Liang Xiaocen , Wang Xuemei , Xing Zifan , Mao Min , Song Da , Li Yang , Long Tao , Zhou Yuchao , Chen Peili , He Fang
{"title":"MgX2O4（X=铬、铁、锰）尖晶石的 B 位阳离子对乙烷氧化脱氢成乙烯的化学循环的影响","authors":"Liang Xiaocen , Wang Xuemei , Xing Zifan , Mao Min , Song Da , Li Yang , Long Tao , Zhou Yuchao , Chen Peili , He Fang","doi":"10.1016/S1872-5813(24)60434-2","DOIUrl":null,"url":null,"abstract":"<div><p>Chemical looping oxidative dehydrogenation (CL-ODH) provides a multifunctional conversion platform that can take advantage of the selective oxidation of lattice oxygen in oxygen carrier to achieve high-valued ethane to ethylene conversion. In this study, we explored the effect of B-site element in MgX<sub>2</sub>O<sub>4</sub> (X=Cr, Fe, or Mn) spinel-type oxygen carriers on the performance of ethane CL-ODH. The properties test and characterization of MgX<sub>2</sub>O<sub>4</sub> spinel were tested by fixed bed and H<sub>2</sub>-TPR, O<sub>2</sub>-TPD, TG, <em>in-situ</em> Raman, SEM, and TEM. The results showed that because MgCr<sub>2</sub>O<sub>4</sub> only released a small amount of adsorbed surface oxygen, it tended to catalyze the conversion of ethane to coke and hydrogen. MgFe<sub>2</sub>O<sub>4</sub> facilitated the deep oxidation of ethane into CO<sub>2</sub> by providing more surface lattice oxygen. Meanwhile, since a significant amount of bulk lattice oxygen was released by the MgMn<sub>2</sub>O<sub>4</sub> oxygen carrier, it could burn hydrogen in a targeted manner to advance the reaction and increased ethylene’s selectivity. Thereby, MgMn<sub>2</sub>O<sub>4</sub> achieved an ethane conversion of 73.72% with an ethylene selectivity of 81.46%. Furthermore, the MgMn<sub>2</sub>O<sub>4</sub> catalyst demonstrated stable reactivity and an ethylene yield of about 62.00% in ethane CL-ODH over the 30 redox cycles. The screening tests indicated that the B-site elements in MgX<sub>2</sub>O<sub>4</sub> spinel oxides could significantly influence their ability to supply lattice oxygen, thereby affecting their performance in ethane CL-ODH reaction.</p></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":null,"pages":null},"PeriodicalIF":0.0000,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Impact of B-site cations of MgX2O4 (X=Cr, Fe, Mn) spinels on the chemical looping oxidative dehydrogenation of ethane to ethylene\",\"authors\":\"Liang Xiaocen , Wang Xuemei , Xing Zifan , Mao Min , Song Da , Li Yang , Long Tao , Zhou Yuchao , Chen Peili , He Fang\",\"doi\":\"10.1016/S1872-5813(24)60434-2\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Chemical looping oxidative dehydrogenation (CL-ODH) provides a multifunctional conversion platform that can take advantage of the selective oxidation of lattice oxygen in oxygen carrier to achieve high-valued ethane to ethylene conversion. In this study, we explored the effect of B-site element in MgX<sub>2</sub>O<sub>4</sub> (X=Cr, Fe, or Mn) spinel-type oxygen carriers on the performance of ethane CL-ODH. The properties test and characterization of MgX<sub>2</sub>O<sub>4</sub> spinel were tested by fixed bed and H<sub>2</sub>-TPR, O<sub>2</sub>-TPD, TG, <em>in-situ</em> Raman, SEM, and TEM. The results showed that because MgCr<sub>2</sub>O<sub>4</sub> only released a small amount of adsorbed surface oxygen, it tended to catalyze the conversion of ethane to coke and hydrogen. MgFe<sub>2</sub>O<sub>4</sub> facilitated the deep oxidation of ethane into CO<sub>2</sub> by providing more surface lattice oxygen. Meanwhile, since a significant amount of bulk lattice oxygen was released by the MgMn<sub>2</sub>O<sub>4</sub> oxygen carrier, it could burn hydrogen in a targeted manner to advance the reaction and increased ethylene’s selectivity. Thereby, MgMn<sub>2</sub>O<sub>4</sub> achieved an ethane conversion of 73.72% with an ethylene selectivity of 81.46%. Furthermore, the MgMn<sub>2</sub>O<sub>4</sub> catalyst demonstrated stable reactivity and an ethylene yield of about 62.00% in ethane CL-ODH over the 30 redox cycles. The screening tests indicated that the B-site elements in MgX<sub>2</sub>O<sub>4</sub> spinel oxides could significantly influence their ability to supply lattice oxygen, thereby affecting their performance in ethane CL-ODH reaction.