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Unveiling the water-resistant mechanism of Cu(I)-O-Co interfaces for catalytic oxidation

Journal 2021 · IF 13.273 · 发表于 2021 年 9 月 4 日
作者: Shuaiqi Zhao,Peng Wu,Jiajin Lin,Yifei Li,Anqi Li,Xiaojing Jin,Yu Chen,Bote Zhao,Yun Zhao,Guangxu Chen,Yongcai Qiu,Daiqi Ye,Shihe Yang
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摘要

The development of low-temperature and water-resistant heterogeneous catalysts without noble metals is vital in the effective treatment of atmospheric pollutants in practical application. Herein, we report that Cu(I)-O-Co interfaces of ultrafine CuO x on Co 3 O 4 prepared by co-precipitation exhibit promising low-temperature activity and good water resistance. Experiment results together with density functional theory (DFT) calculations not only verify that Cu + species are stabilized over Cu(I)-O-Co interfaces because of the strong interaction between Cu 2 O 1 and Co 3 O 4 , but also demonstrate that the Cu(I)-O-Co interface facilitates oxygen species activation for promoting catalytic oxidation and reduces the accumulation of hydroxyl and bicarbonate species on the surface of CuO x /Co 3 O 4 . DFT calculations also reveal that the CO oxidation rate-limiting step via the dissociation pathway under dry conditions is the Co-OO-Cu species dissociation while the CO coupling with the adsorbed O 2 becomes the rate determining step for CO oxidation through the direct pathway over Cu(I)-O-Co interface under humid conditions. Further, the CuO x /Co 3 O 4 catalyst also exhibits superior and stable catalytic activity for toluene oxidation, comparable with partial supported noble metal catalysts (T 90  = 190 °C). The present work gives a useful strategy for the rational design of low-temperature and water-resistant non-precious-based catalysts to be applicable in CO and toluene removal in practical applications.

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