Gao Xiaohui, Bai Yuting, Zhang Hao, Wang Xingyi
Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, PR China.
ACS Omega. 2023 Feb 8;8(7):6791-6800. doi: 10.1021/acsomega.2c07399. eCollection 2023 Feb 21.
Pt species with different chemical states and structures were supported on CeO by solution reduction (Pt/CeO-SR) and wet impregnation (Pt/CeO-WI) and investigated in catalytic oxidation of -decane (CH), -hexane (CH), and propane (CH). Characterization by X-ray diffraction, Raman spectroscopy, X-ray photoelectron spectroscopy, H-temperature programming reduction, and oxygen temperature-programmed desorption showed that Pt and Pt existed on Pt nanoparticles of the Pt/CeO-SR sample, which promoted redox, oxygen adsorption, and activation. On Pt/CeO-WI, Pt species were highly dispersed on CeO as the Pt-O-Ce structure, in which surface oxygen decreased significantly. The Pt/CeO-SR catalyst presents high activity in oxidation of CH with a rate of 0.164 μmol min m at 150 °C. The rate increased with oxygen concentration. Moreover, Pt/CeO-SR presents high stability on feed stream containing 1000 ppm CH at gas hour space velocity = 30,000 h as low as 150 °C for 1800 min. The low activity and stability of Pt/CeO-WI were probably related to its low availability of surface oxygen. In situ Fourier transform infrared results showed that the adsorption of alkane occurred through the interaction with Ce-OH. The adsorption of CH and CH was much weaker than that of CH, which resulted in the decrease in activity for CH and CH oxidation of Pt/CeO catalysts.
通过溶液还原法(Pt/CeO-SR)和湿浸渍法(Pt/CeO-WI)将具有不同化学状态和结构的铂物种负载在CeO上,并对其在癸烷(C₁₀H₂₂)、己烷(C₆H₁₄)和丙烷(C₃H₈)催化氧化中的性能进行了研究。通过X射线衍射、拉曼光谱、X射线光电子能谱、氢气程序升温还原和氧气程序升温脱附表征表明,Pt/CeO-SR样品的铂纳米颗粒上存在Pt⁰和Pt²⁺,这促进了氧化还原、氧吸附和活化。在Pt/CeO-WI上,铂物种以Pt-O-Ce结构高度分散在CeO上,其中表面氧显著减少。Pt/CeO-SR催化剂在150℃下对C₃H₈氧化具有高活性,速率为0.164 μmol min⁻¹ m⁻²。该速率随氧浓度增加。此外,Pt/CeO-SR在气体时空速 = 30,000 h⁻¹、含有10,000 ppm C₃H₈的进料流中,在低至150℃的温度下保持1800分钟时表现出高稳定性。Pt/CeO-WI的低活性和稳定性可能与其表面氧的低可用性有关。原位傅里叶变换红外结果表明,烷烃的吸附是通过与Ce-OH的相互作用发生的。C₁₀H₂₂和C₆H₁₄的吸附比C₃H₈弱得多,这导致Pt/CeO催化剂对C₁₀H₂₂和C₆H₁₄氧化的活性降低。