Bruna Thaisa Martins Ferreira, Vitor Anthony Duarte, Leonardo Hadlich de Oliveira, Washington Luiz Félix Santos, Pedro Augusto Arroyo
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Thus, in this work, H<sub>2</sub>S (up to 2.5 bar) and CO<sub>2</sub> and CH<sub>4</sub> (up to 50 bar) adsorption/desorption isotherms on PAF-30 were determined at 293, 303 and 313 K for the first time in literature. PAF-30 was synthesized and characterized by XRD, FTIR, <sup>13</sup>C-NMR, Ar and CO<sub>2</sub> physisorption, SEM, TEM, TGA and DSC analyzes. Then, adsorption isotherms were determined gravimetrically. Experimental data were modelled with Jensen-Seaton equation. The results indicated that PAF-30 presents adsorption capacities in the order H<sub>2</sub>S > CO<sub>2</sub> > CH<sub>4</sub>. Adsorption/desorption branches do not match for systems studied, due to a hysteresis effect. Adsorption capacity decreases with temperature, indicating that physisorption is the main phenomenon observed. Experimental data were represented by Jensen-Seaton model. Thermodynamic analysis showed that all systems are exothermic and spontaneous. Working capacities obtained indicate that temperature reduces the performance for gas purification and that H<sub>2</sub>S systems are affected by hysteresis loop. 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引用次数: 0
摘要
H2S 和 CO2 被认为是天然气和沼气中的两种主要杂质。必须去除这些杂质，以实现经济和环境限制。为实现这一目标，吸附是一种很有前景的技术。在已研究过的捕获 H2S 和 CO2 的替代吸附剂中，多孔芳香族框架（PAFs）具有合适的选择性和显著的吸附能力，因而具有潜在的应用前景。然而，文献中关于 PAF-30 对 H2S 和 CO2 的吸附/解吸数据仍然很少。因此，本研究首次在文献中测定了 PAF-30 在 293、303 和 313 K 下对 H2S（最高 2.5 巴）、CO2 和 CH4（最高 50 巴）的吸附/解吸等温线。对 PAF-30 进行了合成，并通过 XRD、FTIR、13C-NMR、Ar 和 CO2 物理吸附、SEM、TEM、TGA 和 DSC 分析对其进行了表征。然后，用重力法测定了吸附等温线。实验数据用 Jensen-Seaton 方程建模。结果表明，PAF-30 的吸附能力顺序为 H2S > CO2 > CH4。由于滞后效应，所研究系统的吸附/解吸分支并不一致。吸附容量随温度升高而降低，这表明物理吸附是观察到的主要现象。实验数据用 Jensen-Seaton 模型表示。热力学分析表明，所有系统都是自发放热的。获得的工作容量表明，温度降低了气体净化的性能，H2S 系统受到滞后环的影响。此外，循环吸附结果表明，PAF-30 具有在 PSA 模拟中应用和进一步研究高压条件下 H2S 和 CO2 捕获的潜力。
High-pressure adsorption of H2S, CO2 and CH4 on porous aromatic framework (PAF-30) at different temperatures
H2S and CO2 are considered two main impurities of natural gas and biogas. These impurities must be removed in order to achieve economic and environmental restrictions. Adsorption is a promising technology studied to achieve this goal. Among alternative adsorbents studied to capture H2S and CO2, porous aromatic frameworks (PAFs) had shown potential application because of suitable selectivity and remarkable adsorption capacity. However, H2S and CO2 adsorption/desorption data on PAF-30 are still scarce in literature. Thus, in this work, H2S (up to 2.5 bar) and CO2 and CH4 (up to 50 bar) adsorption/desorption isotherms on PAF-30 were determined at 293, 303 and 313 K for the first time in literature. PAF-30 was synthesized and characterized by XRD, FTIR, 13C-NMR, Ar and CO2 physisorption, SEM, TEM, TGA and DSC analyzes. Then, adsorption isotherms were determined gravimetrically. Experimental data were modelled with Jensen-Seaton equation. The results indicated that PAF-30 presents adsorption capacities in the order H2S > CO2 > CH4. Adsorption/desorption branches do not match for systems studied, due to a hysteresis effect. Adsorption capacity decreases with temperature, indicating that physisorption is the main phenomenon observed. Experimental data were represented by Jensen-Seaton model. Thermodynamic analysis showed that all systems are exothermic and spontaneous. Working capacities obtained indicate that temperature reduces the performance for gas purification and that H2S systems are affected by hysteresis loop. Moreover, cyclic adsorption results show that PAF-30 has potential to be applied and further studied in PSA simulations for H2S and CO2 capture under high-pressure conditions.
期刊介绍：
The journal Adsorption provides authoritative information on adsorption and allied fields to scientists, engineers, and technologists throughout the world. The information takes the form of peer-reviewed articles, R&D notes, topical review papers, tutorial papers, book reviews, meeting announcements, and news.
Coverage includes fundamental and practical aspects of adsorption: mathematics, thermodynamics, chemistry, and physics, as well as processes, applications, models engineering, and equipment design.
Among the topics are Adsorbents: new materials, new synthesis techniques, characterization of structure and properties, and applications; Equilibria: novel theories or semi-empirical models, experimental data, and new measurement methods; Kinetics: new models, experimental data, and measurement methods. Processes: chemical, biochemical, environmental, and other applications, purification or bulk separation, fixed bed or moving bed systems, simulations, experiments, and design procedures.
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