催化作用
脱氢
氧气
化学
过渡金属
金属
甲苯
X射线光电子能谱
X射线吸收光谱法
物理化学
无机化学
吸收光谱法
化学工程
有机化学
物理
量子力学
工程类
作者
Dandan Zhu,Yu Huang,Rong Li,Shiqi Peng,Pengge Wang,Junji Cao
标识
DOI:10.1021/acs.est.3c05431
摘要
Activating surface lattice oxygen (Olatt) through the modulation of metal-oxygen bond strength has proven to be an effective route for facilitating the catalytic degradation of volatile organic compounds (VOCs). Although this strategy has been implemented via the construction of the TM1-O-TM2 (TM represents a transition metal) structure in various reactions, the underlying principle requires exploration when using different TMs. Herein, the Cu2+-O-Fe3+ structure was created by developing CuO-Fe3O4 composites with enhanced interfacial effect, which exhibited superior catalytic activity to their counterparts, with T90 (the temperature of toluene conversion reaching 90%) decreasing by approximately 50 °C. Structural analyses and theoretical calculations demonstrated that the active Cu2+-O-Fe3+ sites at the CuO-Fe3O4 interface improved low-temperature reducibility and oxygen species activity. Particularly, X-ray absorption fine structure spectroscopy revealed the contraction and expansion of Cu-O and Fe-O bonds, respectively, which were responsible for the activation of the surface Olatt. A mechanistic study revealed that toluene can be oxidized by rapid dehydrogenation of methyl assisted by the highly active surface Olatt and subsequently undergo ring-opening and deep mineralization into CO2 following the Mars-van Krevelen mechanism. This study provided a novel strategy to explore interface-enhanced TM catalysts for efficient surface Olatt activation and VOCs abatement.
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