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Hole-Activated Lattice Oxygen Enables Pt-Free Propane Dehydrogenation by Eliminating the Hydrogen Recombination Bottleneck.

Created on 30 Jul 2026

Authors

DongHwan Oh, Jaewoo Jeong, Susung Lee, Younghwan Park, Seunghyuck Chi, Yaejun Baik, Hyungjun Kim, Hyeyoung Shin, Minkee Choi

Published in

Angewandte Chemie (International ed. in English). Pages e1329092. Jul 30, 2026. Epub Jul 30, 2026.

Abstract

Gallia-alumina (GaxAl2- xO3) enables efficient propane dehydrogenation (PDH) via C-H activation at Ga-O pairs, but the overall rate is limited by sluggish hydrogen recombination to H2. Although Pt promotion alleviates this bottleneck, it introduces drawbacks including precious-metal cost and regeneration-induced sintering. Here, we show that Mg doping into GaxAl2- xO3 electronically activates lattice oxygen to enable rapid H2 evolution directly on the oxide, eliminating the need for Pt promotion. Electron paramagnetic resonance spectroscopy reveals the formation of hole-type oxygen species upon Mg incorporation, while kinetic/isotopic measurements and theoretical calculations demonstrate substantially accelerated hydrogen recombination kinetics. In situ infrared spectroscopy further shows rapid depletion of surface hydrogen species, consistent with facilitated H2 formation from Ga-H and O-H intermediates. At 853 K, Mg-doped GaxAl2- xO3 exhibits a threefold higher propylene formation rate than the undoped material at 97% propylene selectivity, outperforming benchmark PtSn/γ-Al2O3 and CrOx/γ-Al2O3 catalysts. Furthermore, the fully oxide-based catalyst shows the slowest deactivation over 30 dehydrogenation-regeneration cycles. These findings establish lattice-oxygen electronic engineering as a practical strategy for achieving both high activity and exceptional regeneration stability in oxide-catalyzed dehydrogenation chemistry.

PMID:
42530975
Bibliographic data and abstract were imported from PubMed on 30 Jul 2026.

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