Abstract

Mn-Ce-Zr-O catalysts doped with varying Mn content were prepared and assessed for the catalytic combustion of chlorobenzene (CB). Nanosized MCZ-0.67 catalyst with amorphous phase exhibited a high and stable catalytic activity among the studied catalysts, achieving 90% CB conversion at 226 °C and withstanding stability tests, including time-based stability and the successive influence of various operating conditions. Meanwhile, the MCZ-0.67 catalyst used showed good recyclability by calcination in air. Characterization results suggested that Mn doping played a dominant role in improving the catalytic performance, resulting in larger surface area, better redox properties and greater amounts of surface active oxygen. In addition, the introduction of Zr was also indispensable for maintaining the good catalytic performance of catalysts. Finally, trace amounts of polychlorinated by-products during CB oxidation were monitored and the oxidation process was discussed.

Highlights

  • Chlorinated volatile organic compounds (CVOCs), widely used as solvents, additives and raw materials in industry, are considered serious hazards to human health and the environment owing to their high toxicity, volatility and durability [1,2]

  • H2-temperature programmed reduction (H2-TPR) tests were measured under a mixed stream of H2 (10 vol%) and Ar (90 vol%), and 100 mg of the catalyst was tested in the range of 50–800 ◦C with a heating ramp of 10 ◦C min−1

  • Transmission electron microscopy (TEM) and scanning transmission electron microscopy (STEM) images were taken at a voltage of 200 kV on a JEM-2100F microscope (JEOL, Akishima, Japan) equipped with an energy dispersive X-ray spectrometer (EDX)

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Summary

Introduction

Chlorinated volatile organic compounds (CVOCs), widely used as solvents, additives and raw materials in industry, are considered serious hazards to human health and the environment owing to their high toxicity, volatility and durability [1,2]. Of the Ce-based transition metal oxides, a CeO2-ZrO2 solid solution, widely applied in the purification of vehicle exhaust [18], the selective catalytic reduction (SCR) of NOx [19] and the catalytic oxidation of VOCs [20], was found to exhibit a high OSC and thermal stability after the doping of a proper amount of ZrO2 into the CeO2 lattice. MnOx compounds are highly active due to their various labile oxygen species and high efficiency in reaction/oxidation cycles [23] and have been widely used in the catalytic removal of various pollutants, including benzene series [24], chlorinated aromatic hydrocarbons [25], nitrogen oxides [26] and aldehydes [27]. Trace amounts of organic by-products during CB oxidation were monitored and the oxidation process was discussed

Catalyst Preparation
Catalyst Characterization
Catalytic Performance Evaluation
Catalyst Stability
Product Analysis
Findings
Conclusions
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