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Non-oxidative methane conversion over Fe©SiO2 catalyst was studied for the first time in a hydrogen (H2) permeable tubular membrane reactor. The membrane reactor is composed of a mixed ionic-electronic SrCe0.7Zr0.2Eu0.1O3−δ thin film (≈20 μm) supported on the outer surface of a one-end capped porous SrCe0.8Zr0.2O3−δ tube. Significant improvement in CH4 conversion was achieved upon H2 removal from the membrane reactor compared to that in a fixed-bed reactor. The Fe©SiO2 catalyst in the H2 permeable membrane reactor demonstrated a stable ≈30 % C2+ single-pass yield, with up to 30 % CH4 conversion and 99 % selectivity to C2 (ethylene and acetylene) and aromatic (benzene and naphthalene) products, at the tested conditions. The selectivity towards C2 or aromatics was manipulated purposely by adding H2 into or removing H2 from the membrane reactor feed and permeate gas streams. [ABSTRACT FROM AUTHOR]

Direct non-oxidative methane conversion (DNMC) converts methane (CH 4 ) in one step to olefin and aromatic hydrocarbons and hydrogen (H 2 ) co-product. Membrane reactors comprising methane activation catalysts and H 2 -permeable membranes can enhance methane conversion by in situ H 2 removal via Le Chatelier's principle. Rigorous description of H 2 kinetic effects on both membrane and catalyst materials in the membrane reactor, however, has been rarely studied. In this work, we report the impact of hydrogen activation by hydrogen-permeable SrCe 0.8 Zr 0.2 O 3-δ (SCZO) perovskite oxide material on DNMC over an iron/silica catalyst. The SCZO oxide has mixed ionic and electronic conductivity and is capable of H 2 activation into protons and electrons for H 2 permeation. In the fixed-bed reactor packed with a mixture of SCZO oxide and iron/silica catalyst, stable and high methane conversion and low coke selectivity in DNMC was achieved by co-feeding of H 2 in methane stream. The characterizations show that SCZO activates H 2 to favor "soft coke" formation on the catalyst. The SCZO could absorb H 2 in situ to lower its local concentration to mitigate the reverse reaction of DNMC in the tested conditions. The co-existence of H 2 co-feed, SCZO oxide, and DNMC catalyst in the present study mimics the conditions of DNMC in the H 2 -permeable SCZO membrane reactor. The findings in this work offer the mechanistic understanding of and guidance for the design of H 2 -permeable membrane reactors for DNMC and other alkane dehydrogenation reactions., Competing Interests: LQ and YD were employed by the Research Institute of Petroleum Processing, SINOPEC, Beijing, China. All remaining authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest., (Copyright © 2022 Cheng, Oh, Sakbodin, Qiu, Diao and Liu.)

Direct non-oxidative methane conversion (DNMC) has been recognized as a single-step technology that directly converts methane into olefins and higher hydrocarbons. High reaction temperature and low catalyst durability, resulting from the endothermic reaction and coke deposition, are two main challenges. We show that a millisecond catalytic wall reactor enables stable methane conversion, C 2+ selectivity, coke yield, and long-term durability. These effects originate from initiation of the DNMC on a reactor wall and maintenance of the reaction by gas-phase chemistry within the reactor compartment. The results obtained under various temperatures and gas flow rates form a basis for optimizing the process towards lighter C 2 or heavier aromatic products. A process simulation was done by Aspen Plus to understand the practical implications of this reactor in DNMC. High carbon and thermal efficiencies and low cost of the reactor materials are realized, indicating the technoeconomic viability of this DNMC technology., (© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Non-oxidative methane conversion over Fe©SiO 2 catalyst was studied for the first time in a hydrogen (H 2 ) permeable tubular membrane reactor. The membrane reactor is composed of a mixed ionic-electronic SrCe 0.7 Zr 0.2 Eu 0.1 O 3-δ thin film (≈20 μm) supported on the outer surface of a one-end capped porous SrCe 0.8 Zr 0.2 O 3-δ tube. Significant improvement in CH 4 conversion was achieved upon H 2 removal from the membrane reactor compared to that in a fixed-bed reactor. The Fe©SiO 2 catalyst in the H 2 permeable membrane reactor demonstrated a stable ≈30 % C 2+ single-pass yield, with up to 30 % CH 4 conversion and 99 % selectivity to C 2 (ethylene and acetylene) and aromatic (benzene and naphthalene) products, at the tested conditions. The selectivity towards C 2 or aromatics was manipulated purposely by adding H 2 into or removing H 2 from the membrane reactor feed and permeate gas streams., (© 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)