4.7 Article

Direct biogas upgrading via CO2 methanation to high-quality biomethane over NiMg/CNT-SiO2 fiber catalysts

Journal

FUEL
Volume 310, Issue -, Pages -

Publisher

ELSEVIER SCI LTD
DOI: 10.1016/j.fuel.2021.122289

Keywords

Biomethane; Biogas upgrading; CO2 methanation; Ni-based catalysts; Carbon nanotubes-silica fiber composite

Funding

  1. Basic Research Fund & Institutional Capacity Building under the Fundamental Fund
  2. National Research Council of Thailand (NRCT)
  3. Graduate School of Chulalongkorn University
  4. State Key Laboratory of Clean Energy Utilization at Zhejiang University [ZJUCEU2018006]

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This research proposed a sustainable method for upgrading biogas to biomethane by catalytic CO2 methanation, focusing on improving the performance of Ni-based catalysts. The Ni/CNT-SF catalyst showed superior catalytic performance compared to other catalysts, achieving high CO2 conversion and CH4 selectivity under optimum conditions. The addition of Mg into the Ni/CNT-SF catalyst enhanced metal-support interaction and increased basic sites, promoting CO2 activation and production of high-quality biomethane.
As an environmentally friendly and renewable alternative fuel, biomethane can be obtained from biogas upgrading; however, the commercial technologies for upgrading are currently an unsustainable global process by releasing CO2 into the atmosphere. Here, this research proposed a novel sustainable method for direct biogas upgrading to high-quality biomethane by catalytic CO2 methanation and focused on the performance improvement of Ni-based catalysts. Carbon nanotubes-silica fiber (CNT-SF) composite as a high-heat transfer fibrous support was successfully synthesized using the Ni/silica fiber (SF) catalyst as a core-fiber seeding structure in ethanol steam reforming. The Ni/CNT-SF catalyst was extensively characterized and investigated in the direct biogas upgrading by CO2 methanation. The results revealed that Ni/CNT-SF catalyst exhibited superior catalytic performance than the Ni/SF and conventional Ni/silica porous (SP) catalysts. This suggested that the Ni/CNT-SF catalyst easily accessed the reactant molecules and exhibited an enhanced metal-support interaction with smaller Ni crystalline size, leading to a higher dispersion of the Ni active site, enhancing the CO2 methanation. Furthermore, the addition of Mg (1-3%wt.) into the Ni/CNT-SF catalyst resulted in a stronger metal-support interaction and increased moderate basic sites, which could suppress the Ni sintering and promote the adsorption and activation of CO2. Under optimum conditions (350 degrees C, 10 bar, H-2/CO2 molar ratio of 4, and GHSV of 24,000 mL.g(-1).h(-1)), the Ni-2Mg/CNT-SF catalyst achieved the highest CO2 conversion, CH4 selectivity, producing high-quality biomethane with CH4 content at approximately 95%, without CH4 losses.

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