</p></div>\",\"PeriodicalId\":15956,\"journal\":{\"name\":\"燃料化学学报\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2024-07-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"燃料化学学报\",\"FirstCategoryId\":\"1087\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1872581324604342\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"Energy\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"燃料化学学报","FirstCategoryId":"1087","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1872581324604342","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"Energy","Score":null,"Total":0}
Impact of B-site cations of MgX2O4 (X=Cr, Fe, Mn) spinels on the chemical looping oxidative dehydrogenation of ethane to ethylene
Chemical looping oxidative dehydrogenation (CL-ODH) provides a multifunctional conversion platform that can take advantage of the selective oxidation of lattice oxygen in oxygen carrier to achieve high-valued ethane to ethylene conversion. In this study, we explored the effect of B-site element in MgX2O4 (X=Cr, Fe, or Mn) spinel-type oxygen carriers on the performance of ethane CL-ODH. The properties test and characterization of MgX2O4 spinel were tested by fixed bed and H2-TPR, O2-TPD, TG, in-situ Raman, SEM, and TEM. The results showed that because MgCr2O4 only released a small amount of adsorbed surface oxygen, it tended to catalyze the conversion of ethane to coke and hydrogen. MgFe2O4 facilitated the deep oxidation of ethane into CO2 by providing more surface lattice oxygen. Meanwhile, since a significant amount of bulk lattice oxygen was released by the MgMn2O4 oxygen carrier, it could burn hydrogen in a targeted manner to advance the reaction and increased ethylene’s selectivity. Thereby, MgMn2O4 achieved an ethane conversion of 73.72% with an ethylene selectivity of 81.46%. Furthermore, the MgMn2O4 catalyst demonstrated stable reactivity and an ethylene yield of about 62.00% in ethane CL-ODH over the 30 redox cycles. The screening tests indicated that the B-site elements in MgX2O4 spinel oxides could significantly influence their ability to supply lattice oxygen, thereby affecting their performance in ethane CL-ODH reaction.
期刊介绍：
Journal of Fuel Chemistry and Technology (Ranliao Huaxue Xuebao) is a Chinese Academy of Sciences(CAS) journal started in 1956, sponsored by the Chinese Chemical Society and the Institute of Coal Chemistry, Chinese Academy of Sciences(CAS). The journal is published bimonthly by Science Press in China and widely distributed in about 20 countries. Journal of Fuel Chemistry and Technology publishes reports of both basic and applied research in the chemistry and chemical engineering of many energy sources, including that involved in the nature, processing and utilization of coal, petroleum, oil shale, natural gas, biomass and synfuels, as well as related subjects of increasing interest such as C1 chemistry, pollutions control and new catalytic materials. Types of publications include original research articles, short communications, research notes and reviews. Both domestic and international contributors are welcome. Manuscripts written in Chinese or English will be accepted. Additional English titles, abstracts and key words should be included in Chinese manuscripts. All manuscripts are subject to critical review by the editorial committee, which is composed of about 10 foreign and 50 Chinese experts in fuel science. Journal of Fuel Chemistry and Technology has been a source of primary research work in fuel chemistry as a Chinese core scientific periodical.
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