{"title":"用于二氧化碳辅助乙烷脱氢的掺嘎尖晶石型 Co-Al 催化剂","authors":"Shuyang Xu, Weiming Hua, Yinghong Yue, Zi Gao","doi":"10.1016/j.apcata.2024.119959","DOIUrl":null,"url":null,"abstract":"<div><p>A series of Ga-doped spinel-typed Co-Al catalysts were prepared via one-step evaporation-induced self-assembly (EISA) method. These catalysts present promising catalytic performance for CO<sub>2</sub>-assisted ethane dehydrogenation, which can be ascribed to the conjunction effect of cobalt and gallium species. The incorporation of Ga into the structure of Co-Al spinel has been recognized for enhancing CO<sub>2</sub> conversion via reverse water-gas shift reaction, leading to a favorable equilibrium shift towards ethylene, along with an improved catalyst stability as a result of coexisting Boudouard reaction. Through X-ray photoelectron spectroscopy (XPS), X-ray absorption fine structure (XAFS), NH<sub>3</sub> and CO<sub>2</sub> temperature-programmed desorption (TPD) characterizations, coordinatively unsaturated Co<sup>2+</sup> and Ga<sup>3+</sup> cations were identified as collaborative catalytic active sites, with gallium species taking the prominent role. These sites were closely associated with the formation of acid-base pairs on the catalyst surface, which were crucial for the adsorption and activation of the reactants.</p></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":null,"pages":null},"PeriodicalIF":4.7000,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Ga-doped spinel-typed Co-Al catalysts for CO2-assisted ethane dehydrogenation\",\"authors\":\"Shuyang Xu, Weiming Hua, Yinghong Yue, Zi Gao\",\"doi\":\"10.1016/j.apcata.2024.119959\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>A series of Ga-doped spinel-typed Co-Al catalysts were prepared via one-step evaporation-induced self-assembly (EISA) method. These catalysts present promising catalytic performance for CO<sub>2</sub>-assisted ethane dehydrogenation, which can be ascribed to the conjunction effect of cobalt and gallium species. The incorporation of Ga into the structure of Co-Al spinel has been recognized for enhancing CO<sub>2</sub> conversion via reverse water-gas shift reaction, leading to a favorable equilibrium shift towards ethylene, along with an improved catalyst stability as a result of coexisting Boudouard reaction. Through X-ray photoelectron spectroscopy (XPS), X-ray absorption fine structure (XAFS), NH<sub>3</sub> and CO<sub>2</sub> temperature-programmed desorption (TPD) characterizations, coordinatively unsaturated Co<sup>2+</sup> and Ga<sup>3+</sup> cations were identified as collaborative catalytic active sites, with gallium species taking the prominent role. These sites were closely associated with the formation of acid-base pairs on the catalyst surface, which were crucial for the adsorption and activation of the reactants.</p></div>\",\"PeriodicalId\":243,\"journal\":{\"name\":\"Applied Catalysis A: General\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":4.7000,\"publicationDate\":\"2024-09-12\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Catalysis A: General\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0926860X24004046\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Catalysis A: General","FirstCategoryId":"1","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0926860X24004046","RegionNum":2,"RegionCategory":"化学","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
通过一步蒸发诱导自组装(EISA)法制备了一系列掺镓尖晶石型 Co-Al 催化剂。这些催化剂在二氧化碳辅助的乙烷脱氢反应中表现出良好的催化性能,这可归因于钴和镓物种的结合效应。在 Co-Al 尖晶石结构中加入镓已被公认为能通过反向水气变换反应提高二氧化碳的转化率,从而导致向乙烯的有利平衡转变,同时由于共存的布杜尔反应,催化剂的稳定性也得到了提高。通过 X 射线光电子能谱 (XPS)、X 射线吸收精细结构 (XAFS)、NH3 和 CO2 温度编程解吸 (TPD) 表征,确定了配位不饱和 Co2+ 和 Ga3+ 阳离子为协同催化活性位点,其中镓物种起着突出作用。这些位点与催化剂表面酸碱对的形成密切相关,对反应物的吸附和活化至关重要。
Ga-doped spinel-typed Co-Al catalysts for CO2-assisted ethane dehydrogenation
A series of Ga-doped spinel-typed Co-Al catalysts were prepared via one-step evaporation-induced self-assembly (EISA) method. These catalysts present promising catalytic performance for CO2-assisted ethane dehydrogenation, which can be ascribed to the conjunction effect of cobalt and gallium species. The incorporation of Ga into the structure of Co-Al spinel has been recognized for enhancing CO2 conversion via reverse water-gas shift reaction, leading to a favorable equilibrium shift towards ethylene, along with an improved catalyst stability as a result of coexisting Boudouard reaction. Through X-ray photoelectron spectroscopy (XPS), X-ray absorption fine structure (XAFS), NH3 and CO2 temperature-programmed desorption (TPD) characterizations, coordinatively unsaturated Co2+ and Ga3+ cations were identified as collaborative catalytic active sites, with gallium species taking the prominent role. These sites were closely associated with the formation of acid-base pairs on the catalyst surface, which were crucial for the adsorption and activation of the reactants.
期刊介绍:
Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications.
Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.