{"title":"化学循环燃烧铜矿氧载体的动力学研究","authors":"Xin Tian, Mingze Su, Haibo Zhao","doi":"10.3390/fire7070245","DOIUrl":null,"url":null,"abstract":"Chemical looping combustion (CLC) has been validated as one of the most promising technologies for fossil fuel combustion, which can produce high-purity CO2 streams ready for capture and sequestration in power production. The selection of an appropriate oxygen carrier is one of the most important issues for the CLC process, and the reduction kinetics investigation of the oxygen carrier with fuel gas can provide the basis for CLC reactor design and simulation optimization. In this study, copper ore was chosen as an oxygen carrier, and the oxygen release property of copper ore under a nitrogen environment at various temperatures (1073–1193 K) was first investigated in a thermogravimetric analyzer (TGA). Subsequently, the reduction kinetics of copper ore with CO and H2 were evaluated by the TGA at temperatures ranging from 773 K to 1073 K, using a continuous stream of 5, 10, 15, 20, 25, and 30 vol. % of CO or H2 balanced by CO2 or N2. It was found that the reaction rates of these reactions accelerated with the increase in temperature and fuel gas concentration in inlet gas. Both the oxygen release process of copper ore and the reduction process of copper ore with reducing gases can be described by the unreacted shrinking core model (USCM). The reaction mechanism function for the oxygen-releasing and reduction process of copper ore oxygen carrier was varied. The activation energy of the oxygen-releasing process, reduction process with CO, and reduction process with H2 were calculated as 99.35, 5.08, and 4.28 kJ/mol, respectively. The pre-exponential factor ranged from 1.96 × 10−1 to 1.84 × 103. The reaction order depended on the fuel gas, which was 1 and 0.86, respectively, for reaction with CO and H2.","PeriodicalId":508952,"journal":{"name":"Fire","volume":"11 3","pages":""},"PeriodicalIF":0.0000,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Kinetics Investigation of Copper Ore Oxygen Carrier for Chemical Looping Combustion\",\"authors\":\"Xin Tian, Mingze Su, Haibo Zhao\",\"doi\":\"10.3390/fire7070245\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Chemical looping combustion (CLC) has been validated as one of the most promising technologies for fossil fuel combustion, which can produce high-purity CO2 streams ready for capture and sequestration in power production. The selection of an appropriate oxygen carrier is one of the most important issues for the CLC process, and the reduction kinetics investigation of the oxygen carrier with fuel gas can provide the basis for CLC reactor design and simulation optimization. In this study, copper ore was chosen as an oxygen carrier, and the oxygen release property of copper ore under a nitrogen environment at various temperatures (1073–1193 K) was first investigated in a thermogravimetric analyzer (TGA). Subsequently, the reduction kinetics of copper ore with CO and H2 were evaluated by the TGA at temperatures ranging from 773 K to 1073 K, using a continuous stream of 5, 10, 15, 20, 25, and 30 vol. % of CO or H2 balanced by CO2 or N2. It was found that the reaction rates of these reactions accelerated with the increase in temperature and fuel gas concentration in inlet gas. Both the oxygen release process of copper ore and the reduction process of copper ore with reducing gases can be described by the unreacted shrinking core model (USCM). The reaction mechanism function for the oxygen-releasing and reduction process of copper ore oxygen carrier was varied. The activation energy of the oxygen-releasing process, reduction process with CO, and reduction process with H2 were calculated as 99.35, 5.08, and 4.28 kJ/mol, respectively. The pre-exponential factor ranged from 1.96 × 10−1 to 1.84 × 103. The reaction order depended on the fuel gas, which was 1 and 0.86, respectively, for reaction with CO and H2.\",\"PeriodicalId\":508952,\"journal\":{\"name\":\"Fire\",\"volume\":\"11 3\",\"pages\":\"\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2024-07-12\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Fire\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/10.3390/fire7070245\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Fire","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.3390/fire7070245","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
引用次数: 0
摘要
化学循环燃烧(CLC)已被证实是化石燃料燃烧中最有前途的技术之一,它可以产生高纯度的二氧化碳流,并可在发电过程中进行捕集和封存。选择合适的氧载体是 CLC 过程中最重要的问题之一,而氧载体与燃料气体的还原动力学研究可为 CLC 反应器的设计和模拟优化提供依据。本研究选择铜矿石作为氧载体,首先在热重分析仪(TGA)上研究了铜矿石在不同温度(1073-1193 K)氮气环境下的氧释放特性。随后,在 773 K 至 1073 K 的温度范围内,使用连续流 5、10、15、20、25 和 30 体积百分比的 CO 或 H2(由 CO2 或 N2 平衡),通过 TGA 评估了铜矿与 CO 和 H2 的还原动力学。研究发现,这些反应的反应速率随着温度和入口气体中燃料气体浓度的增加而加快。铜矿的释氧过程和铜矿与还原性气体的还原过程都可以用未反应收缩核心模型(USCM)来描述。铜矿氧载体释氧和还原过程的反应机理函数是变化的。计算得出氧释放过程、与 CO 的还原过程和与 H2 的还原过程的活化能分别为 99.35、5.08 和 4.28 kJ/mol。预指数范围为 1.96 × 10-1 至 1.84 × 103。反应顺序取决于燃料气体,与 CO 和 H2 反应的顺序分别为 1 和 0.86。
Kinetics Investigation of Copper Ore Oxygen Carrier for Chemical Looping Combustion
Chemical looping combustion (CLC) has been validated as one of the most promising technologies for fossil fuel combustion, which can produce high-purity CO2 streams ready for capture and sequestration in power production. The selection of an appropriate oxygen carrier is one of the most important issues for the CLC process, and the reduction kinetics investigation of the oxygen carrier with fuel gas can provide the basis for CLC reactor design and simulation optimization. In this study, copper ore was chosen as an oxygen carrier, and the oxygen release property of copper ore under a nitrogen environment at various temperatures (1073–1193 K) was first investigated in a thermogravimetric analyzer (TGA). Subsequently, the reduction kinetics of copper ore with CO and H2 were evaluated by the TGA at temperatures ranging from 773 K to 1073 K, using a continuous stream of 5, 10, 15, 20, 25, and 30 vol. % of CO or H2 balanced by CO2 or N2. It was found that the reaction rates of these reactions accelerated with the increase in temperature and fuel gas concentration in inlet gas. Both the oxygen release process of copper ore and the reduction process of copper ore with reducing gases can be described by the unreacted shrinking core model (USCM). The reaction mechanism function for the oxygen-releasing and reduction process of copper ore oxygen carrier was varied. The activation energy of the oxygen-releasing process, reduction process with CO, and reduction process with H2 were calculated as 99.35, 5.08, and 4.28 kJ/mol, respectively. The pre-exponential factor ranged from 1.96 × 10−1 to 1.84 × 103. The reaction order depended on the fuel gas, which was 1 and 0.86, respectively, for reaction with CO and H2.