混合氧化铁化学链蒸汽甲烷重整的热力学评价和过程模拟,RSC Advances

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混合氧化铁化学链蒸汽甲烷重整的热力学评价和过程模拟
RSC Advances ( IF 3.9 ) Pub Date : 2020-12-24 , DOI: 10.1039/d0ra08610j
Virginia H Collins-Martinez ₁ , José F Cazares-Marroquin _{1,

2} , Jesús M Salinas-Gutierrez ₁ , Juan C Pantoja-Espinoza ₁ , Alejandro Lopez-Ortiz ₁ , Miguel J Melendez-Zaragoza ₁

Affiliation

使用混合氧化铁的蒸汽重整化学循环 (CL-SMR) 具有替代当前部分氧化 (POX) 和蒸汽重整 (SMR) 工艺的潜力。在这项研究中，提出了在 CL-SMR 反应方案下使用 FeMoO ₄、Fe ₂ ZnO ₄和 Fe ₂ MnO ₄作为氧载体 (OC)，以克服目前甲烷 POX 和 SMR 工艺的缺点。本研究旨在寻找用于生产合成气的潜在铁基金属氧化物，合成气可在蒸汽中的有利条件下再生，同时生产 H ₂. 进行了使用混合铁氧化物的 CL-SMR 反应方案的热力学评估和过程模拟。结果表明，FeMoO ₄、Fe ₂ ZnO ₄和Fe ₂ MnO ₄分别在750 ℃、730 ℃和600 ℃下产生合成气。然而，FeMoO ₄在有利条件下没有完全再生，而 Fe ₂ ZnO ₄和 Fe ₂ MnO ₄分别在 440 ℃和 640 ℃下完全再生。Fe ₂ MnO ₄在所研究的 OC 中显示出对合成气生产最有利的操作条件。初步实验研究涉及使用 Fe ₂ O ₃和 MnO 作为前体通过固态方法合成 Fe ₂ MnO ₄ ，通过XRD 对其进行表征，同时在 TGA CH ₄ -H ₂ O 氧化还原循环中评估其氧化还原性能，使用 CH ₄进行还原，然后对 OC 进行蒸汽氧化。_{结果表明，使用 Fe 2} MnO ₄既可以用甲烷还原也可以用水蒸气氧化提出了用于 CL-SMR 反应方案的合理还原-氧化速率，验证了本研究中进行的理论研究的可行性。

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The thermodynamic evaluation and process simulation of the chemical looping steam methane reforming of mixed iron oxides

Steam reforming chemical looping (CL-SMR) using mixed iron oxides has the potential as an alternative to the current partial oxidation (POX) and steam reforming (SMR) processes. In this study, the use of FeMoO₄, Fe₂ZnO₄ and Fe₂MnO₄ as oxygen carriers (OC) under the CL-SMR reaction scheme was proposed to overcome the current disadvantages of methane POX and SMR processes. This research is aimed at finding potential iron-based metal oxides for the production of syngas, which can be regenerated under favorable conditions in steam, while producing H₂. Thermodynamic evaluation and process simulation of the CL-SMR reaction scheme using mixed iron-oxides was performed. Results indicate that FeMoO₄, Fe₂ZnO₄ and Fe₂MnO₄ generated syngas at 750 °C, 730 °C and 600 °C, respectively. However, FeMoO₄ was not fully regenerated under favorable conditions, whereas Fe₂ZnO₄ and Fe₂MnO₄ were completely regenerated at 440 °C and 640 °C, respectively. Fe₂MnO₄ showed the most favorable operating conditions among the studied OC towards the production of syngas. Preliminary experimental studies involved the synthesis of Fe₂MnO₄ through a solid-state method using Fe₂O₃ and MnO as precursors, which was characterized via XRD, while its redox performance was evaluated in a TGA CH₄–H₂O redox cycle, with reduction using CH₄ followed by the steam oxidation of OC. Results indicate that both reduction with methane and oxidation with water vapor using Fe₂MnO₄ present reasonable reduction–oxidation rates to be used in the CL-SMR reaction scheme, verifying the feasibility of the theoretical study performed in the present investigation.

更新日期：2020-12-24

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