
科学技术与工程

中国技术经济学会
面向氨燃料发动机废气N2O去除的Cu/TiO2催化剂的性能及催化机理
Performance and Catalytic Mechanism of Cu/TiO2 Catalyst for Removal of N2O from Exhaust Gas of NH3-fuel Engines
推动绿氨燃料上船应用已被普遍认为是实现全球航运业绿色低碳转型可行途径。然而,船用氨燃料发动机存在的N2O排放问题已成为阻碍氨动力船舶发展的关键技术瓶颈之一。针对这一问题,采用浸渍法制备出一系列以TiO2为载体的过渡金属氧化物催化剂,考察了过渡金属元素类型对催化剂N2O去除性能的影响,并研究获得了性能优化的Cux/TiO2催化剂。结果表明,与Fe5/TiO2、Mn5/TiO2、Co5/TiO2、Ni5/TiO2催化剂相比,Cu5/TiO2催化剂显示出优异的催化活性,其N2O转化率可在350 ℃达到100%。除此之外,Cu5/TiO2催化剂还具有良好的抗水性能。5%是最佳的铜负载量。采用X射线衍射、N2吸附脱附、H2程序升温还原、O2程序升温脱附、原位漫反射傅里叶变换红外光谱等表征手段对性能较优的Cu5/TiO2催化剂的物化性质和表面反应中间体进行了表征,从多角度深入讨论了相关催化反应机理。结果显示,与其他Cux/TiO2催化剂相比,Cu5/TiO2催化剂具有较高的活性物种分散度、比表面积、氧空位含量以及较强的氧化还原性能,有利于其展现出较优的催化活性。Cu5/TiO2催化剂表面的主要活性物种为Cu2+和Cu+,N2O的吸附和解离是催化反应的关键步骤。
The application of green NH3-fuel on board has been widely regarded as a feasible way to realize the green and low-carbon transformation of the global shipping industry. However, the N2 O emission problem of marine NH3-fuel engines has become one of the key technical bottlenecks hindering the development of ammonia-powered ships. To solve this problem, a series of TiO2-supported transition metal oxide catalysts were prepared by impregnation method. The effect of transition metal element types on the N2O removal performance of the catalysts was investigated, and the N2O removal performance of Cux/TiO2 catalysts was optimized. The results show that compared with Fe5/TiO2, Mn5/TiO2, Co5/TiO2 and Ni5/TiO2 catalysts, Cu5/TiO2 catalyst shows excellent catalytic activity, the N2O conversion efficiency can reach 100% at 350 ℃. In addition, Cu5/TiO2 catalyst also has good water resistance. The experimental results show that 5% is the best Cu loading amount. X-ray diffraction, N2 adsorption-desorption, H2 temperature programmed reduction, O2 temperature programmed desorption, and in-situ diffuse reflectance infrared Fourier transform spectroscopy were used to characterize the physicochemical properties and surface reaction intermediates of Cu5/TiO2 catalyst, and the relevant catalytic reaction mechanisms were discussed in depth from multiple perspectives. The characterization results show that compared with other Cux/TiO2 catalysts, Cu5/TiO2 catalyst has higher dispersion of active species, specific surface area, oxygen vacancy content and stronger redox performance, which is conducive to its better catalytic activity. The main active species on the surface of Cu5/TiO2 catalyst are Cu2+and Cu+ species, and the adsorption and deionization of N2O is a key step in the catalytic reaction.
氨燃料发动机 / 废气处理 / Cu/TiO2催化剂 / N2O催化分解
NH3-fuel engine / exhaust gas treatment / Cu/TiO2 catalyst / catalytic decomposition of N2O
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