Amorphous and homogeneously Zr-doped MnOx with enhanced acid and redox properties for catalytic oxidation of 1,2-Dichloroethane

Series of MnOx based catalysts were prepared and investigated for 1,2-dichloroethane (1,2-DCE) oxidation. RZrMn prepared by a novel reflux method presented an amorphous structure and homogeneous dispersion of Zr, which prominently enhanced acid and redox properties, such as more surface oxygen species and vacancies (OAds/OLatt = 0.53), better reducibility, severer Jahn-Teller distortion, more total acid amount (396 mu mol.g- 1) and Bronsted acid sites. Compared with the pristine MnOx and ZrO2, R-ZrMn exhibited a better catalytic activity for 1,2-DCE oxidation (T90 = 287 degrees C and the reaction rate at 150 degrees C was 5.13 mu mol min- 1.g- 1), less formation of chlorinated by-products, high durability and resistance-H2O. Catalytic oxidation of 1,2-DCE and the formation of chlorinated by-products on MnOx based catalysts was typically represented as a synergistic catalysis process of acid and redox sites, and a positive relationship between total acid amount or OAds/OLatt and reaction rate of 1,2DCE oxidation was clearly observed. Meanwhile, a possible mechanism and formation pathway were proposed.

Automated summary

A series of MnOx based catalysts were prepared and investigated for 1,2-dichloroethane (1,2-DCE) oxidation. The RZrMn catalyst prepared by a novel reflux method showed improved acid and redox properties, leading to better catalytic activity, durability and resistance against water for 1,2-DCE oxidation. The catalytic oxidation process and formation of by-products on MnOx based catalysts were found to be influenced by acid and redox sites, with a positive correlation between total acid amount or OAds/OLatt and reaction rate.