氮氧化物转化率和 69% 的丙酮转化率。催化剂的结晶度较低,通过配体引入结构缺陷调整了活性成分的比例。同时,催化性能的增强归因于微球内部空间的光能散射,在添加两种光活性物质后,2.17 eV 的能量得以有效传递。表面活性氧浓度的升高促进了氧化,而 Mn/Mn+1(Mn3+/Mn4+ 和 Co2+/Co3+)氧化还原循环则在光热低温反应中提供了表面氧。密度泛函理论计算阐明了丙酮和 NO 同时降解的机理。
Effects of organic ligands and photoactive substances on MOFs-derived Co3O4@MnOx hollow-sphere structure for efficient energy transfer and photothermocatalysis of acetone and NO
A set of MOFs-derived Co3O4@MnOx hollow-sphere were synthesized to develop a catalyst for the photothermal catalytic removal of NO using acetone as a reducing agent. The study systematically investigated the impact of organic ligands and photoactive substances on energy transfer and photothermocatalytic reactions involving acetone and NO under 5 vol % H2O with the catalysts. At 240°C, sample C-5/1 (with an organic ligand added and Co/Mn molar ratio of 5/1) demonstrated 75 % NO conversion and 65 % acetone conversion. The highest catalytic performance was observed in the L-Py sample (with photoactive substance was added), achieving 80 % NO and 69 % acetone conversion at 240°C. The catalyst demonstrated low crystallinity, and the introduction structural defects through ligands adjusted the ratio of active components. Meanwhile, enhanced catalytic performance was attributed to light energy scattering in the inner space of microspheres, resulting in the efficient transfer of 2.17 eV energy with the addition of two photoactive substances. The elevated concentration of surface-active oxygen facilitated oxidation, while Mn/Mn+1 (Mn3+/Mn4+ and Co2+/Co3+) redox cycling supplied surface oxygen in the photothermal low-temperature response. The proposed mechanism for the simultaneous degradation of acetone and NO was elucidated using Density Functional Theory calculations.
期刊介绍:
The aim of the journal is to provide a respectful outlet for ''sound science'' papers in all research areas on surfaces and interfaces. We define sound science papers as papers that describe new and well-executed research, but that do not necessarily provide brand new insights or are merely a description of research results.
Surfaces and Interfaces publishes research papers in all fields of surface science which may not always find the right home on first submission to our Elsevier sister journals (Applied Surface, Surface and Coatings Technology, Thin Solid Films)