Journal Article

PUBDB-2025-03964

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Micro-environment regulation for strong metal–support interaction in $RuO_2$-doped barium cerate for boosting photocatalytic ammonia production

Choong, C. E. ; Hong, Y. ; Nandy, S.Extern*DESY* ; Wong, K. T. ; Weng, B. ; Choi, E. ; Yoon, Y. (Corresponding author) ; Jang, M. (Corresponding author)

2026
Elsevier Amsterdam

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Please use a persistent id in citations: doi:10.1016/j.apcatb.2025.125870

Abstract: Modulating the local microenvironment via strong metal-support interaction (SMSI) approach in Ru-based photocatalyst for improving photocatalytic ammonia production is poorly understood. Herein, we investigate the mechanism of the SMSI effect of RuO$_2$ on barium cerate (BC) by forming Ru-O-Ce electron transfer channel to enhance the photocatalytic ammonium (NH$_4^+$) production. Among the prepared photocatalysts, BC-Ru$_{0.25}$ showed the highest NH$_4^+$ formation rate of 3.533 mmol g$^{−1}$ h$^{−1}$ with a 5.464 % apparent quantum efficiency (AQE), which was 5.17-fold higher than BC. In-situ X-ray photoelectron spectroscopy (XPS) and X-ray absorption near edge structure (XANES) analyses revealed that RuO$_2$ doping on BC promoted the formation of Ru-O-Ce bonds and degenerate barium 3d orbitals, creating an asymmetric coordination environment that improved N$_2$ interaction. Additionally, the formation of a Ru-O-Ce electron channel on BC prolonged the electron decay time and improved spatial separation, resulting in higher nitric oxide (NO) radical formation due to the promotion of hydroxyl radical generation from photoexcited holes. Notably, in-situ surface-enhanced Raman spectroscopy (SERS) analysis revealed that RuO$_2$ loading on BC altered the electronic state of Ba owing to the SMSI effect, improved N$_2$ interaction on the Ba-O bonds, and facilitated the NH$_4^+$ production. Density functional theory (DFT) calculations showed that RuO$_2$-doping of BC can result in Ba-N bonding and promote the nitric oxide reduction reaction (NORR) by reducing the energy barrier of the rate-determining step and accelerating the protonation process. This study demonstrates the SMSI effects via the strategy of a Ru-based dopant on NH$_4^+$ photocatalytic production.

Note: These measurements were carried out during in house research beamtime: H-20010499 Waiting for fulltext

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Contributing Institute(s):

1. PETRA-S (FS-PETRA-S)
2. DOOR-User (DOOR ; HAS-User)

Research Program(s):

1. 632 - Materials – Quantum, Complex and Functional Materials (POF4-632) (POF4-632)
2. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)

Experiment(s):

1. PETRA Beamline P64 (PETRA III)

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Database coverage:
; Clarivate Analytics Master Journal List ; Current Contents - Engineering, Computing and Technology ; Current Contents - Physical, Chemical and Earth Sciences ; Ebsco Academic Search ; Essential Science Indicators ; IF >= 20 ; JCR ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

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