Autor: |
Ojeda-López R; Laboratório de Pesquisa em Adsorção e Captura de CO2 (LPACO2), Departamento de Engenharia Química, Universidade Federal do Ceará (UFC), Fortaleza 60455-760, CE, Brazil.; Departamento de Química, Universidad Autónoma Metropolitana-Iztapalapa (UAM-I), 09340 Mexico City, Mexico., Ramos-Sánchez G; Departamento de Química, Universidad Autónoma Metropolitana-Iztapalapa (UAM-I), 09340 Mexico City, Mexico.; CONACYT, Universidad Autónoma Metropolitana-Iztapalapa (UAM-I), 09340 Mexico City, Mexico., García-Mendoza C; Laboratorio de Nanotecnología, Centro de Investigación de Ciencia y Tecnología Avanzada de Tabasco (CICTAT), División Académica de Ingeniería y Arquitectura, Universidad Juárez Autónoma de Tabasco (UJAT), 86690 Tabasco, Mexico., C S Azevedo D; Laboratório de Pesquisa em Adsorção e Captura de CO2 (LPACO2), Departamento de Engenharia Química, Universidade Federal do Ceará (UFC), Fortaleza 60455-760, CE, Brazil., Guzmán-Vargas A; Laboratorio de Investigación en Materiales Porosos, Catálisis Ambiental y Química Fina, ESIQIE, Instituto Politécnico Nacional (IPN), 07738 Mexico City, Mexico., Felipe C; Departamento de Biociencias e Ingeniería, Centro Interdisciplinario de Investigaciones y Estudios sobre Medio Ambiente y Desarrollo (CIIEMAD), Instituto Politécnico Nacional (IPN), 07340 Mexico City, Mexico. |
Abstrakt: |
This work investigates the interplay of carbonization temperature and the chemical composition of carbon microfibers (CMFs), and their impact on the equilibration time and adsorption of three molecules (N 2 , CO 2 , and CH 4 ). PAN derived CMFs were synthesized by electrospinning and calcined at three distinct temperatures (600, 700 and 800 °C), which led to samples with different textural and chemical properties assessed by FTIR, TGA/DTA, XRD, Raman, TEM, XPS, and N 2 adsorption. We examine why samples calcined at low/moderate temperatures (600 and 700 °C) show an open hysteresis loop in nitrogen adsorption/desorption isotherms at -196.15 °C. The equilibrium time in adsorption measurements is nearly the same for these samples, despite their distinct chemical compositions. Increasing the equilibrium time did not allow for the closure of the hysteresis loop, but by rising the analysis temperature this was achieved. By means of the isosteric enthalpy of adsorption measurements and ab initio calculations, adsorbent/adsorbate interactions for CO 2 , CH 4 and N 2 were found to be inversely proportional to the temperature of carbonization of the samples (CMF-600 > CMF-700 > CMF-800). The enhancement of adsorbent/adsorbate interaction at lower carbonization temperatures is directly related to the presence of nitrogen and oxygen functional groups on the surface of CMFs. Nonetheless, a higher concentration of heteroatoms also causes: (i) a reduction in the adsorption capacity of CO 2 and CH 4 and (ii) open hysteresis loops in N 2 adsorption at cryogenic temperatures. Therefore, the calcination of PAN derived microfibers at temperatures above 800 °C is recommended, which results in materials with suitable micropore volume and a low content of surface heteroatoms, leading to high CO 2 uptake while keeping acceptable selectivity with regards to CH 4 and moderate adsorption enthalpies. |