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
(2024) In Journal of Applied Crystallography 57. p.1489-1502- 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... (More)
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 KHCO3/K2CO3 electrolyte, the face-centered cubic (f.c.c.) Ag gradually transforms first to a trigonal Ag2CO3 phase, followed by the formation of a monoclinic Ag2CO3 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.
(Less)
- author
- Frank, Sara
; Ceccato, Marcel
; Jeppesen, Henrik S.
; Marks, Melissa J.
; Nielsen, Mads L.N.
; Lu, Ronghui
; Gammelgaard, Jens Jakob
; Quinson, Jonathan
; Sharma, Ruchi
; Jensen, Julie S.
; Hjelme, Sara
; Friberg Klysner, Cecilie
; Billinge, Simon J.L.
; Just, Justus
LU
; Gjørup, Frederik H.
LU
; Catalano, Jacopo
and Lock, Nina
(Less) - organization
- publishing date
- 2024-10
- type
- Contribution to journal
- publication status
- published
- subject
- keywords
- cell design, electrocatalysis, operando studies, structure-property relationships, X-ray absorption spectroscopy, X-ray scattering
- in
- Journal of Applied Crystallography
- volume
- 57
- pages
- 14 pages
- publisher
- International Union of Crystallography
- external identifiers
-
- scopus:85206817639
- pmid:39387078
- ISSN
- 0021-8898
- DOI
- 10.1107/S1600576724007817
- language
- English
- LU publication?
- yes
- id
- 70c75eea-942f-4ca2-b61f-94cb2cda7a80
- date added to LUP
- 2024-12-17 15:59:07
- date last changed
- 2025-07-16 08:50:45
@article{70c75eea-942f-4ca2-b61f-94cb2cda7a80,
abstract = {{<p>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 KHCO3/K2CO3 electrolyte, the face-centered cubic (f.c.c.) Ag gradually transforms first to a trigonal Ag2CO3 phase, followed by the formation of a monoclinic Ag2CO3 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.</p>}},
author = {{Frank, Sara and Ceccato, Marcel and Jeppesen, Henrik S. and Marks, Melissa J. and Nielsen, Mads L.N. and Lu, Ronghui and Gammelgaard, Jens Jakob and Quinson, Jonathan and Sharma, Ruchi and Jensen, Julie S. and Hjelme, Sara and Friberg Klysner, Cecilie and Billinge, Simon J.L. and Just, Justus and Gjørup, Frederik H. and Catalano, Jacopo and Lock, Nina}},
issn = {{0021-8898}},
keywords = {{cell design; electrocatalysis; operando studies; structure-property relationships; X-ray absorption spectroscopy; X-ray scattering}},
language = {{eng}},
pages = {{1489--1502}},
publisher = {{International Union of Crystallography}},
series = {{Journal of Applied Crystallography}},
title = {{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}},
url = {{http://dx.doi.org/10.1107/S1600576724007817}},
doi = {{10.1107/S1600576724007817}},
volume = {{57}},
year = {{2024}},
}