Non-oxidative direct conversion of methane: Improved reactivity via linkage with dehydroaromatization

IF 7.2 2区工程技术 Q1 CHEMISTRY, APPLIED

Fuel Processing Technology Pub Date : 2024-03-01 DOI:10.1016/j.fuproc.2024.108067

Jin-Ju Lee , Sungwoo Lee , Youn-Sang Bae , Jechan Lee , Yong Tae Kim

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Abstract

The direct conversion of methane without an oxidant is an attractive approach to increase carbon efficiency. However, the reaction must be engineered appropriately. Herein, we propose a methane to olefins, aromatics, and hydrogen (MTOAH) system in which methane activation is promoted by co-feeding hydrocarbons generated from the Mo/HZSM-5 surface. The intentional separation of the catalyst and the gas-phase reaction at different temperatures (700 °C and 1020 °C) enables active and stable methane conversion via periodic reactions and regenerations. The linkage between MDA and MTOAH using 6Mo/HZSM-5 (30), which notably contributed to increasing the C2 production in MTOAH, was stabilized with 8.2% methane conversion during 49.5 h of the periodic CH₄ reaction-H₂ regeneration cycle. This study provides a new direction for achieving the efficient and carbon-neutral conversion of methane into useful chemicals.

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甲烷的非氧化直接转化：通过脱氢芳香化作用提高反应活性

在不使用氧化剂的情况下直接转化甲烷是提高碳效率的一种有吸引力的方法。但是，必须对反应进行适当的设计。在本文中，我们提出了一种甲烷制烯烃、芳烃和氢（MTOAH）系统，在该系统中，甲烷的活化是通过从 Mo/HZSM-5 表面生成的碳氢化合物共同进料来促进的。在不同温度（700 ℃ 和 1020 ℃）下有意分离催化剂和气相反应，可通过周期性反应和再生实现活跃而稳定的甲烷转化。使用 6Mo/HZSM-5（30）的 MDA 和 MTOAH 之间的联系显著提高了 MTOAH 中 C2 的产量，在 49.5 小时的周期性 CH4 反应-H2 再生循环中，甲烷转化率稳定在 8.2%。这项研究为实现甲烷向有用化学品的高效和碳中和转化提供了新的方向。

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来源期刊

Fuel Processing Technology 工程技术-工程：化工

CiteScore

13.20

自引率

9.30%

发文量

398

审稿时长

26 days

期刊介绍： Fuel Processing Technology (FPT) deals with the scientific and technological aspects of converting fossil and renewable resources to clean fuels, value-added chemicals, fuel-related advanced carbon materials and by-products. In addition to the traditional non-nuclear fossil fuels, biomass and wastes, papers on the integration of renewables such as solar and wind energy and energy storage into the fuel processing processes, as well as papers on the production and conversion of non-carbon-containing fuels such as hydrogen and ammonia, are also welcome. While chemical conversion is emphasized, papers on advanced physical conversion processes are also considered for publication in FPT. Papers on the fundamental aspects of fuel structure and properties will also be considered.