Hongyu Pan, Mingrui Han*, Tianjun Zhang, Bingnan Ji, Mingyue Pan, Zefan Li and Shipeng Zhu,
{"title":"煤中 N2/CH4/CO2 竞争吸附的影响因素和吸附过程","authors":"Hongyu Pan, Mingrui Han*, Tianjun Zhang, Bingnan Ji, Mingyue Pan, Zefan Li and Shipeng Zhu, ","doi":"10.1021/acs.energyfuels.4c0436310.1021/acs.energyfuels.4c04363","DOIUrl":null,"url":null,"abstract":"<p >To investigate the influence of key factors (temperature, pressure, and particle size) on the competitive adsorption of N<sub>2</sub>/CH<sub>4</sub>/CO<sub>2</sub> on coal, a self-built multicomponent gas adsorption apparatus was used based on the breakthrough curve method to conduct competitive adsorption experiments under different conditions. The adsorption process was dynamically analyzed by combining adsorption kinetics models with the pore structure characteristics of the samples. The results showed that increasing the temperature promotes competitive adsorption and enhances the preferential adsorption of CO<sub>2</sub>, while increasing the pressure and particle size mesh number inhibits competitive adsorption and weakens the preferential adsorption of CO<sub>2</sub>. The experimental data fitted well with the Yoon-Nelson, Thomas, and Clark kinetic models, with <i>R</i><sup>2</sup> values all above 0.9. The mass transfer rate constants followed the order <i>k</i>(N<sub>2</sub>) > <i>k</i>(CH<sub>4</sub>) > <i>k</i>(CO<sub>2</sub>). As temperature and pressure increased or particle size mesh number increased, the <i>k</i> values for each component increased, enhancing the gas mass transfer rate. The adsorption capacities (<i>q</i><sub><i>T</i></sub>) and Clark constants (<i>A</i>) for each component showed the order CO<sub>2</sub> > CH<sub>4</sub> > N<sub>2</sub>, indicating that the coal samples had the highest adsorption capacity and strength for CO<sub>2</sub>, followed by CH<sub>4</sub> and then N<sub>2</sub>. Lowering the temperature, increasing the pressure, or increasing the particle size mesh number all led to increases in <i>q</i><sub><i>T</i></sub> and <i>A</i> for each component. The samples exhibited good pore connectivity, with the most developed micropores having a diameter of 2.05 nm, and relatively large specific surface area and pore volume. During competitive adsorption, N<sub>2</sub> was initially adsorbed and then displaced by CH<sub>4</sub> and CO<sub>2</sub>, with CH<sub>4</sub> subsequently displaced by CO<sub>2</sub>. These conclusions provide some guidance for the study of competitive adsorption of multicomponent gases in coal, further improving the related theory of coal competitive adsorption.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"38 22","pages":"22182–22191 22182–22191"},"PeriodicalIF":5.3000,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Influencing Factors and Adsorption Process of N2/CH4/CO2 Competitive Adsorption in Coal\",\"authors\":\"Hongyu Pan, Mingrui Han*, Tianjun Zhang, Bingnan Ji, Mingyue Pan, Zefan Li and Shipeng Zhu, \",\"doi\":\"10.1021/acs.energyfuels.4c0436310.1021/acs.energyfuels.4c04363\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >To investigate the influence of key factors (temperature, pressure, and particle size) on the competitive adsorption of N<sub>2</sub>/CH<sub>4</sub>/CO<sub>2</sub> on coal, a self-built multicomponent gas adsorption apparatus was used based on the breakthrough curve method to conduct competitive adsorption experiments under different conditions. The adsorption process was dynamically analyzed by combining adsorption kinetics models with the pore structure characteristics of the samples. The results showed that increasing the temperature promotes competitive adsorption and enhances the preferential adsorption of CO<sub>2</sub>, while increasing the pressure and particle size mesh number inhibits competitive adsorption and weakens the preferential adsorption of CO<sub>2</sub>. The experimental data fitted well with the Yoon-Nelson, Thomas, and Clark kinetic models, with <i>R</i><sup>2</sup> values all above 0.9. The mass transfer rate constants followed the order <i>k</i>(N<sub>2</sub>) > <i>k</i>(CH<sub>4</sub>) > <i>k</i>(CO<sub>2</sub>). As temperature and pressure increased or particle size mesh number increased, the <i>k</i> values for each component increased, enhancing the gas mass transfer rate. The adsorption capacities (<i>q</i><sub><i>T</i></sub>) and Clark constants (<i>A</i>) for each component showed the order CO<sub>2</sub> > CH<sub>4</sub> > N<sub>2</sub>, indicating that the coal samples had the highest adsorption capacity and strength for CO<sub>2</sub>, followed by CH<sub>4</sub> and then