Shaokai Cheng , Wenbo Li , Hong Peng , Yuexin Han , Peng Gao , Yongsheng Sun
{"title":"Ce7O12在还原气氛中的还原行为和动力学:来自H2和CO比较的见解","authors":"Shaokai Cheng , Wenbo Li , Hong Peng , Yuexin Han , Peng Gao , Yongsheng Sun","doi":"10.1016/j.ces.2025.122060","DOIUrl":null,"url":null,"abstract":"<div><div>Enhancing separation of iron and rare earths by staged roasting was proposed, with a pilot-scale experiment conducted. However, the reaction of bastnaesite pyrolysis product (Ce<sub>7</sub>O<sub>12</sub>) in reduction roasting stage is rarely reported. This study explored reduction of Ce<sub>7</sub>O<sub>12</sub> under H<sub>2</sub> and CO using thermogravimetry, and analyzed the non-isothermal reaction kinetics. The results indicated that the unique Ce/O induced by lattice defects enabled Ce<sub>7</sub>O<sub>12</sub> to react with reducing gases. The weight loss during H<sub>2</sub> and CO reduction was 2.8 % and 2.5 %, with the detection of H<sub>2</sub>O and CO<sub>2</sub>. The optimal reaction model for H<sub>2</sub> reduction was shrinking core model (<em>m</em> = 1/2), while that for CO reduction was chemical reaction model (<em>n</em> = 3/2). During the reduction process, the CO reduction started at a lower temperature than the H<sub>2</sub> reduction, and the reaction was more intense. After reduction, the XRD peaks shifted to lower angles, the lattice spacing increased, and the Ce oxidation degree decreased, implying the transition of Ce<sup>4+</sup> to Ce<sup>3+</sup>. The reduction products exhibited a decrease in specific surface area and total pore volume, while the pore diameter increased.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"318 ","pages":"Article 122060"},"PeriodicalIF":4.3000,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Reduction behavior and kinetics of Ce7O12 in reducing atmospheres: Insights from the comparison of H2 and CO\",\"authors\":\"Shaokai Cheng , Wenbo Li , Hong Peng , Yuexin Han , Peng Gao , Yongsheng Sun\",\"doi\":\"10.1016/j.ces.2025.122060\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Enhancing separation of iron and rare earths by staged roasting was proposed, with a pilot-scale experiment conducted. However, the reaction of bastnaesite pyrolysis product (Ce<sub>7</sub>O<sub>12</sub>) in reduction roasting stage is rarely reported. This study explored reduction of Ce<sub>7</sub>O<sub>12</sub> under H<sub>2</sub> and CO using thermogravimetry, and analyzed the non-isothermal reaction kinetics. The results indicated that the unique Ce/O induced by lattice defects enabled Ce<sub>7</sub>O<sub>12</sub> to react with reducing gases. The weight loss during H<sub>2</sub> and CO reduction was 2.8 % and 2.5 %, with the detection of H<sub>2</sub>O and CO<sub>2</sub>. The optimal reaction model for H<sub>2</sub> reduction was shrinking core model (<em>m</em> = 1/2), while that for CO reduction was chemical reaction model (<em>n</em> = 3/2). During the reduction process, the CO reduction started at a lower temperature than the H<sub>2</sub> reduction, and the reaction was more intense. After reduction, the XRD peaks shifted to lower angles, the lattice spacing increased, and the Ce oxidation degree decreased, implying the transition of Ce<sup>4+</sup> to Ce<sup>3+</sup>. The reduction products exhibited a decrease in specific surface area and total pore volume, while the pore diameter increased.</div></div>\",\"PeriodicalId\":271,\"journal\":{\"name\":\"Chemical Engineering Science\",\"volume\":\"318 \",\"pages\":\"Article 122060\"},\"PeriodicalIF\":4.3000,\"publicationDate\":\"2025-06-17\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemical Engineering Science\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0009250925008838\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Engineering Science","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0009250925008838","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Reduction behavior and kinetics of Ce7O12 in reducing atmospheres: Insights from the comparison of H2 and CO
Enhancing separation of iron and rare earths by staged roasting was proposed, with a pilot-scale experiment conducted. However, the reaction of bastnaesite pyrolysis product (Ce7O12) in reduction roasting stage is rarely reported. This study explored reduction of Ce7O12 under H2 and CO using thermogravimetry, and analyzed the non-isothermal reaction kinetics. The results indicated that the unique Ce/O induced by lattice defects enabled Ce7O12 to react with reducing gases. The weight loss during H2 and CO reduction was 2.8 % and 2.5 %, with the detection of H2O and CO2. The optimal reaction model for H2 reduction was shrinking core model (m = 1/2), while that for CO reduction was chemical reaction model (n = 3/2). During the reduction process, the CO reduction started at a lower temperature than the H2 reduction, and the reaction was more intense. After reduction, the XRD peaks shifted to lower angles, the lattice spacing increased, and the Ce oxidation degree decreased, implying the transition of Ce4+ to Ce3+. The reduction products exhibited a decrease in specific surface area and total pore volume, while the pore diameter increased.
期刊介绍:
Chemical engineering enables the transformation of natural resources and energy into useful products for society. It draws on and applies natural sciences, mathematics and economics, and has developed fundamental engineering science that underpins the discipline.
Chemical Engineering Science (CES) has been publishing papers on the fundamentals of chemical engineering since 1951. CES is the platform where the most significant advances in the discipline have ever since been published. Chemical Engineering Science has accompanied and sustained chemical engineering through its development into the vibrant and broad scientific discipline it is today.