Dispersed Pr on Nickel Oxide for Efficient Nitrous Oxide Direct Decomposition in Simulated Nitric Acid Exhaust

作者：Zhuoyi Zhang, Yunshuo Wu, Yuxin Sun, Haiqiang Wang, Zhongbiao Wu, Xuanhao Wu · 发表于：ACS ES&T Engineering · 年份：2024 · DOI：10.1021/acsestengg.4c00314 · 被引用次数：15 · 研究领域：Catalytic Processes in Materials Science、Gas Sensing Nanomaterials and Sensors、Advanced Photocatalysis Techniques

Nitrous oxide (N 2 O) is a potent greenhouse gas with a high global warming potential. The N 2 O direct decomposition (deN 2 O) is currently the most widely used technique due to its operational simplicity and lack of secondary pollution. The presence of impurity gases in industrial exhaust increases the challenge of eliminating N 2 O, urging the development of highly active and stable catalysts for its degradation. In this study, a series of praseodymium (Pr)-doped nickel oxide (NiO) catalysts were synthesized for N 2 O degradation. These catalysts showed higher N 2 O decomposition activity ( T 100 = 400–440 °C) than pure NiO ( T 100 = 480 °C) and also demonstrated high resistance to impurity gases in simulated industrial nitric acid tail gas. In the catalyst with a Pr to Ni ratio of 0.002, the highly dispersed Pr on the NiO surface regulated its particle size and increased specific surface area and pore volume. DFT calculations revealed that Pr significantly enhanced the electron-donating ability of Ni 2+, facilitating the dissociative adsorption of N 2 O on the catalyst surface, where O existed in the form of Ni 3+ -O*. Additionally, Pr reduced the desorption energy of O 2, the rate-determining step. During the reaction, Pr 3+ transferred electrons to Ni 3+ via f-d electron hopping, stabilizing the active Ni 2+ sites and enabling an efficient catalytic reaction. These findings demonstrate the practical potential of this catalyst and provide new insights into the degradatio...