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

作者：Zhao, Shuaiqi; Wu, Peng; Lin, Jiajin; Li, Yifei; Li, Anqi; Jin, Xiaojing; Chen, Yu; Zhao, Bote; Zhao, Yun^*; Chen, Guangxu; Qiu, Yongcai^*; Ye, Daiqi; Yang, Shihe

来源：Chemical Engineering Journal, 2022, 429: 132219.

DOI：10.1016/j.cej.2021.132219

• DFT
• CuOx
• Interface
• Water-resistant
• Toluene oxidation

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 CuOx on Co3O4 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 Cu2O1 and Co3O4, 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 CuOx/Co3O4. 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 O2 becomes the rate determining step for CO oxidation through the direct pathway over Cu(I)-O-Co interface under humid conditions. Further, the CuOx/Co3O4 catalyst also exhibits superior and stable catalytic activity for toluene oxidation, comparable with partial supported noble metal catalysts (T90 = 190 degrees 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.

• 单位
  y; 北京大学