N-rich porous carbons with tunable affinity for CO2 adsorption achieve size-sieving CO2/N2 selectivity in turbostratic interlayers,Journal of Materials Chemistry A

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N-rich porous carbons with tunable affinity for CO2 adsorption achieve size-sieving CO2/N2 selectivity in turbostratic interlayers
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2022-11-09 , DOI: 10.1039/d2ta05911h
James N. Burrow ₁ , J. Ehren Eichler ₂ , Yu Wang ₃ , David C. Calabro ₃ , C. Buddie Mullins _{1,

2,

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Affiliation

While nitrogen- (N-) rich porous carbons hold promise to enable efficient carbon capture from post-combustion flue gas via temperature swing adsorption, a widespread tradeoff of surface chemistry with textural properties has resulted in a lack of detailed understanding in the relationships between a carbon adsorbent's material properties and its propensity for selective CO₂ adsorption. This study details a comprehensive screening of the CO₂ and N₂ adsorption performance for a set of turbostratic porous carbons with a wide range of microporosity (0–0.7 cm³ g⁻¹) and N-content (0–22 at%). By employing a temperature-dependent dual site Langmuir isotherm model, the energetics and capacities of CO₂ adsorption were related to the carbons' textural and surface chemical properties. The isosteric heats of adsorption were dependent on the N content, with the most N-rich carbons exhibiting zero-loading isosteric heats upwards of 45 kJ mol⁻¹ compared to around only 20 kJ mol⁻¹ for unfunctionalized carbons. On the other hand, the N₂ adsorption was a strong function primarily of the surface area and microporosity. As a result, the selectivity and predicted carbon capture performance for a simplified temperature swing adsorption process model were shown to be highly tunable by enhancing the N content (and limiting the N₂-accessible porosity) of the carbon adsorbents. This work provides useful structure–function relationships and helps to answer the longstanding question of the validity of N-incorporation for tuning the CO₂ adsorption performance of N-rich porous carbon adsorbents.

中文翻译：

对 CO2 吸附具有可调亲和力的富氮多孔碳在湍层夹层中实现尺寸筛分 CO2/N2 选择性

虽然富含氮 (N-) 的多孔碳有望通过变温吸附从燃烧后烟气中有效捕获碳，但表面化学与结构特性之间的广泛权衡导致对两者之间的关系缺乏详细了解。碳吸附剂的材料特性及其选择性吸附CO _{2的倾向。}本研究详细介绍了一组具有广泛微孔率（0-0.7 cm ³ g ^-1 ）的乱层多孔碳的 CO ₂和 N _{2吸附性能}) 和 N 含量 (0–22 at%)。通过采用温度相关的双位点朗缪尔等温线模型，CO ₂吸附的能量和容量与碳的结构和表面化学性质有关。等量吸附热取决于 N 含量，其中最富 N 的碳表现出高达 45 kJ mol ^-1的零负载等量热，而未官能化碳的等量吸附热仅为 20 kJ mol ^-1左右。另一方面，N ₂吸附主要是表面积和微孔率的强函数。_{结果，通过提高碳吸附剂的 N 含量（并限制 N 2}可接近的孔隙率），简化的变温吸附过程模型的选择性和预测的碳捕获性能被证明是高度可调的。这项工作提供了有用的结构-功能关系，并有助于回答长期存在的问题，即掺氮对调节富氮多孔碳吸附剂的 CO _{2吸附性能的有效性。}

更新日期：2022-11-14

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