Rh K-Edge High-Energy-Resolution Fluorescence-Detected X-ray Absorption Near-Edge Structure Spectroscopy Reveals Deactivated RhAlO x Structure in Aged Rh/γ-Al2O3 Catalyst

被引：0

作者：

Sato, Mizuki ^{[1
]}

Awaya, Keisuke ^{[2
]}

Tsushida, Masayuki ^{[3
]}

Machida, Masato ^{[2
,4
]}

Hiraoka, Nozomu ^{[5
]}

Ohyama, Junya ^{[2
,4
]}

机构：

[1] Kumamoto Univ, Grad Sch Sci & Technol, Chuo Ku, Kumamoto 8608555, Japan

[2] Kumamoto Univ, Fac Adv Sci & Technol, Kumamoto 8608555, Japan

[3] Kumamoto Univ, Tech Div, Kumamoto 8608555, Japan

[4] Kumamoto Univ, Inst Ind Nanomat IINa, Kumamoto 8608555, Japan

[5] Natl Synchrotron Radiat Res Ctr, Hsinchu 30092, Taiwan

来源：

ACS CATALYSIS | 2025年 / 15卷 / 08期

基金：

日本学术振兴会;

关键词：

X-ray absorption spectroscopy; HERFD-XANES; rhodium; rhodium aluminate; deactivation; three-way catalyst; IDENTIFICATION; NANOPARTICLES; RH/AL2O3; BEHAVIOR; IMPACT;

D O I：

10.1021/acscatal.5c00633

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Rh K-edge high-energy-resolution fluorescence-detected (HERFD) X-ray absorption near-edge structure (XANES) spectroscopy was used to investigate the deactivated structure in an aged Rh/gamma-Al2O3 catalyst for automotive gas purification, which has been difficult to identify using conventional XANES spectroscopy. HERFD-XANES spectroscopy uncovered the distinct spectral features of the deactivated structure in the aged Rh/gamma-Al2O3 catalyst, which differed from those of supported Rh2O3 and Rh metal species. Spectral simulations of possible deactivated structures revealed the formation of Rh3+ doped in gamma-Al2O3 or rhodium aluminate with octahedral coordination (octahedral RhAlO x ) as the deactivated structure. The spectrum of octahedral RhAlO x was extracted from the measured spectra of fresh and aged Rh/gamma-Al2O3 samples before and after H2 treatment at 600 degrees C using linear combination fitting analysis, thereby enabling the quantification of the fraction of octahedral RhAlO x present in the aged Rh/gamma-Al2O3 catalyst. This study not only demonstrates the identification and quantification of octahedral RhAlO x in aged Rh/Al2O3 using Rh K-edge HERFD-XANES spectroscopy but also highlights the potential of HERFD-XANES spectroscopy to deepen our understanding of catalyst structures and consequently facilitate catalyst development.

引用

页码：6466 / 6472

页数：7

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