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Surface-Phosphorylated Ceria for Chlorine-Tolerance Catalysis.

Yuetan Su¹, Kexin Cao¹, Yunhao Lu²

¹Key Laboratory of Environment Remediation and Ecological Health, Ministry of Education, College of Environmental and Resource Sciences, Zhejiang University, 866 Yuhangtang Road, Hangzhou 310058, P. R. China.

Environmental Science & Technology

|December 4, 2023

Summary

We discovered a new phosphorylated ceria catalyst that effectively destroys chlorinated pollutants. This advanced catalyst demonstrates high activity and stability, even in the presence of chlorine, paving the way for industrial applications in pollution control.

Keywords:

CeO2 chlorinated organics chlorine tolerance environmental catalysis surface phosphorylation

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Area of Science:

Catalysis
Materials Science
Surface Chemistry

Background:

Understanding active sites is crucial for designing effective catalysts.
Ceria (CeO2) based catalysts are widely studied for various catalytic applications.
Chlorine tolerance remains a significant challenge for many catalytic processes.

Purpose of the Study:

To computationally discover and experimentally validate a novel surface-phosphorylated ceria catalyst.
To investigate the active site structure and reaction mechanism of the catalyst.
To demonstrate the catalyst's performance and stability in degrading chlorinated volatile organic compounds (VOCs).

Main Methods:

Ab initio molecular dynamics (AIMD) calculations to probe atomic behavior.
In situ near-ambient pressure X-ray photoelectron spectroscopy (in situ NAP-XPS) for surface analysis.
Experimental catalysis testing, including a pilot-scale test for chlorinated VOC destruction.

Main Results:

Identification of a predominantly HPO4 active structure on CeO2 facets.
Observation of mobile hydrogen atoms on the catalyst surface at elevated temperatures.
Demonstration of robust chlorine tolerance and high catalytic activity for chlorinated VOC degradation.
Sustained catalyst stability over 68 days in a pilot test.

Conclusions:

Surface phosphorylation creates a highly active and chlorine-tolerant ceria catalyst.
A unique hydrogen atom hopping mechanism contributes to chlorine radical quenching.
The developed catalyst shows significant potential for industrial applications in treating chlorinated off-gases.