臭氧
解吸
分解
湿度
分子
催化作用
工作(物理)
极地的
环境修复
化学
降级(电信)
机制(生物学)
环境科学
化学工程
活化能
相对湿度
环境化学
材料科学
地下水修复
化学物理
臭氧消耗
反应机理
能量(信号处理)
化学极性
吸附
纳米技术
有机分子
作者
Kai Ren,Hui Li,Haojun Zhao,Rui Wen,Yumin Wang,Ruiting Hao,Chunning Zhao,Xiang Wan,Weichao Wang
标识
DOI:10.1021/acs.est.6c03388
摘要
Humidity severely inhibits catalytic residual ozone decomposition at room temperature due to competitive adsorption between H 2 O and O 3, 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/YMn 2 O 5 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 YMn 2 O 5 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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