4.8 Article

Feasible coupling of CH4/H2 mixtures to H2 storage in liquid organic hydrogen carrier systems

Journal

JOURNAL OF POWER SOURCES
Volume 541, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.jpowsour.2022.231721

Keywords

Liquid organic hydrogen carrier; Low-purity hydrogen; Methane; Catalyst activation; Hydrogenation; Supported Ru catalysts

Funding

  1. National Research Foundation of Korea (NRF) - Ministry of Science and ICT, Republic of Korea [2019M3E6A1064908]
  2. Korea Research Institute of Chemical Technology [KK2011-00]
  3. Ministry of Education, Republic of Korea [2016R1A6A1A03013422]
  4. National Research Council of Science & Technology (NST), Republic of Korea [KK2011-00] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
  5. National Research Foundation of Korea [2019M3E6A1064908] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)

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This study investigates the impacts of CH4 fraction on the essential steps for liquid organic hydrogen carrier systems. The results show that a CH4 fraction higher than 30% negatively affects the carbon content and catalytic activity, but has less impact under mild conditions.
The cheap CH4-containing hydrogen mixtures are available in petrochemical industry and nevertheless, their usage is limited because of economic issue. We herein demonstrate the impacts of CH4 fraction (fCH(4)) in CH4/H2 mixtures on the essential steps for liquid organic hydrogen carrier (LOHC) systems. In the preparation of Ru/ Al2O3 catalysts by thermolysis in CH4/H-2 mixtures, the fCH(4) affects the content of carbon formed by methane decomposition but not the size of Ru nanoparticles, indicating that it should be avoided to use a CH4/H-2 mixture with the fCH(4)of higher than 30%. When CH4/H2 mixtures are used for the hydrogenation of monobenzyltoluene, the higher fCH4 reduces the catalytic activity, particularly at high temperatures and H-2 partial pressures because of competitive adsorption of CH4 and H-2 on the Ru surface. Such an effect of CH4 is lessened under mild conditions, which is confirmed by the experiments using the same CH4/H-2 mixture for both catalyst preparation and hydrogenation reaction. Therefore, it is feasible to use the CH4/H-2 mixture of up to 30% fCH(4) for the preparation of Ru/A(2)O(3) and for stable H-2 storage performance at lower temperatures and H-2 partial pressures, thus enabling to couple the CH4/H-2 mixture to LOHC systems.

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