Influence of nickel precursors on the properties and performance of Ni impregnated zeolite 5A and 13X catalysts in CO2 methanation

Liangyuan Wei,Wim Haije,Narendra Kumar,Janne Peltonen,Markus Peurla,Henrik Grenman,Wiebren De Jong

doi:10.1016/j.cattod.2020.05.025

Liangyuan Wei, Wim Haije + Show 5 more

Open Access

https://doi.org/10.1016/j.cattod.2020.05.025

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Abstract

Zeolite 13X and 5A supported Ni catalysts were synthesized for CO2 methanation using the evaporation impregnation method. The influence of using different Ni precursors (nitrate, citrate, and acetate) as well as calcination temperatures on the catalyst properties and performance were investigated. XRD, SEM-EDX, TEM, STEM-EDX, N2 physisorption, H2-TPR, TPD-NH3 and TG/DTA were used for detailed characterization of the catalysts. The parent structure of the zeolites did not change during catalyst synthesis. Using nickel citrate and acetate resulted in smaller NiO particle size compared to nitrate. STEM-EDX results showed that all the Ni-precursor complexes entered more efficiently the 13X zeolite structure, which is mainly due to steric hindrance resulting from the smaller pore size of 5A. Methanation experiments revealed that the 13X catalysts synthesized using nickel citrate (5% Ni) displayed clearly higher activity, compared to the catalysts synthesized using nickel nitrate or nickel acetate. A 79% conversion at 320 °C was obtained with 100% selectivity towards CH4 and the catalyst showed excellent stability during 200 h testing. Overall, it can be concluded that the Ni precursor significantly influences the physico-chemical characteristics and catalytic properties of Ni 13X and Ni 5A zeolite catalysts in CO2 methanation: complex size and pore size matter.

Highlights

Decreasing carbon dioxide emissions is a crucial task for all countries, in order to limit the severe challenges arising from global warming [1,2]
X-ray powder diffraction(XRD) The XRD background corrected diffractograms for calcined Ni modified 13X and 5A zeolite catalysts with different Ni precursors are shown in Fig. S. 3
The XRD patterns indicate that the crystal structure of 13X zeolite is maintained after the modification by precursors nickel nitrate, nickel citrate and nickel acetate

Summary

Introduction

Decreasing carbon dioxide emissions is a crucial task for all countries, in order to limit the severe challenges arising from global warming [1,2]. The availability of the raw materials CO2 and H2 in the future is a key factor in the large-scale production of synthetic fuel and chemicals. Large amounts of CO2 can be currently obtained from industrial facilities such as, fossil fuel-burning power plants and plants with CCS technologies (like oxyfuel combustion, chemical-looping combustion and calcium looping) [3,4,5]. This work investigates the utilization of H2 and CO2 to produce CH4 via the Sabatier reaction (1), which is a promising method for storing energy in large scale in a form directly usable in already existing infrastructure [11]. It has the potential to provide a new way of obtaining renewable completely carbon neutral CH4 for stabilizing energy demand, provided that CO2 can be efficiently captured from biomass derived gas sources and air in the future [12,13]

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