{"title":"Promoting proximity to enhance Fe-Ca interaction for efficient integrated CO2 capture and hydrogenation","authors":"Shuzhuang Sun, Bocheng Yu, Yanmei Shen, Yu Liu, Hongman Sun, Xuan Bie, Mengna Wu, Yongqing Xu, Chunfei Wu, Hui Zhou","doi":"10.1016/j.seppur.2024.130227","DOIUrl":null,"url":null,"abstract":"Integrated CO<sub>2</sub> capture and utilization (ICCU) using “capture-conversion” dual functional materials (DFMs) paves a cost-effective path for restricting CO<sub>2</sub> emissions by eliminating the energy-intensive intermediate processes. The interactions between catalysts and absorbents are believed pivotal in ICCU; however, there is a lack of environment-friendly strategy to fabricate the interaction for industrial applications. Here, we propose a solvent-free mechanochemical approach to promote the interaction by improving the proximity between natural calcium and iron sources. The interaction was systemically investigated and confirmed using XRD, XPS, TEM, TPR, etc. As a result, the mechanochemical approach derived DFM achieved 5.5 mmol/g CO<sub>2</sub> capacity, 87 % CO<sub>2</sub> conversion, and 100 % CO selectivity at 650 °C, significantly outperforming the CaO-alone benchmark (CO<sub>2</sub> capacity < 4.5mmol/g, CO<sub>2</sub> conversion < 73 %). Further incorporating MgO would alleviate the sintering and promote the CO<sub>2</sub> capture stability (< 15 % decrease after 20 cycles) by acting as a thermal-stable barrier. Based on in situ XRD, it is further confirmed that Fe-Ca interaction exhibits a dynamic looping mechanism in ICCU. The techno-economic analysis strongly supports the superiority of ICCU catalyzed by naturally sourced DFMs on eliminating the energy and H<sub>2</sub> consumption for CO<sub>2</sub> capture and upgradation. As a result, producing CO via ICCU using mechanochemical derived DFMs exhibits 20 % and 10 % cost decrease compared to the conventional CCU and ICCU using CaO alone scenarios, pointing out the potential of ICCU technology in industrial applications.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1000,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Separation and Purification Technology","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.seppur.2024.130227","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Integrated CO2 capture and utilization (ICCU) using “capture-conversion” dual functional materials (DFMs) paves a cost-effective path for restricting CO2 emissions by eliminating the energy-intensive intermediate processes. The interactions between catalysts and absorbents are believed pivotal in ICCU; however, there is a lack of environment-friendly strategy to fabricate the interaction for industrial applications. Here, we propose a solvent-free mechanochemical approach to promote the interaction by improving the proximity between natural calcium and iron sources. The interaction was systemically investigated and confirmed using XRD, XPS, TEM, TPR, etc. As a result, the mechanochemical approach derived DFM achieved 5.5 mmol/g CO2 capacity, 87 % CO2 conversion, and 100 % CO selectivity at 650 °C, significantly outperforming the CaO-alone benchmark (CO2 capacity < 4.5mmol/g, CO2 conversion < 73 %). Further incorporating MgO would alleviate the sintering and promote the CO2 capture stability (< 15 % decrease after 20 cycles) by acting as a thermal-stable barrier. Based on in situ XRD, it is further confirmed that Fe-Ca interaction exhibits a dynamic looping mechanism in ICCU. The techno-economic analysis strongly supports the superiority of ICCU catalyzed by naturally sourced DFMs on eliminating the energy and H2 consumption for CO2 capture and upgradation. As a result, producing CO via ICCU using mechanochemical derived DFMs exhibits 20 % and 10 % cost decrease compared to the conventional CCU and ICCU using CaO alone scenarios, pointing out the potential of ICCU technology in industrial applications.
期刊介绍:
Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.