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Issue 29, 2020
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Hard X-ray-based techniques for structural investigations of CO2 methanation catalysts prepared by MOF decomposition

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Abstract

Thermal decomposition of metal–organic framework (MOF) precursors is a recent method to create well-dispersed metal centers within active catalyst materials with enhanced stability, as required for dynamic operation conditions in light of challenges caused by the renewable energy supply. Here, we use a hard X-ray-based toolbox of pair distribution function (PDF) and X-ray absorption spectroscopy (XAS) analysis combined with X-ray diffraction and catalytic activity tests to investigate structure–activity correlations of methanation catalysts obtained by thermal decomposition of a Ni(BDC)(PNO) MOF precursor. Increasing the decomposition temperature from 350 to 500 °C resulted in Nifcc nanoparticles with increasing particle sizes, alongside a decrease in Ni2+ species and strain-induced peak broadening. For lower temperatures and inert atmosphere, Ni3C and NiO phases co-existed. A graphitic shell stabilized the Ni particles. Compared to an inert atmosphere, reducing conditions led to larger particles and a faster decomposition of the MOF precursor. Catalytic studies revealed that the decomposition at an intermediate temperature of 375 °C in 5% H2/He is the best set of parameters to obtain high specific surface areas while maintaining particle sizes that feature many active Ni centers for the formation of CH4.

Graphical abstract: Hard X-ray-based techniques for structural investigations of CO2 methanation catalysts prepared by MOF decomposition

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Supplementary files

Article information


Submitted
01 Mar 2020
Accepted
02 Jul 2020
First published
21 Jul 2020

This article is Open Access

Nanoscale, 2020,12, 15800-15813
Article type
Paper

Hard X-ray-based techniques for structural investigations of CO2 methanation catalysts prepared by MOF decomposition

N. Prinz, L. Schwensow, S. Wendholt, A. Jentys, M. Bauer, W. Kleist and M. Zobel, Nanoscale, 2020, 12, 15800
DOI: 10.1039/D0NR01750G

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