National Institute for Research and Development of
Isotopic and Molecular Technologies – INCDTIM

CO₂ methanation by MOF based / derived ordered mesoporous catalysts

Project financed by UEFISCDI

Project Code: TE – PN-III-P1-1.1-TE-2019-1447

Program: PNCDI III, Programul 1 – Dezvoltarea sistemului național de CD / Resurse Umane

Project Type: Proiecte de cercetare pentru stimularea tinerelor echipe independente (TE)

Contract Nr.: TE 161 / 2020

Duration: 01.11.2020 – 31.10.2022

Project leader:

Dr. Maria MIHEȚ

e-mail: maria.mihet[at]itim-cj[dot]ro

Phone: (+40)264-584037, ext. 122,129

fax: (+40)264-420042

INCDTIM – National Institute for Research and Development of Isotopic and Molecular Technologies, Department of Mass Spectrometry, Chromatography and Applied Physics

67-103 Donat Str., PO Box 700, RO-400293, Cluj-Napoca, Romania

Abstract

Methanation of CO₂ is receiving a revived scientific and technological interest: chemical storage of renewable energy as CH₄ (Power-to-Gas concept), combined with the use of CO₂ (CO₂ capture and utilization) bring both an energetic and an environmental advantage. Highly efficient CO₂ methanation catalysts, with good CH₄ selectivity should have catalytic functionalities ensuring both CO₂ and H₂ activation. In this context, metal-organic frameworks (MOFs), – a class of extended coordination networks obtained by assembling metal centers to organic linkers – could ensure enhanced dispersion of active metals inside their ordered porous structure, while their gas sorption and storage capacity could be beneficial in respect to CO₂ activation.

The main objective of the project is the development of ordered mesoporous MOF-based and MOF-derived Ni catalysts with enhanced catalytic and operational performance in the methanation of CO₂. Two strategies are pursued: (a) nucleation of MOF crystals on preshaped solid macrostructures (MOF-based catalysts), and (b) sacrificial use by thermolysis of MOFs to form MOF-derived structures, which inherit the characteristics and properties of the original MOF (high surface area, ordered porous structure, uniform distribution of constituent elements). Thus, after Ni nanoparticle incorporation, ordered mesoporous catalysts could be obtained, with enhanced mass transfer (better accessibility of active sites) and heat integration (better conductive heat transfer) in the catalytic bed. MOF-based and MOF-derived ordered mesoporous Ni catalysts will be structurally, morphologically and functionally characterized, while catalytic tests will pursue the evaluation of catalytic performance under differential and integral conditions, at different temperatures, CO₂:H₂ ratios, or flow conditions. Stability tests will allow the evaluation of the catalysts life time, while deactivation possibilities might be investigated and regeneration methods proposed.

Objectives

The main objective of the present project proposal is the development of ordered mesoporous MOF-based and MOF-derived Ni catalysts with enhanced catalytic and operational performance in the CO₂ methanation process.

From the catalytic performance point of view, high CO₂ conversion with corresponding excellent methane selectivity are aimed, with good stability and minimal deactivation.

The specific objectives derived from this main objective are:

O1 – Synthesis and characterization of MOF-based ordered mesoporous Ni catalysts.

O2 – Synthesis and characterization of MOF-derived ordered mesoporous Ni catalysts.

O3 – Catalytic activity performance of MOF-based and MOF-derived ordered mesoporous Ni catalysts – comparative study in the CO₂ methanation reaction (experimental set-up, catalytic tests under differential and integral reaction conditions, stability tests, deactivation tests).