Understanding the Impact of Hydrogen Activation by SrCe0.8Zr0.2O3-δ Perovskite Membrane Material on Direct Non-Oxidative Methane Conversion

Cheng, Sichao; Oh, Su Cheun; Sakbodin, Mann; Qiu, Limei; Diao, Yuxia; Liu, Dongxia

doi:10.3389/fchem.2021.806464

Title: Understanding the Impact of Hydrogen Activation by SrCe_0.8Zr_0.2O_3-δ Perovskite Membrane Material on Direct Non-Oxidative Methane Conversion

Journal Article · Mon Jan 10 00:00:00 EST 2022 · Frontiers in Chemistry

DOI:https://doi.org/10.3389/fchem.2021.806464· OSTI ID:1904841

Cheng, Sichao ^[1]; Oh, Su Cheun ^[1]; Sakbodin, Mann ^[1]; Qiu, Limei ^[2]; Diao, Yuxia ^[2]; Liu, Dongxia ^[1]

University of Maryland, College Park, MD (United States)
SINOPEC, Beijing (China)

Direct non-oxidative methane conversion (DNMC) converts methane (CH₄) in one step to olefin and aromatic hydrocarbons and hydrogen (H₂) co-product. Membrane reactors comprising methane activation catalysts and H₂-permeable membranes can enhance methane conversion by in situ H₂ removal via Le Chatelier's principle. Rigorous description of H₂ 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_0.8Zr_0.2O_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 H₂ activation into protons and electrons for H₂ 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 H₂ in methane stream. The characterizations show that SCZO activates H₂ to favor “soft coke” formation on the catalyst. The SCZO could absorb H₂in situ to lower its local concentration to mitigate the reverse reaction of DNMC in the tested conditions. The co-existence of H₂ co-feed, SCZO oxide, and DNMC catalyst in the present study mimics the conditions of DNMC in the H₂-permeable SCZO membrane reactor. The findings in this work offer the mechanistic understanding of and guidance for the design of H₂-permeable membrane reactors for DNMC and other alkane dehydrogenation reactions.

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Research Organization:: Univ. of Maryland, College Park, MD (United States)

Sponsoring Organization:: USDOE Office of Fossil Energy (FE); National Science Foundation (NSF)

Grant/Contract Number:: FE0031877; CBET-1928325

OSTI ID:: 1904841

Journal Information:: Frontiers in Chemistry, Vol. 9; ISSN 2296-2646

Publisher:: Frontiers Research FoundationCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Understanding the Impact of Hydrogen Activation by SrCe0.8Zr0.2O3-δ Perovskite Membrane Material on Direct Non-Oxidative Methane Conversion

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Title: Understanding the Impact of Hydrogen Activation by SrCe_0.8Zr_0.2O_3-δ Perovskite Membrane Material on Direct Non-Oxidative Methane Conversion