{"title":"促进氧活化和 H2S 选择性氧化的 La2FeMO6 双包晶石中的不对称氧空位","authors":"","doi":"10.1016/S1872-2067(24)60051-3","DOIUrl":null,"url":null,"abstract":"<div><p>Tuning oxygen vacancy (V<sub>O</sub>) in metal oxides catalysts that efficiently activates O<sub>2</sub> molecule to promote oxidation reactions remains challenging. Herein, transition metal (M = Mn, Co, and Mo) doping was used to moderate the coordination environment of V<sub>O</sub> in La<sub>2</sub>FeMO<sub>6</sub> and promote activity for selective oxidation of hydrogen sulfide (H<sub>2</sub>S). Various techniques reveal that the introduction of Mn and Co forms the homogeneous double perovskite phase, which results in the formation of asymmetric V<sub>O</sub>. Although these asymmetric V<sub>O</sub> are more difficult to form than symmetric Fe-V<sub>O</sub>-Fe due to the shorter bond distance and stronger bond strength of Fe-O, they are more conducive to the dissociation of O<sub>2</sub> molecules. Among them, the formed rich Fe-V<sub>O</sub>-Mn sites from the alternate substitution of Mn to Fe boosted the activation of O<sub>2</sub> molecules of Mn-substituted LaFeO<sub>3</sub>. Therefore, enhanced catalytic activity and outstanding sulfur selectivity were achieved as a result of promoted oxygen mobility and reducibility. This work provides an attractive strategy for rational design of advanced oxidation catalysts.</p></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":null,"pages":null},"PeriodicalIF":15.7000,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Asymmetric oxygen vacancies in La2FeMO6 double perovskite for boosting oxygen activation and H2S selective oxidation\",\"authors\":\"\",\"doi\":\"10.1016/S1872-2067(24)60051-3\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Tuning oxygen vacancy (V<sub>O</sub>) in metal oxides catalysts that efficiently activates O<sub>2</sub> molecule to promote oxidation reactions remains challenging. Herein, transition metal (M = Mn, Co, and Mo) doping was used to moderate the coordination environment of V<sub>O</sub> in La<sub>2</sub>FeMO<sub>6</sub> and promote activity for selective oxidation of hydrogen sulfide (H<sub>2</sub>S). Various techniques reveal that the introduction of Mn and Co forms the homogeneous double perovskite phase, which results in the formation of asymmetric V<sub>O</sub>. Although these asymmetric V<sub>O</sub> are more difficult to form than symmetric Fe-V<sub>O</sub>-Fe due to the shorter bond distance and stronger bond strength of Fe-O, they are more conducive to the dissociation of O<sub>2</sub> molecules. Among them, the formed rich Fe-V<sub>O</sub>-Mn sites from the alternate substitution of Mn to Fe boosted the activation of O<sub>2</sub> molecules of Mn-substituted LaFeO<sub>3</sub>. Therefore, enhanced catalytic activity and outstanding sulfur selectivity were achieved as a result of promoted oxygen mobility and reducibility. This work provides an attractive strategy for rational design of advanced oxidation catalysts.</p></div>\",\"PeriodicalId\":9832,\"journal\":{\"name\":\"Chinese Journal of Catalysis\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":15.7000,\"publicationDate\":\"2024-07-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chinese Journal of Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1872206724600513\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chinese Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1872206724600513","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
引用次数: 0
摘要
调节金属氧化物催化剂中的氧空位(VO)以有效激活 O2 分子从而促进氧化反应仍然是一项挑战。在这里,过渡金属(M = 锰、钴和钼)的掺杂被用来调节 La2FeMO6 中 VO 的配位环境,并提高硫化氢(H2S)选择性氧化的活性。各种技术表明,锰和钴的引入形成了均匀的双包晶相,从而形成了不对称的 VO。虽然由于 Fe-O 的键距较短且键强度较强,这些不对称 VO 比对称的 Fe-VO-Fe 更难形成,但它们更有利于 O2 分子的解离。其中,锰与铁交替取代形成的富Fe-VO-Mn位点促进了锰取代LaFeO3对O2分子的活化。因此,由于促进了氧的流动性和还原性,催化活性得到了增强,硫的选择性也更加突出。这项工作为合理设计高级氧化催化剂提供了一种有吸引力的策略。
Asymmetric oxygen vacancies in La2FeMO6 double perovskite for boosting oxygen activation and H2S selective oxidation
Tuning oxygen vacancy (VO) in metal oxides catalysts that efficiently activates O2 molecule to promote oxidation reactions remains challenging. Herein, transition metal (M = Mn, Co, and Mo) doping was used to moderate the coordination environment of VO in La2FeMO6 and promote activity for selective oxidation of hydrogen sulfide (H2S). Various techniques reveal that the introduction of Mn and Co forms the homogeneous double perovskite phase, which results in the formation of asymmetric VO. Although these asymmetric VO are more difficult to form than symmetric Fe-VO-Fe due to the shorter bond distance and stronger bond strength of Fe-O, they are more conducive to the dissociation of O2 molecules. Among them, the formed rich Fe-VO-Mn sites from the alternate substitution of Mn to Fe boosted the activation of O2 molecules of Mn-substituted LaFeO3. Therefore, enhanced catalytic activity and outstanding sulfur selectivity were achieved as a result of promoted oxygen mobility and reducibility. This work provides an attractive strategy for rational design of advanced oxidation catalysts.
期刊介绍:
The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.