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Zeolite-seed-directed Ru nanoparticles highly resistant against sintering for efficient nitrogen activation to ammonia
Science Bulletin ( IF 18.9 ) Pub Date : 2020-02-14 , DOI: 10.1016/j.scib.2020.02.010
Lingling Li 1 , Jihui Cai 1 , Yi Liu 1 , Jun Ni 1 , Bingyu Lin 1 , Xiuyun Wang 1 , Chak-Tong Au 1 , Lilong Jiang 1
Affiliation  

To stabilize Ru nanoparticles against sintering is an urgent problem in the utilization of Ru-based catalysts for NH3 synthesis. In the present study, we used Ru-containing ZSM-5 as seeds to crystallize ZSM-5, and the resulted Ru@ZSM-5 catalyst is highly resistant against Ru sintering. According to the results of diffuse reflectance infrared fourier transform spectroscopy (DRIFTS) and transmission electron microscopy (TEM) analyses, the average size of Ru nanoparticles is around 3.6 nm, which is smaller than that of Ru/ZSM-5-IWI prepared by incipient wetness impregnation. In NH3 synthesis (N2:H2 = 1:3) at 400 °C and 1 MPa, Ru@ZSM-5 displays a formation rate of 5.84 mmolNH3 gcat−1 h−1, which is much higher than that of Ru/ZSM-5-IWI (2.13 mmolNH3 gcat−1 h−1). According to the results of TEM, N2-temperature-programmed desorption (N2-TPD), X-ray photoelectron spectroscopy (XPS) and X-ray absorption fine structure (XAFS) studies, it is deduced that the superior performance of Ru@ZSM-5 is attributable to the small particle size and the ample existence of metallic Ru0 sites. This method of zeolite encapsulation is a feasible way to stabilize Ru nanoparticles for NH3 synthesis.



中文翻译:

沸石晶种导向的 Ru 纳米颗粒高度抗烧结,可有效将氮活化为氨

稳定Ru纳米颗粒以防止烧结是利用Ru基催化剂用于NH 3合成中的一个紧迫问题。在本研究中,我们使用含 Ru 的 ZSM-5 作为晶种来结晶 ZSM-5,所得 Ru@ZSM-5 催化剂对 Ru 烧结具有高度抵抗力。根据漫反射红外傅立叶变换光谱 (DRIFTS) 和透射电子显微镜 (TEM) 分析的结果,Ru 纳米粒子的平均尺寸约为 3.6 nm,小于早期制备的 Ru/ZSM-5-IWI。湿浸渍。在 400 °C 和 1 MPa 下的 NH 3合成(N 2 :H 2 = 1:3)中,Ru@ZSM-5 显示出 5.84 mmol NH 3 g cat的形成速率-1 h -1,远高于Ru/ZSM-5-IWI(2.13 mmol NH 3 g cat -1 h -1)。根据TEM、N 2 -程序升温脱附(N 2 -TPD)、X射线光电子能谱(XPS)和X射线吸收精细结构(XAFS)研究的结果,推断Ru的优越性能@ZSM-5 归因于小粒径和大量存在的金属 Ru 0位点。这种沸石包封方法是稳定用于 NH 3合成的 Ru 纳米粒子的可行方法。

更新日期:2020-02-14
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