The zip file 'Masspec_data.zip': Contains the raw data of the mass spectrometer measurements during the operando experiment (.rga and .ana files) for both samples. The folder also contains the exported data (.txt files) for readability and accessibility. Furthermore, a flow scheme of the gas mixing set-up is provided. The zip file 'SCRIPTS_fromBeamtime.zip': Contains the macros used during the beamtime to understand the datasets. The zip file 'OverviewChanges.zip': Contains the time we started the BCDI measurements ('_BCDI.txt'), we changed the gases ('_gases.txt') and we heated/cooled ('_heating.txt') for both samples. The zip file 'Samples.zip': Contains the raw AFM and SEM images shown in the manuscript. The zip files 'Sample150_P10ID01#4.zip' and 'Sample670_EBL2021.zip' contain all relevant datasets/measurements of the operando BCDI measurements. A list of the corresponding folder name to the BCDI datasets is given in the pdf file 'ImportantDatasetsList.pdf'. Note: The sample naming was changed for the manuscript, the data might contain the old sample names. 'Sample-150' corresponds to 'P10_ID01#4' and 'Sample-650' corresponds to 'EBL2021'.