Berlin 2024 – scientific programme

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O: Fachverband Oberflächenphysik

O 85: Heterogeneous Catalysis I

O 85.8: Talk

Thursday, March 21, 2024, 12:15–12:30, TC 006

Labile Oxygen-rich Mullite for Ozone Activation to Produce Highly Oxidizing Surface Peroxide — •Linfeng Su¹, Xu Chen², Huaping Zhao¹, Zhiyi Lu², and Yong Lei¹ — ¹Fachgebiet Angewandte Nanophysik, Institut für Physik & IMN MacroNano, Technische Universität Ilmenau, 98693 Ilmenau, Germany — ²Key Laboratory of Advanced Fuel Cells and Electrolyzers Technology of Zhejiang Province, Ningbo Institute of Materials Technology and Engineering, CAS, Ningbo, Zhejiang, 315201, PR China

Materials with labile oxygen (Olab) have represented great potential in catalysis owing to their unique electronic structure over conventional adsorbed oxygen and lattice oxygen. In this work, we demonstrate that the Olab can be generated in Mullite-Olab by introducing Al-O4 tetrahedral. The bridging oxygens between Al-O4 and M-O4 (M=Al or Si) are identified as Olab. Mullite-Olab exhibits excellent performance in catalytic ozone activation with a high quasi-first order rate constant (k=0.112 min-1) for degradation of atrazine, while the degradation constant closes to 0 for mullite without Olab. Operando Raman and DFT simulations further reveal that Olab is the catalytic active center, which activates ozone via an unusual surface peroxide pathway to generate surface high-oxidative Olab-O* species. Additionally, the catalytic ozonation based on Mullite-Olab also plays a crucial role in treating actual acrylic fiber wastewater. This work provides an advanced Mullite-Olab catalyst with an unconventional ozonation mechanism, promising for future non-biodegradable wastewater treatment.

Keywords: Labile oxygen; Catalytic ozonation; Atrazine; Surface peroxide