Operando X‐ray Powder Diffraction Study of Mechanochemical Activation Tested for the CO Oxidation over Au@Fe2O3 as Model Reaction

• Published in: ChemCatChem Vol. 14; no. 19
• Main Authors: Petersen, Hilke, De Bellis, Jacopo, Leiting, Sebastian, Das, Saurabh Mohan, Schmidt, Wolfgang, Schüth, Ferdi, Weidenthaler, Claudia
• Format: Journal Article
• Language: English
• Published: Weinheim Wiley Subscription Services, Inc 10.10.2022
• Subjects: Anisotropic crystallite size; Carbon monoxide; Catalysts; Catalytic activity; CO oxidation; Crystallites; Diffraction; External pressure; Gas analysis; Gold; Inorganic materials; Mechanochemistry; Operando analysis; Oxidation; Supported catalysts; Vessels
• ISSN: 1867-3880; 1867-3899
• DOI: 10.1002/cctc.202200703

Mechanochemistry has proven to be an excellent green synthesis method for preparing organic, pharmaceutical, and inorganic materials. Mechanocatalysis, inducing a catalytic reaction by mechanical forces, is an emerging field because neither external temperature nor pressure inputs are required. Previous studies reported enhanced catalytic activity during the mechanical treatment of supported gold catalysts for CO oxidation. So far, the processes inside the milling vessel during mechanocatalysis could not be monitored. In this work, the results of high‐energy operando X‐ray powder diffraction experiments and online gas analysis will be reported. A specific milling setup with a custom‐made vessel and gas dosing system was developed. To prove the feasibility of the experimental setup for operando diffraction studies during mechanocatalysis, the CO oxidation with Au@Fe2O3 as a catalyst was selected as a well‐known model reaction. The operando studies enabled monitoring morphology changes of the support as well as changes in the crystallite size of the gold catalyst. The change of the crystal size is directly correlated to changes in the active surface area and thus to the CO2 yield. The studies confirm the successful implementation of the operando setup, and its potential to be applied to other catalytic reactions. We present the first operando investigation of the mechanochemical activation of a catalyst in a ball mill. Gold supported on Fe2O3 was used for CO oxidation during mechanical activation. The catalyst was analyzed via XRPD and the CO conversion was determined via mass spectrometry, providing an invaluable insight into the structure‐performance relations.