Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming 650500, China.
Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming 650500, China.
J Environ Sci (China). 2025 Apr;150:188-201. doi: 10.1016/j.jes.2024.02.022. Epub 2024 Mar 17.
To improve the activity of Co/AlO catalysts in selective catalytic oxidation of ammonia (NH-SCO), valence state and size of active centers of AlO-supported Co catalysts were adjusted by conducting H reduction pretreatment. The NH-SCO activity of the adjusted 2Co/AlO catalyst was substantially improved, outperforming other catalysts with higher Co-loading. Fresh Co/AlO catalysts exhibited multitemperature reduction processes, enabling the control of the valence state of the Co-active centers by adjusting the reduction temperature. Changes in the state of the Co-active centers also led to differences in redox capacity of the catalysts, resulting in different reaction mechanisms for NH-SCO. However, in situ diffuse reflectance infrared Fourier transform spectra revealed that an excessive O activation capacity caused overoxidation of NH to NO and NO. The NH-SCO activity of the 2Co/AlO catalyst with low redox capacity was successfully increased while controlling and optimizing the N selectivity by modulating the active centers via H pretreatment, which is a universal method used for enhancing the redox properties of catalysts. Thus, this method has great potential for application in the design of inexpensive and highly active catalysts.
为提高 Co/AlO 催化剂在氨选择性催化氧化(NH-SCO)中的活性,通过进行 H 还原预处理来调整 AlO 负载的 Co 催化剂的活性中心的价态和尺寸。调整后的 2Co/AlO 催化剂的 NH-SCO 活性得到了显著提高,优于其他负载更高 Co 的催化剂。新鲜的 Co/AlO 催化剂表现出多温度还原过程,通过调整还原温度来控制 Co 活性中心的价态。Co 活性中心状态的变化也导致了催化剂氧化还原能力的差异,从而导致 NH-SCO 的反应机制不同。然而,原位漫反射红外傅里叶变换光谱表明,过度的 O 活化能力会导致 NH 过度氧化为 NO 和 NO。通过 H 预处理调节活性中心,可以成功提高低氧化还原能力的 2Co/AlO 催化剂的 NH-SCO 活性,同时控制和优化 N 的选择性,这是一种通过调节活性中心来增强催化剂氧化还原性能的通用方法。因此,该方法在设计廉价且高活性催化剂方面具有很大的应用潜力。