不同来源的二氧化铈和二氧化铈-氧化锆纳米材料捕获二氧化碳,Physical Chemistry Chemical Physics

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不同来源的二氧化铈和二氧化铈-氧化锆纳米材料捕获二氧化碳
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2023-05-31 , DOI: 10.1039/d3cp00896g
D Panayotov ₁ , V Zdravkova ₁ , O Lagunov ₁ , S Andonova ₁ , I Spassova ₁ , D Nihtianova ₂ , G Atanasova ₁ , N Drenchev ₁ , E Ivanova ₁ , M Mihaylov ₁ , K Hadjiivanov ₁

Affiliation

研究了不同来源的二氧化铈和二氧化铈-氧化锆纳米材料，以阐明它们的结构和结构特征在控制CO ₂捕获性能中的作用。研究了两种商业二氧化铈和两种自制样品，CeO ₂和CeO ₂ –ZrO ₂ (75% CeO ₂ )混合氧化物。通过多种分析技术对样品进行了表征，包括 XRD、TEM、N ₂ -吸附、XPS、H ₂ -TPR、拉曼和 FTIR 光谱。应用静态和动态CO _{2吸附实验来评估CO}₂捕获性能。通过原位FTIR 光谱和 CO ₂ –TPD 分析评估了形成的表面物质的类型及其热稳定性。_{两种商业二氧化铈样品具有相似的结构和结构特征，在CO 2}吸附时形成相同类型的碳酸盐类表面物质，因此在静态和动态条件下表现出几乎相同的CO ₂捕获性能。吸附物质的热稳定性按照二齿(B)碳酸盐、碳酸氢盐(HC)和三齿碳酸盐(T-III、T-II、TI)的顺序增加。_{CeO 2}的还原增加了最强键合的TI三齿碳酸盐的相对量。预吸附的水导致羟基化并增强碳酸氢盐的形成。尽管合成的CeO ₂样品具有较高的表面积（高出30%），但其在CO ₂吸附突破曲线中显示出不利的长传质区。由于其复杂的孔隙结构，该样品可能经历严重的颗粒内CO ₂扩散阻力。_{混合CeO 2} -ZrO ₂氧化物具有与合成的CeO ₂相同的表面积，表现出最高的CO ₂捕获能力，为136 μmol g ^-1在动态条件下。_{这与该样品上CO 2}吸附位点（包括缺陷）的最高浓度有关。CeO ₂ –ZrO ₂系统对气流中水蒸气的存在表现出最低的敏感性，因为该材料上缺乏解离水吸附。

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Capturing CO2 by ceria and ceria–zirconia nanomaterials of different origin

Ceria and ceria–zirconia nanomaterials of different origin were studied in order to elucidate the role of their structural and textural characteristics in controlling the performance towards CO₂ capture. Two commercial cerias and two home-prepared samples, CeO₂ and CeO₂–ZrO₂ (75% CeO₂) mixed oxide, were investigated. The samples were characterized by a number of analytical techniques including XRD, TEM, N₂-adsorption, XPS, H₂-TPR, Raman and FTIR spectroscopy. Static and dynamic CO₂ adsorption experiments were applied to assess the CO₂ capture performance. The type of surface species formed and their thermal stability were evaluated by in situ FTIR spectroscopy and CO₂–TPD analysis. The two commercial ceria samples possessed similar structural and textural characteristics, formed the same types of carbonate-like surface species upon CO₂ adsorption and, consequently, demonstrated almost identical CO₂ capture performance under both static and dynamic conditions. The thermal stability of the adsorbed species increased in the order bidentate (B) carbonates, hydrogen carbonates (HC) and tridentate carbonates (T-III, T-II, T-I). Reduction of CeO₂ increased the relative amount of the most strongly bonded T-I tridentate carbonates. Preadsorbed water led to hydroxylation and enhanced formation of hydrogen carbonates. Although the synthesized CeO₂ sample had a higher surface area (by 30%) it showed a disadvantageous long mass transfer zone in the CO₂-adsorption breakthrough curves. Because of its complex pore structure, this sample probably experiences severe intraparticle CO₂ diffusion resistance. Having the same surface area as the synthesized CeO₂, the mixed CeO₂–ZrO₂ oxide exhibited the highest CO₂ capture capacity of 136 μmol g⁻¹ under dynamic conditions. This was related to the highest concentration of CO₂ adsorption sites (including defects) on this sample. The CeO₂–ZrO₂ system showed the lowest sensitivity to the presence of water vapor in the gas stream due to the lack of dissociative water adsorption on this material.

更新日期：2023-05-31

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