N<sub>2</sub>. Lowering the temperature, increasing the pressure, or increasing the particle size mesh number all led to increases in <i>q</i><sub><i>T</i></sub> and <i>A</i> for each component. The samples exhibited good pore connectivity, with the most developed micropores having a diameter of 2.05 nm, and relatively large specific surface area and pore volume. During competitive adsorption, N<sub>2</sub> was initially adsorbed and then displaced by CH<sub>4</sub> and CO<sub>2</sub>, with CH<sub>4</sub> subsequently displaced by CO<sub>2</sub>. These conclusions provide some guidance for the study of competitive adsorption of multicomponent gases in coal, further improving the related theory of coal competitive adsorption.</p>\",\"PeriodicalId\":35,\"journal\":{\"name\":\"Energy & Fuels\",\"volume\":\"38 22\",\"pages\":\"22182–22191 22182–22191\"},\"PeriodicalIF\":5.3000,\"publicationDate\":\"2024-11-04\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Energy & Fuels\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.energyfuels.4c04363\",\"RegionNum\":3,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENERGY & FUELS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Energy & Fuels","FirstCategoryId":"5","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.energyfuels.4c04363","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENERGY & FUELS","Score":null,"Total":0}
引用次数: 0
摘要
为研究关键因素(温度、压力和粒度)对煤上 N2/CH4/CO2 竞争吸附的影响,采用基于突破曲线法的自制多组分气体吸附仪进行了不同条件下的竞争吸附实验。结合吸附动力学模型和样品的孔隙结构特征,对吸附过程进行了动态分析。结果表明,升高温度会促进竞争吸附,增强对 CO2 的优先吸附;而升高压力和粒径目数会抑制竞争吸附,减弱对 CO2 的优先吸附。实验数据与 Yoon-Nelson、Thomas 和 Clark 动力学模型非常吻合,R2 值均在 0.9 以上。传质速率常数的顺序为 k(N2) > k(CH4) > k(CO2)。随着温度和压力的升高或颗粒大小目数的增加,各组分的 k 值也随之增加,从而提高了气体的传质速率。各组分的吸附容量(qT)和克拉克常数(A)呈现出 CO2 > CH4 > N2 的顺序,表明煤样对 CO2 的吸附容量和强度最大,其次是 CH4,然后是 N2。降低温度、提高压力或增加粒度目数都会导致各组分的 qT 和 A 增加。样品表现出良好的孔隙连通性,最发达的微孔直径为 2.05 nm,比表面积和孔隙体积相对较大。在竞争吸附过程中,N2 最初被吸附,然后被 CH4 和 CO2 取代,CH4 随后被 CO2 取代。这些结论为煤中多组分气体的竞争吸附研究提供了一定的指导,进一步完善了煤竞争吸附的相关理论。
Influencing Factors and Adsorption Process of N2/CH4/CO2 Competitive Adsorption in Coal
To investigate the influence of key factors (temperature, pressure, and particle size) on the competitive adsorption of N2/CH4/CO2 on coal, a self-built multicomponent gas adsorption apparatus was used based on the breakthrough curve method to conduct competitive adsorption experiments under different conditions. The adsorption process was dynamically analyzed by combining adsorption kinetics models with the pore structure characteristics of the samples. The results showed that increasing the temperature promotes competitive adsorption and enhances the preferential adsorption of CO2, while increasing the pressure and particle size mesh number inhibits competitive adsorption and weakens the preferential adsorption of CO2. The experimental data fitted well with the Yoon-Nelson, Thomas, and Clark kinetic models, with R2 values all above 0.9. The mass transfer rate constants followed the order k(N2) > k(CH4) > k(CO2). As temperature and pressure increased or particle size mesh number increased, the k values for each component increased, enhancing the gas mass transfer rate. The adsorption capacities (qT) and Clark constants (A) for each component showed the order CO2 > CH4 > N2, indicating that the coal samples had the highest adsorption capacity and strength for CO2, followed by CH4 and then N2. Lowering the temperature, increasing the pressure, or increasing the particle size mesh number all led to increases in qT and A for each component. The samples exhibited good pore connectivity, with the most developed micropores having a diameter of 2.05 nm, and relatively large specific surface area and pore volume. During competitive adsorption, N2 was initially adsorbed and then displaced by CH4 and CO2, with CH4 subsequently displaced by CO2. These conclusions provide some guidance for the study of competitive adsorption of multicomponent gases in coal, further improving the related theory of coal competitive adsorption.
期刊介绍:
Energy & Fuels publishes reports of research in the technical area defined by the intersection of the disciplines of chemistry and chemical engineering and the application domain of non-nuclear energy and fuels. This includes research directed at the formation of, exploration for, and production of fossil fuels and biomass; the properties and structure or molecular composition of both raw fuels and refined products; the chemistry involved in the processing and utilization of fuels; fuel cells and their applications; and the analytical and instrumental techniques used in investigations of the foregoing areas.