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

Nanoscale
Nils PrinzMirijam Zobel

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 maintaini...Continue Reading

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Citations

Jun 12, 2021·Journal of the American Chemical Society·Zhihengyu ChenKarena W Chapman
Nov 18, 2021·Chemical Reviews·Maxwell W Terban, Simon J L Billinge

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Methods Mentioned

BETA
X-ray

Software Mentioned

XANES
xpdtools
LC
XAS
diffpy
PDFgetX3
cmi

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