TY - JOUR
T1 - Electronic coupling in bifunctional Pd–CoOx interfaces drives reactive oxygen activation for acetone low-temperature oxidation
AU - Wu, Yani
AU - Liu, Jicheng
AU - Liu, Jiamei
AU - Jiang, Zeyu
AU - Tian, Mingjiao
AU - Wang, Jingjing
AU - Dang, Fan
AU - Ai, Chunli
AU - Albilali, Reem
AU - He, Chi
N1 - Publisher Copyright:
© 2026 Elsevier B.V.
PY - 2026/6/15
Y1 - 2026/6/15
N2 - Integrating transition-metal oxides into noble-metal catalysts has proven effective in enhancing catalytic performance. However, oxygenated volatile organic compounds (OVOCs) purification over bimetallic catalysts is still limited by weak coupling and the accumulation of reaction intermediates. Strengthening the interaction in bimetallic sites offers a promising strategy to overcome these limitations, as it can modulate the electronic structure and d-band center of noble-metal species, thereby promoting the activation of OVOCs and ensuring the desired reaction pathways. Herein, bifunctional Pd–CoOx sites were stabilized on rod-like SBA-15, where electronic coupling between Pd2+ and Co2+ enables efficient charge redistribution and promotes molecular oxygen activated to highly reactive oxygen (O−). This interfacial synergy directs acetone oxidation via a kinetically favorable pathway of acetone, aldehydes to carboxylates, while promoting rapid decomposition of key intermediates such as CH2O* and C2H4O2, and avoids the formation of C2H2O intermediate. Meanwhile, this oxygen-mediated pathway remains operative under complex reaction atmospheres (H2S and CH3Cl), accounting for the exceptional catalytic stability of PdCoOx/SBA-15. This work offers valuable insights on the development of specific catalysts with functional active sites to synergistically enhance reactants and surface oxygen species activation for efficient OVOCs oxidation.
AB - Integrating transition-metal oxides into noble-metal catalysts has proven effective in enhancing catalytic performance. However, oxygenated volatile organic compounds (OVOCs) purification over bimetallic catalysts is still limited by weak coupling and the accumulation of reaction intermediates. Strengthening the interaction in bimetallic sites offers a promising strategy to overcome these limitations, as it can modulate the electronic structure and d-band center of noble-metal species, thereby promoting the activation of OVOCs and ensuring the desired reaction pathways. Herein, bifunctional Pd–CoOx sites were stabilized on rod-like SBA-15, where electronic coupling between Pd2+ and Co2+ enables efficient charge redistribution and promotes molecular oxygen activated to highly reactive oxygen (O−). This interfacial synergy directs acetone oxidation via a kinetically favorable pathway of acetone, aldehydes to carboxylates, while promoting rapid decomposition of key intermediates such as CH2O* and C2H4O2, and avoids the formation of C2H2O intermediate. Meanwhile, this oxygen-mediated pathway remains operative under complex reaction atmospheres (H2S and CH3Cl), accounting for the exceptional catalytic stability of PdCoOx/SBA-15. This work offers valuable insights on the development of specific catalysts with functional active sites to synergistically enhance reactants and surface oxygen species activation for efficient OVOCs oxidation.
KW - Acetone oxidation
KW - Bifunctional sites
KW - Electronic modulation
KW - Molecular oxygen activation
KW - Surface reaction mechanism
UR - https://www.scopus.com/pages/publications/105037195796
U2 - 10.1016/j.cej.2026.176790
DO - 10.1016/j.cej.2026.176790
M3 - 文章
AN - SCOPUS:105037195796
SN - 1385-8947
VL - 538
JO - Chemical Engineering Journal
JF - Chemical Engineering Journal
M1 - 176790
ER -