Liu Jianhua, Xu Guangyan, An Qi, Wang Yingjie, Yu Yunbo, He Hong
School of Rare Earths, University of Science and Technology of China, Hefei 230026, China.
Ganjiang Innovation Academy, Chinese Academy of Sciences, Ganzhou 341000, China.
ACS Omega. 2023 Apr 6;8(15):13944-13954. doi: 10.1021/acsomega.3c00381. eCollection 2023 Apr 18.
Ammonia selective catalytic oxidation (NH-SCO) is a commercial technology applied to diesel vehicles to eliminate ammonia leakage. In this study, a series of Pt/AlO catalysts were synthesized by an impregnation method, and the state of Pt species was carefully adjusted by heat treatment. These Pt/AlO catalysts were further systematically characterized by Brunauer-Emmett-Teller, X-ray diffraction, X-ray photoelectron spectroscopy, X-ray absorption fine structure, UV-vis, H-tempertaure-programmed reduction, and NH-temperature-programmed desorption. The characterization results showed that dispersed oxidized Pt species were present on conventional Pt/AlO samples, while high-temperature treatment induced the aggregation of platinum species to form metallic Pt nanoparticles. The Pt/AlO catalysts treated at high temperatures showed superior activity and water tolerance in the NH-SCO reaction. Diffuse reflectance infrared Fourier-transform spectroscopy combined with mass spectrometry experiments revealed that the Lewis acid sites were more reactive than the Brønsted acid sites. Moreover, compared to oxidized Pt species, metallic Pt nanoparticles were beneficial for oxygen activation and were less affected by water vapor, thus contributing to the superior activity and water tolerance of Pt/Al-800.
氨选择性催化氧化(NH-SCO)是一种应用于柴油车辆以消除氨泄漏的商业技术。在本研究中,通过浸渍法合成了一系列Pt/AlO催化剂,并通过热处理仔细调整了Pt物种的状态。这些Pt/AlO催化剂进一步通过布鲁诺尔-埃米特-特勒法、X射线衍射、X射线光电子能谱、X射线吸收精细结构、紫外可见光谱、H程序升温还原和NH程序升温脱附进行了系统表征。表征结果表明,常规Pt/AlO样品上存在分散的氧化态Pt物种,而高温处理导致铂物种聚集形成金属Pt纳米颗粒。高温处理的Pt/AlO催化剂在NH-SCO反应中表现出优异的活性和耐水性。漫反射红外傅里叶变换光谱结合质谱实验表明,路易斯酸位点比布朗斯特酸位点更具反应活性。此外,与氧化态Pt物种相比,金属Pt纳米颗粒有利于氧的活化,且受水蒸气的影响较小,从而有助于Pt/Al-800具有优异的活性和耐水性。