Structure–activity relations in heterogeneous catalysis can be revealed through in situ and operando measurements of catalysts in their active state. While hard X-ray tomography is an ideal method for non-invasive, multimodal 3D structural characterization on the micron to nm scale, performing tomography under controlled gas and temperature conditions is challenging. Here, we present a flexible sample environment for operando hard X-ray tomography at synchrotron radiation sources. The setup features are discussed, with demonstrations of operando powder X-ray diffraction tomography (XRD-CT) and energy-dispersive tomographic X-ray absorption spectroscopy (ED-XAS-CT). Catalysts for CO2 methanation and partial oxidation of methane are shown as case studies. The setup can be adapted for different hard X-ray microscopy, spectroscopy, or scattering synchrotron radiation beamlines, is compatible with absorption, diffraction, fluorescence, and phase-contrast imaging, and can operate with scanning focused beam or full-field acquisition mode. We present an accessible methodology for operando hard X-ray tomography studies, which offer a unique source of 3D spatially resolved characterization data unavailable to contemporary methods.
Sample Environment for Operando Hard X-ray Tomography—An Enabling Technology for Multimodal Characterization in Heterogeneous Catalysis