High-Entropy Lanthanoid Oxide Catalysts for Oxidative Coupling of Methane.
- 1Materials and Structures Laboratory, Institute of Integrated Research, Institute of Science Tokyo, Nagatsuta-cho 4259-R3-6, Midori-ku, Yokohama-city, Kanagawa226-8501, Japan.
Abstract
High-entropy engineering of metal oxides provides a powerful platform for developing highly active and structurally robust catalysts; however, its application to heterogenous catalysis that requires stringent selectivity control remains largely unexplored. The low-temperature oxidative coupling of methane (OCM) demands catalysts that combine structural stability with precise tuning of surface basic strength. Here, we report a high-entropy lanthanoid oxide catalyst, (LaSmEuGdDy)0.4O3, synthesized via a sol-gel method using lanthanoid acetates and aspartic acid. The catalyst afforded ethylene and ethane in ∼12.3% total yield at temperatures less than 600 °C and maintained its catalytic activity for 240 h at 600 °C. Comparative studies with single-component lanthanoid oxides revealed that the high-entropy catalyst lowers the OCM onset temperature and markedly enhances catalyst durability. CO2 temperature-programmed desorption demonstrated that the surface basic strength of the high-entropy oxide can be systematically controlled through the average ionic radius, promoting the formation of moderately basic sites essential for low-temperature C-H activation. X-ray diffraction and photoelectron spectroscopy further showed that C-type rare-earth oxides exhibit superior resistance to transformation into less-active Ln2O2CO3 compared with A-type oxides and that the high-entropy configuration mitigates the progressive depletion of surface basic strength during prolonged OCM operation. These findings establish high-entropy design as an effective strategy for simultaneously controlling structural stability and surface functionality, opening new opportunities for selective heterogeneous catalysis.
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BibTeX
@article{takahashi2026highentropy,
title = {{High-Entropy Lanthanoid Oxide Catalysts for Oxidative Coupling of Methane.}},
author = {Rena Takahashi and Keiju Wachi and Keigo Kamata},
journal = {Journal of the American Chemical Society},
year = {2026},
month = oct,
doi = {10.1021/jacs.6c15276},
url = {https://europepmc.org/article/MED/42954514},
note = {CC BY-NC-ND},
}
RIS
TY - JOUR
TI - High-Entropy Lanthanoid Oxide Catalysts for Oxidative Coupling of Methane.
AU - Rena Takahashi
AU - Keiju Wachi
AU - Keigo Kamata
PY - 2026
DA - 2026/10/01
JO - Journal of the American Chemical Society
DO - 10.1021/jacs.6c15276
UR - https://europepmc.org/article/MED/42954514
AB - High-entropy engineering of metal oxides provides a powerful platform for developing highly active and structurally robust catalysts; however, its application to heterogenous catalysis that requires stringent selectivity control remains largely unexplored. The low-temperature oxidative coupling of methane (OCM) demands catalysts that combine structural stability with precise tuning of surface basic strength. Here, we report a high-entropy lanthanoid oxide catalyst, (LaSmEuGdDy)0.4O3, synthesized via a sol-gel method using lanthanoid acetates and aspartic acid. The catalyst afforded ethylene and ethane in ∼12.3% total yield at temperatures less than 600 °C and maintained its catalytic activity for 240 h at 600 °C. Comparative studies with single-component lanthanoid oxides revealed that the high-entropy catalyst lowers the OCM onset temperature and markedly enhances catalyst durability. CO2 temperature-programmed desorption demonstrated that the surface basic strength of the high-entropy oxide can be systematically controlled through the average ionic radius, promoting the formation of moderately basic sites essential for low-temperature C-H activation. X-ray diffraction and photoelectron spectroscopy further showed that C-type rare-earth oxides exhibit superior resistance to transformation into less-active Ln2O2CO3 compared with A-type oxides and that the high-entropy configuration mitigates the progressive depletion of surface basic strength during prolonged OCM operation. These findings establish high-entropy design as an effective strategy for simultaneously controlling structural stability and surface functionality, opening new opportunities for selective heterogeneous catalysis.
SN - 0002-7863
SN - 1520-5126
ER -