Dispersive x-ray absorption spectroscopy for time-resolved in situ monitoring of mechanochemical reactions

Author(s)

Buzanich, Ana Guilherme ; Cakir, C. Tufan ; Radtke, Martin ; Haider, M. Bilal ; Emmerling, Franziska ; de Olive, Paulo F. M. ; Michalchuk, Adam A. L.

• Document type: Journal article
• Source: Journal of Chemical Physics; v. 157, n. 21, p. 11-pg., 2022-12-07.

Abstract

X-ray absorption spectroscopy (XAS) provides a unique, atom-specific tool to probe the electronic structure of solids. By surmounting long-held limitations of powder-based XAS using a dynamically averaged powder in a Resonant Acoustic Mixer (RAM), we demonstrate how time-resolved in situ (TRIS) XAS provides unprecedented detail of mechanochemical synthesis. The use of a custom-designed dispersive XAS (DXAS) setup allows us to increase the time resolution over existing fluorescence measurements from & SIM;15 min to 2 s for a complete absorption spectrum. Hence, we here establish TRIS-XAS as a viable method for studying mechanochemical reactions and sampling reaction kinetics. The generality of our approach is demonstrated through RAM-induced (i) bottom-up Au nanoparticle mechanosynthesis and (ii) the synthesis of a prototypical metal organic framework, ZIF-8. Moreover, we demonstrate that our approach also works with the addition of a stainless steel milling ball, opening the door to using TRIS-DXAS for following conventional ball milling reactions. We expect that our TRIS-DXAS approach will become an essential part of the mechanochemical tool box. (C) 2022 Author(s).All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY)license (http://creativecommons.org/licenses/by/4.0/). (AU)

• FAPESP's process: 20/14955-6 - Designing the next generation of advanced multicomponent materials through mechanochemical synthesis
• Grantee: Paulo Filho Marques de Oliveira
• Support Opportunities: Research Grants - Young Investigators Grants
• FAPESP's process: 21/12899-4 - Designing the next generation of advanced multicomponent materials through mechanochemical synthesis
• Grantee: Paulo Filho Marques de Oliveira
• Support Opportunities: Scholarships in Brazil - Young Researchers