Yao Pan, Li Jiayi, Pei Mingming, Liu Fudong, Xu Haidi, Chen Yaoqiang
Institute of New Energy and Low-Carbon Technology, Sichuan University, Chengdu, Sichuan 610207, China.
Department of Civil, Environmental, and Construction Engineering, Catalysis Cluster for Renewable Energy and Chemical Transformations (REACT), Nano Science Technology Center (NSTC), University of Central Florida, Orlando, Florida 32816, United States.
ACS Appl Mater Interfaces. 2024 Mar 27;16(12):14694-14703. doi: 10.1021/acsami.3c16747. Epub 2024 Mar 13.
Improving the N selectivity is always a great challenge for the selective catalytic oxidation of ammonia (NH-SCO) over noble-metal-based (especially Pt) catalysts. In this work, Cu as an efficient promoter was introduced into the Pt/SSZ-13 catalyst to significantly improve the N selectivity of the NH-SCO reaction. A PtCu alloy was formed in the PtCu/SSZ-13 catalyst, as confirmed by X-ray diffraction, transmission electron microscopy, energy dispersive spectrometry mapping, and X-ray absorption spectroscopy results. As indicated by the X-ray photoelectron spectroscopy analysis, the Pt species in the alloyed PtCu nanoparticle was mainly present in the electron-rich state on PtCu/SSZ-13, while the electron-deficient Cu and isolated Cu species were both present on the surface of PtCu/SSZ-13. Due to such a unique alloyed structure with an altered oxidation state, the N selectivity of NH-SCO on the PtCu/SSZ-13 catalyst was remarkably improved, while the NH-SCO activity was kept comparable to that on Pt/SSZ-13. The reaction path was changed from the NH mechanism on Pt/SSZ-13 to both NH and internal selective catalytic reduction mechanisms on the PtCu/SSZ-13 catalyst, which was considered the main reason for the enhanced N selectivity. This work provides a new route to synthesize efficient alloy catalysts for optimizing the N selectivity of NH-SCO for NH slip control in diesel exhaust purification.
对于基于贵金属(尤其是铂)的催化剂上的氨选择性催化氧化(NH-SCO)而言,提高氮选择性一直是一项巨大挑战。在本工作中,将铜作为一种高效促进剂引入到Pt/SSZ-13催化剂中,以显著提高NH-SCO反应的氮选择性。X射线衍射、透射电子显微镜、能量色散光谱图谱和X射线吸收光谱结果证实,在PtCu/SSZ-13催化剂中形成了PtCu合金。X射线光电子能谱分析表明,合金化的PtCu纳米颗粒中的铂物种在PtCu/SSZ-13上主要以富电子状态存在,而贫电子的铜和孤立的铜物种都存在于PtCu/SSZ-13的表面。由于这种具有改变的氧化态的独特合金结构,PtCu/SSZ-13催化剂上NH-SCO的氮选择性得到显著提高,同时NH-SCO活性与Pt/SSZ-13上的活性相当。反应路径从Pt/SSZ-13上的NH机理转变为PtCu/SSZ-13催化剂上的NH和内部选择性催化还原机理,这被认为是氮选择性提高的主要原因。这项工作为合成高效合金催化剂提供了一条新途径,以优化用于柴油废气净化中控制氨泄漏的NH-SCO的氮选择性。