Plasma‐catalytic one‐step steam reforming of methane to methanol: Revealing the catalytic cycle on Cu/mordenite

IF 3.5 3区工程技术 Q2 ENGINEERING, CHEMICAL

AIChE Journal Pub Date : 2024-08-30 DOI:10.1002/aic.18582

Yingzi Hao, Shangkun Li, Wei Fang, Ximiao Wang, Zhaolun Cui, Kristof M. Bal, Nick Gerrits, Hongchen Guo, Erik C. Neyts, Annemie Bogaerts, Yanhui Yi

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引用次数: 0

Abstract

Direct CH4 to CH3OH conversion is a long‐standing grand challenge in catalysis. We present one‐step steam reforming of methane to methanol (OSRMtM) by combining an atmospheric pressure CH4/H2O/Ar plasma with a Cu/Mordenite (Cu/MOR) catalyst at 170°C, achieving 77% CH3OH selectivity with 3.0% CH4 conversion. Catalyst characterization and plasma diagnostics, as well as D2O and H218O‐labeled isotope tracer experiments reveal that the excellent reaction performance is attributed to Cu‐O active sites confined by MOR zeolite. During plasma‐catalytic OSRMtM, both CH4 and H2O are activated in the plasma and dissociated to produce radicals (CH3, OH, and H). These radicals drive the redox process between Cu2+ and Cu+, playing an important role in plasma‐catalytic OSRMtM. Although a gradual reduction of Cu2+ to Cu+ leads to slow deactivation, the catalytic performance can be completely recovered through simple calcination, which enables a continuous plasma‐catalytic OSRMtM process using a fluidized‐bed reactor.

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等离子催化甲烷一步蒸汽转化为甲醇：揭示铜/莫来石的催化循环

将 CH4 直接转化为 CH3OH 是催化领域长期存在的巨大挑战。我们将常压 CH4/H2O/Ar 等离子体与 Cu/Mordenite (Cu/MOR) 催化剂在 170°C 的温度下结合使用，提出了一步蒸汽转化甲烷为甲醇（OSRMtM）的方法，实现了 77% 的 CH3OH 选择性和 3.0% 的 CH4 转化率。催化剂表征和等离子体诊断以及 D2O 和 H218O 标记的同位素示踪实验表明，优异的反应性能归功于 MOR 沸石限定的 Cu-O 活性位点。在等离子体催化 OSRMtM 过程中，CH4 和 H2O 在等离子体中被激活并解离产生自由基（CH3、OH 和 H）。这些自由基推动了 Cu2+ 和 Cu+ 之间的氧化还原过程，在等离子体催化 OSRMtM 中发挥了重要作用。虽然 Cu2+ 逐渐还原为 Cu+ 会导致缓慢的失活，但通过简单的煅烧就能完全恢复催化性能，从而实现了使用流化床反应器的连续等离子体催化 OSRMtM 工艺。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

AIChE Journal 工程技术-工程：化工

CiteScore

7.10

自引率

10.80%

发文量

411

审稿时长

3.6 months

期刊介绍： The AIChE Journal is the premier research monthly in chemical engineering and related fields. This peer-reviewed and broad-based journal reports on the most important and latest technological advances in core areas of chemical engineering as well as in other relevant engineering disciplines. To keep abreast with the progressive outlook of the profession, the Journal has been expanding the scope of its editorial contents to include such fast developing areas as biotechnology, electrochemical engineering, and environmental engineering. The AIChE Journal is indeed the global communications vehicle for the world-renowned researchers to exchange top-notch research findings with one another. Subscribing to the AIChE Journal is like having immediate access to nine topical journals in the field. Articles are categorized according to the following topical areas: Biomolecular Engineering, Bioengineering, Biochemicals, Biofuels, and Food Inorganic Materials: Synthesis and Processing Particle Technology and Fluidization Process Systems Engineering Reaction Engineering, Kinetics and Catalysis Separations: Materials, Devices and Processes Soft Materials: Synthesis, Processing and Products Thermodynamics and Molecular-Scale Phenomena Transport Phenomena and Fluid Mechanics.