Tan Wei, Wang Jiaming, Li Lulu, Liu Annai, Song Ge, Guo Kai, Luo Yidan, Liu Fudong, Gao Fei, Dong Lin
Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, PR China.
Department of Civil, Environmental, and Construction Engineering, Catalysis Cluster for Renewable Energy and Chemical Transformations (REACT), NanoScience Technology Center (NSTC), University of Central Florida, Orlando, FL 32816, United States.
J Hazard Mater. 2020 Apr 15;388:121729. doi: 10.1016/j.jhazmat.2019.121729. Epub 2019 Nov 20.
A series of ceria-zirconia solid solutions (CeZrO) were prepared by co-precipitation method and then sulfated with SO + O at 200 °C. Subsequent testing with the selective catalytic reduction of NO by NH (NH-SCR) showed that the activity of the sulfated CeZrO catalysts oxide catalysts exhibited a volcano-type tendency with increasing Zr content. Furthermore, the sulfated CeZrO catalyst showed the most desirable NH-SCR activity at 250-300 °C, and exhibited much better SO resistance at 250 °C. Detailed characterization results demonstrated that CeZrO could adsorb more surface sulfate species and then produce more stable acid sites than pure CeO at 200 °C. After sulfation treatment, more Ce and oxygen vacancies were formed on the surface of CeZrO. In situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) experiments suggested that the nitrates species deposited on the surface of as-prepared CeZrO, which showed no reactivity, could barely deposit on the same sample after sulfation. While, the sulfated CeZrO had more reactive acid sites to participate in the NH-SCR and the reaction proceeded via Eley-Rideal mechanism. This work proved that sulfation treatment could be used in designing an efficient cerium-zirconium based NH-SCR catalyst with great application prospect.
通过共沉淀法制备了一系列铈锆固溶体(CeZrO),然后在200℃下用SO + O进行硫酸化处理。随后进行的氨选择性催化还原NO(NH-SCR)测试表明,硫酸化的CeZrO催化剂的活性随Zr含量的增加呈现出火山型趋势。此外,硫酸化的CeZrO催化剂在250-300℃时表现出最理想的NH-SCR活性,并且在250℃时表现出更好的抗SO性能。详细的表征结果表明,在200℃时,CeZrO比纯CeO能吸附更多的表面硫酸根物种,进而产生更稳定的酸性位点。硫酸化处理后,CeZrO表面形成了更多的Ce和氧空位。原位漫反射红外傅里叶变换光谱(原位DRIFTS)实验表明,沉积在未处理的CeZrO表面的硝酸盐物种没有反应活性,硫酸化后几乎不能沉积在同一样品上。而硫酸化的CeZrO具有更多参与NH-SCR反应的活性酸性位点,反应通过Eley-Rideal机理进行。这项工作证明,硫酸化处理可用于设计具有广阔应用前景的高效铈锆基NH-SCR催化剂。