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; National-Regional Engineering Center for Recovery of Waste Gases from Metallurgical and Chemical Industries, Kunming University of Science and Technology, Kunming 650500, China.
J Environ Sci (China). 2024 Jan;135:640-655. doi: 10.1016/j.jes.2022.10.047. Epub 2022 Nov 8.
Phosphate ions promoted Cu-SAPO-34 (P-Cu-SAPO-34) were prepared using bulk CuO particles as Cu precursor by a solid-state ion exchange technique for the selective catalytic reduction of NO with NH (NH-SCR). The effects of high temperature (H-T) hydrothermal aging on the NO removal (de-NO) performance of Cu-SAPO-34 with and without phosphate ions were systematically investigated at atomic level. The results displayed that both Cu-SAPO-34 and P-Cu-SAPO-34 presented relatively poor NO removal activity with a low conversion (< 30%) at 250-500°C. However, after H-T hydrothermal treatment (800°C for 10 hr at 10% HO), these two samples showed significantly satisfied NO elimination performance with a quite high conversion (70%-90%) at 250-500°C. Additionally, phosphate ions decoration can further enhance the catalytic performance of Cu-SAPO-34 after hydrothermal treatment (Cu-SAPO-34H). The textural properties, morphologies, structural feature, acidity, redox characteristic, and surface-active species of the fresh and hydrothermally aged samples were analyzed using various characterization methods. The systematical characterization results revealed that increases of 28% of the isolated Cu active species (Cu-2Z, Cu (OH)-Z) mainly from bulk CuO and 50% of the Brønsted acid sites, the high dispersion of isolated Cu active component as well as the Brønsted acid sites were mainly responsible for the accepted catalytic activity of these two hydrothermally aged samples, especially for P-Cu-SAPO-34H.
磷酸盐离子促进的 Cu-SAPO-34(P-Cu-SAPO-34)是通过一种固态离子交换技术,使用块状 CuO 颗粒作为 Cu 前体制备的,用于 NH-SCR 中选择性催化还原 NO。在原子水平上系统地研究了高温(H-T)水热老化对具有和不具有磷酸盐离子的 Cu-SAPO-34 的 NO 去除(脱 NO)性能的影响。结果表明,Cu-SAPO-34 和 P-Cu-SAPO-34 在 250-500°C 下的 NO 去除活性均较差,转化率较低(<30%)。然而,经过 H-T 水热处理(在 10%HO 下 800°C 处理 10 小时)后,这两种样品在 250-500°C 下表现出非常满意的 NO 消除性能,转化率相当高(70%-90%)。此外,磷离子修饰可以进一步增强 Cu-SAPO-34 在水热处理后的催化性能(Cu-SAPO-34H)。通过各种表征方法分析了新鲜和水热老化样品的织构性质、形貌、结构特征、酸性、氧化还原特性和表面活性物种。系统的表征结果表明,孤立的 Cu 活性物种(Cu-2Z、Cu(OH)-Z)的增加量为 28%,主要来自块状 CuO,Brønsted 酸位的增加量为 50%,孤立的 Cu 活性组分的高分散性以及 Brønsted 酸位是导致这两种水热老化样品具有较高催化活性的主要原因,特别是对 P-Cu-SAPO-34H 而言。