Carbon monoxide oxidation catalysed by defective palladium chloride: DFT calculations, EXAFS, and in situ DRIRS measurements
文献信息
Qiaohong Li, Luyang Qiao, Ruiping Chen, Zuju Ma, Rui Si, Yuangen Yao, Kechen Wu
We examined the potential catalytic role of the palladium chloride catalyst in CO oxidation using density functional theory and experimental investigations. The active plane of the palladium chloride catalyst is identified as (140). We found that the defective PdCl2(140) surface is able to facilitate the activation of O2 and subsequently promote the oxidation of CO. The most significant reaction channel, the Eley–Rideal mechanism (MER1), proceeds first by a peroxo-type (OOCO) intermediate formation, second by O adsorption with the first CO2 release, then by the second CO attraction and the second CO2 formation, and finally by the second CO2 desorption and restoration of the defective PdCl2(140) surface. The rate-determining step is the formation of the second CO2 in the whole catalytic cycle. Compared to the previously reported catalytic systems, the reaction activation barrier (0.54 eV) of CO oxidation in the PdCl2 catalyst is low, indicating PdCl2 as a potential high-performance catalyst for CO oxidation. The present results enrich our understanding of CO oxidation of Pd-based catalysts and provide a basis for fabricating Pd-based catalysts with high activity.
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.














