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Dipole-Spin Synergy in PdO/YMn2O5 Enables Fast Ozone Decomposition from -45 to >45 °C at High Humidity
Kai Ren1, Huan Li1, Haojun Zhao1
1College of Electronic Information and Optical Engineering, Nankai University, Tianjin 300071, China.
Abstract:
Humidity severely inhibits catalytic residual ozone decomposition at room temperature due to competitive adsorption between H2O and O3, thereby hindering the wide application of ozone as an oxidant. Here, we propose a synergistic strategy to fundamentally overcome catalytic water poisoning by modulating interfacial electric dipoles and active site spin states, and demonstrate its validation with a specifically designed PdO/YMn2O5 heterojunction catalyst, which enables 100% ozone removal under the harsh condition of 90% relative humidity (RH) and a weight gas hourly space velocity (WHSV) of 2,400,000 mL·g-1·h-1 with superior durability at room temperature. Moreover, it also enables efficient ozone decomposition from -45 to 45 °C under humid condition. XPS, EXAFS, and DFT calculations reveal that electron transfer from PdO to YMn2O5 establishes a strong interfacial dipole, creates electron-rich Mn sites that electrostatically repel polar water molecules while enhancing ozone adsorption. Critically, this electronic restructuring concurrently modulates the Mn spin state, drastically lowering the energy barrier for the rate-limiting desorption of triplet oxygen. This work elucidates the fundamental mechanism of dipole-spin synergy, establishing a new paradigm for designing humidity-resistant catalysts for efficient environmental remediation under extreme operating conditions.
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