Advanced Operando and In Situ X-ray Characterization
Argonne National Laboratory
Description
Argonne National Laboratory has well established capabilities for operando and in situ X-ray spectroscopy and X-ray scattering characterization of catalysts. A suite of reactors are maintained, including (a) a high-pressure (up to 90 bar), high-temperature (up to 600 °C) reactor for three-phase (liquid, gas, solid) operando X-ray Absorption Spectroscopy (XAS), (b) a high temperature (up to 900 °C) thin-walled quartz tube plug flow micro-reactor suitable for both X-ray spectroscopy and X-ray scattering, as well as (c) multiple other reactor systems for in situ measurements.
Capability Bounds
The process parameters, reactor compatibility, and XAS feasibility are determined on a case-by-case basis. Catalyst requirements range from milligram to gram quantities.
Unique Aspects
Colocated catalyst testing laboratory and X-ray light source with significant expertise in both fields. Ability to conduct operando x-ray spectroscopic studies on catalytic systems for a wide ranging of process conditions including reactions involving gas-solid, liquid-solid, and gas-liquid-solid process conditions at temperatures up 1000 oC to or pressures up to 90 atms.
Availability
Availability is dependent on scheduling experiment time at the Advanced Photon Source (APS). One floor-mounted (“walk-in”) hood is dedicated to process and experiment protocol testing prior to X-ray analysis.
Benefit
In many cases, measuring and understanding the active site electronic structure and coordination environment under non-ambient or catalytic conditions provides key insights into catalyst synthesis, reactions, and deactivation.
Capability Expert(s)
Ted Krause, A. Jeremy Kropf
References
B. Wood, E. Schwegler, W.-I. Choi, and T. Ogitsu, “Hydrogen-Bond Dynamics of Water at the Interface with InP/GaP(001) and the Implications for Photoelectrochemistry,” J. Am. Chem. Soc. 135, 15774 (2013).
T. A. Pham, D. Lee, E. Schwegler, G. Galli, “Interfacial Effects on the Band Edges of Functionalized Si Surfaces in Liquid Water,” J. Am. Chem. Soc. 136, 17071 (2014).
B.C. Wood, T. Ogitsu, and E. Schwegler, “Ab initio modeling of water-semiconductor interfaces for photocatalytic water splitting: The role of surface oxygen and hydroxyl,” J. Photon. Energy 1, 016002 (2011).
