Catalytic Removal of Oxygen Impurities from Pressurized Oxy-Combustion Flue Gas for the Production of High-Purity Carbon Dioxide

Lu, Hong; Jiang, Ye; Abiodun, Oki; Schideman, Luke; Kuhn, Andrew; Yang, Hong; Lu, Yongqi

doi:10.1021/acs.energyfuels.1c04341

Title: Catalytic Removal of Oxygen Impurities from Pressurized Oxy-Combustion Flue Gas for the Production of High-Purity Carbon Dioxide

Journal Article · 20 February 2022 · Energy and Fuels

DOI: https://doi.org/10.1021/acs.energyfuels.1c04341 · OSTI ID:1875660

Lu, Hong ^[1];

^[2]; Abiodun, Oki ^[3]; Schideman, Luke ^[4]; Kuhn, Andrew ^[5];

^[4];

^[4]

Univ. of Illinois at Urbana-Champaign, IL (United States); University of Illinois at Urbana-Champaign
Univ. of Illinois at Urbana-Champaign, IL (United States); China Univ. of Petroleum, Qingdao (China)
Univ. of Illinois at Urbana-Champaign, IL (United States); Intel Corporation, Chandler, AZ (United States)
Univ. of Illinois at Urbana-Champaign, IL (United States)
Univ. of Illinois at Urbana-Champaign, IL (United States); Virginia Commonwealth Univ., Richmond, VA (United States)

Flue gas purification is important for pressurized oxy-combustion systems to produce pure carbon dioxide (CO₂) streams ready for storage or utilization. A catalytic approach to removing oxygen (O₂) impurities from pressurized oxy-combustion flue gas via reduction with methane (CH₄) was investigated in this work. Two types of catalysts were studied: palladium (Pd)-based catalysts supported on titania (TiO₂) prepared by incipient wetness impregnation and cobalt–manganese (CoMn) composite catalysts prepared by coprecipitation. The performance of the catalysts was evaluated in a high-pressure–high-temperature, fixed-bed reactor at a pressure of 15 bar and a gas hourly space velocity of 30 000 h^–1 (standard conditions), with a simulated feeding gas composed of 3 vol % O₂, 1.5 vol % CH₄, and CO₂ as the balance gas. Among the Pd catalysts, 5% Pd/TiO₂ achieved the maximum 86% O₂ removal at ≥350 °C. The CoMn oxide catalysts displayed comparable or better activities for O₂ reduction compared with the Pd catalysts. Among them, the Co₄₀Mn₁ catalyst exhibited the best performance, able to reduce 99.9% of O₂ impurities at ~370 °C with negligible carbon monoxide (CO) formation (<10 ppmv). Both trivalent and divalent Co and Mn were detected on the catalyst surface, and the superior activity of Co₄₀Mn₁ might be associated with the resultant disordered structure. Furthermore, the activity of the catalyst was not affected by the presence of a trace amount of nitric oxide (NO) gas contaminant. Results of this study provide the basis for scale-up studies in both the synthesis and performance of non-noble metal catalysts.

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Research Organization:: Univ. of Illinois at Urbana-Champaign, IL (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: FE0029161

OSTI ID:: 1875660

Journal Information:: Energy and Fuels, Journal Name: Energy and Fuels Journal Issue: 5 Vol. 36; ISSN 0887-0624

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
catalyst
environmental pollution
flue gas
oxides
oxygen impurity
palladium
pressurized oxy-combustion
purification
transition metals

Title: Catalytic Removal of Oxygen Impurities from Pressurized Oxy-Combustion Flue Gas for the Production of High-Purity Carbon Dioxide

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