Catalytic peroxone process for low-temperature denitration with enhanced Ti-OOH formation on P-TiO2: Experimental, DFT, and semi-in-situ UV–vis studies. (15th December 2022)

• Record Type: Journal Article
• Authors: Zhang, Mingjia; Zhang, Shule; Meng, Fanyu; Hu, Mengjie; Wang, Zhongyu; Zeng, Yiqing; Zhong, Qin
• Is Part Of: Fuel. Volume 330(2022)
• Publication Date: 2022-12-15
• Subjects: P-TiO2 -- Catalytic peroxone process -- Denitration -- First-principles study -- Semi-in-situ UV–vis DRS; CPP Catalytic peroxone process; Fuel -- Periodicals; Coal -- Periodicals; Coal; Fuel; Periodicals; 662.6
• DOI: 10.1016/j.fuel.2022.125664
• Languages: English
• ISSNs: 0016-2361

Abstract

Graphical abstract: Highlights: P-doped TiO2 was employed in catalytic peroxone reaction for high-efficiency NO oxidation. The Ti-OOH formation is greatly promoted on the P-TiO2 by reducing the energy barriers. A possible promotion mechanism was investigated in detail by combining characterizations and DFT calculations. A semi-in-situ UV–vis chamber was developed and used to clarify the reaction occurs on the interface of the catalyst. Abstract: Promoting the formation of Ti-OOH in the TiO2 -based-catalyst/H2 O2 /O3 system is critical to further develop the catalytic peroxone process for low-temperature flue gas denitration. In this study, a series of phosphorus-doped TiO2 with rich Lewis acid sites and high stability was designed and established, achieving 94 % NO oxidation efficiency with less oxidant (373 K, H2 O2 /NO = 1.2, O3 /NO = 0.5) and high GHSV (1.2 × 10 5 h −1 ). Combining characterizations and DFT results, a possible mechanism was proposed: phosphorus-doping enhanced the Lewis acidity, which was conducive to the adsorption and activation of H2 O2 . Moreover, P-TiO2 significantly promoted the H2 O dissociation and Ti-OOH formation process by reducing the energy barrier, thereby promoting the synergistic effect between O3 and Ti-OOH. The semi-in-situ UV–vis DRS demonstrated that the catalytic peroxone process occurs at the solid–liquid interface and the Ti-OOH is consumed in the catalytic process. We hope this work provide a new investigation method and insight into the catalyst design.