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CO2 adsorption on PEHA-functionalized geothermal silica waste: a kinetic study and quantum chemistry approach
Reaction Chemistry & Engineering ( IF 3.4 ) Pub Date : 2022-05-27 , DOI: 10.1039/d2re00077f Jonatan Estévez-Jácome 1 , Carlos Argáez 2 , Rosa-María Ramírez-Zamora 1 , Brenda Alcántar-Vázquez 1
Reaction Chemistry & Engineering ( IF 3.4 ) Pub Date : 2022-05-27 , DOI: 10.1039/d2re00077f Jonatan Estévez-Jácome 1 , Carlos Argáez 2 , Rosa-María Ramírez-Zamora 1 , Brenda Alcántar-Vázquez 1
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The use of solid waste and industrial by-products as alternatives to traditional raw materials to develop CO2 adsorbents has recently gained interest. In the present work, silica waste produced in a geothermal plant was impregnated with pentaethylenehexamine (PEHA) to prepare an amine-modified CO2 adsorbent. The SiO2–PEHA adsorbent was characterized, and the effects of temperature and initial CO2 concentration on the CO2 adsorption were assessed. Experimental CO2 adsorption results were fitted to pseudo-first-order (PFO), pseudo-second-order (PSO), Elovich, and intraparticle diffusion (IP diffusion) kinetic models. In addition, using the Gaussian 16 computational chemistry software package with the 6-311+(d,p) basis set coupled with the B3LYP hybrid density functional theory model, an adsorption mechanism between PEHA and CO2 was proposed. The results showed that the CO2 adsorption rate increases as the temperature and the initial CO2 concentration increase. This happens as the resistance to CO2 diffusion decreases until the mass transfer limitations dominate. The maximum CO2 adsorption capacity was 1.05 mmol CO2 per g material at 60 °C with 10 vol% CO2. The PSO model showed the best fit for the CO2 adsorption process on the SiO2–PEHA material. This suggests a chemical reaction between CO2 and PEHA molecules. Quantum chemical techniques allowed corroborating the formation of ammonium carbamate as a product of the exothermic reaction of CO2 adsorption on the SiO2–PEHA material.
中文翻译：
PEHA功能化地热二氧化硅废料上的CO2吸附：动力学研究和量子化学方法
使用固体废物和工业副产品作为传统原材料的替代品来开发 CO 2吸附剂最近引起了人们的兴趣。在目前的工作中，将地热发电厂产生的二氧化硅废料用五亚乙基六胺 (PEHA) 浸渍以制备胺改性的 CO 2吸附剂。对SiO 2 -PEHA 吸附剂进行了表征，并评估了温度和初始CO 2浓度对CO 2吸附的影响。实验 CO 2吸附结果适合准一级 (PFO)、准二级 (PSO)、Elovich 和颗粒内扩散 (IP 扩散) 动力学模型。此外，利用具有6-311+(d,p)基组的Gaussian 16计算化学软件包，结合B3LYP混合密度泛函理论模型，提出了PEHA与CO 2之间的吸附机理。结果表明，CO 2吸附率随着温度和初始CO 2浓度的增加而增加。这会随着对 CO 2扩散的阻力降低直到传质限制占主导地位而发生。最大CO 2吸附量为1.05 mmol CO 2每克材料在 60 °C 和 10 vol% CO 2下。PSO 模型显示了对 SiO 2 -PEHA 材料上 CO 2吸附过程的最佳拟合。这表明CO 2和PEHA分子之间发生化学反应。量子化学技术可以证实氨基甲酸铵的形成是 CO 2吸附在 SiO 2 -PEHA 材料上的放热反应的产物。
更新日期：2022-05-27
中文翻译：
PEHA功能化地热二氧化硅废料上的CO2吸附：动力学研究和量子化学方法
使用固体废物和工业副产品作为传统原材料的替代品来开发 CO 2吸附剂最近引起了人们的兴趣。在目前的工作中，将地热发电厂产生的二氧化硅废料用五亚乙基六胺 (PEHA) 浸渍以制备胺改性的 CO 2吸附剂。对SiO 2 -PEHA 吸附剂进行了表征，并评估了温度和初始CO 2浓度对CO 2吸附的影响。实验 CO 2吸附结果适合准一级 (PFO)、准二级 (PSO)、Elovich 和颗粒内扩散 (IP 扩散) 动力学模型。此外，利用具有6-311+(d,p)基组的Gaussian 16计算化学软件包，结合B3LYP混合密度泛函理论模型，提出了PEHA与CO 2之间的吸附机理。结果表明，CO 2吸附率随着温度和初始CO 2浓度的增加而增加。这会随着对 CO 2扩散的阻力降低直到传质限制占主导地位而发生。最大CO 2吸附量为1.05 mmol CO 2每克材料在 60 °C 和 10 vol% CO 2下。PSO 模型显示了对 SiO 2 -PEHA 材料上 CO 2吸附过程的最佳拟合。这表明CO 2和PEHA分子之间发生化学反应。量子化学技术可以证实氨基甲酸铵的形成是 CO 2吸附在 SiO 2 -PEHA 材料上的放热反应的产物。
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