The AUREX cell: a versatile operando electrochemical cell for studying catalytic materials using X-ray diffraction, total scattering and X-ray absorption spectroscopy under working conditions
Year: 2024
Type: article
Abstract: Understanding the structure–property relationship in electrocatalysts under working conditions is crucial for the rational design of novel and improved catalytic materials. This paper presents the Aarhus University reactor for electrochemical studies using X-rays (AUREX) operando electrocatalytic flow cell, designed as an easy-to-use versatile setup with a minimal background contribution and a uniform flow field to limit concentration polarization and handle gas formation. The cell has been employed to measure operando total scattering, diffraction and absorption spectroscopy as well as simultaneous combinations thereof on a commercial silver electrocatalyst for proof of concept. This combination of operando techniques allows for monitoring of the short-, medium- and long-range structure under working conditions, including an applied potential, liquid electrolyte and local reaction environment. The structural transformations of the Ag electrocatalyst are monitored with non-negative matrix factorization, linear combination analysis, the Pearson correlation coefficient matrix, and refinements in both real and reciprocal space. Upon application of an oxidative potential in an Ar-saturated aqueous 0.1 M KHCO 3 /K 2 CO 3 electrolyte, the face-centered cubic (f.c.c.) Ag gradually transforms first to a trigonal Ag 2 CO 3 phase, followed by the formation of a monoclinic Ag 2 CO 3 phase. A reducing potential immediately reverts the structure to the Ag (f.c.c.) phase. Following the electrochemical-reaction-induced phase transitions is of fundamental interest and necessary for understanding and improving the stability of electrocatalysts, and the operando cell proves a versatile setup for probing this. In addition, it is demonstrated that, when studying electrochemical reactions, a high energy or short exposure time is needed to circumvent beam-induced effects.
Language: English
Field: Energy
Domain: Physical Sciences
Open Access status: hybrid
Estimated APC paid: $4,870
Funders: U.S. Department of Energy, Aarhus Universitet, National Research Foundation, Danmarks Grundforskningsfond, VINNOVA, Svenska Forskningsrådet Formas, Carlsbergfondet, Vetenskapsrådet, DanScatt, Office of Science, Deutsches Elektronen-Synchrotron, Division of Materials Research, Basic Energy Sciences
Awards: G1384804680, G1492569427, G208125138, G2268950645, G2770114408, G317939215, G3216578014, G3728818118, G4716817704, G5096929151, MAX IV operations – Formas, G5224014036, G5229471624, G594270511, G6778391521, GENESIS: A NEXT GENERATION SYNTHESIS CENTER, G712881263, GENESIS: A NEXT GENERATION SYNTHESIS CENTER, MAX IV operations 2019-2021, G8674945231, G8693631393
OpenAlex ID: W4402680620