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Title: Best Practices for Operando Battery Experiments: Influences of X-ray Experiment Design on Observed Electrochemical Reactivity

Journal Article · · Journal of Physical Chemistry Letters

Operando experiments are increasingly being applied to capture dynamic reaction intermediates and explore kinetic effects in energy storage research and other areas. A critical assumption of such operando studies is that the data accurately represents the intrinsic system behavior, that is, the system is not perturbed by interaction with the probe or by the sample environment used to replicate the reaction conditions. Here we explore how electrochemical reactivity can be impacted by experiment design, including by X-ray beam interactions or by features of some operando electrochemical cell designs. The results show that without careful experiment design, the electrochemical reactivity in the region being probed by the X-ray beam can be retarded relative to the rest of the cell without obvious signs in the overall cell capacity or electrochemical profile. This can lead to conflicting reports in the literature and incorrect conclusions on reaction mechanisms. Recommendations for reliable operando electrochemical experiments are given.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Northeastern Center for Chemical Energy Storage (NECCES)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
DOE Contract Number:
AC02-06CH11357; SC0001294
OSTI ID:
1392027
Journal Information:
Journal of Physical Chemistry Letters, Vol. 6, Issue 11; ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English