摘要
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N_(2)O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TiO_(2)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N_(2)O去除性能的影响,并研究获得了性能优化的Cu_(x)/TiO_(2)催化剂。结果表明,与Fe_(5)/TiO_(2)、Mn_(5)/TiO_(2)、Co_(5)/TiO_(2)、Ni_(5)/TiO_(2)催化剂相比,Cu_(5)/TiO_(2)催化剂显示出优异的催化活性,其N_(2)O转化率可在350℃达到100%。除此之外,Cu_(5)/TiO_(2)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、N_(2)吸附脱附、H_(2)程序升温还原、O_(2)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Cu_(5)/TiO_(2)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Cu_(x)/TiO_(2)催化剂相比,Cu_(5)/TiO_(2)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。Cu_(5)/TiO_(2)催化剂表面的主要活性物种为Cu^(2+)和Cu^(+),N_(2)O的吸附和解离是催化反应的关键步骤。
The application of green NH_(3)-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 N_(2)O emission problem of marine NH_(3)-fuel engines has become one of the key technical bottlenecks hindering the development of ammonia-powered ships.To solve this problem,a series of TiO_(2)-supported transition metal oxide catalysts were prepared by impregnation method.The effect of transition metal element types on the N_(2)O removal performance of the catalysts was investigated,and the N_(2)O removal performance of Cu_(x)/TiO_(2)catalysts was optimized.The results show that compared with Fe_(5)/TiO_(2),Mn 5/TiO_(2),Co 5/TiO_(2)and Ni 5/TiO_(2)catalysts,Cu_(5)/TiO_(2)catalyst shows excellent catalytic activity,the N_(2)O conversion efficiency can reach 100%at 350℃.In addition,Cu_(5)/TiO_(2)catalyst also has good water resistance.The experimental results show that 5%is the best Cu loading amount.X-ray diffraction,N_(2)adsorption-desorption,H_(2) temperature programmed reduction,O_(2)temperature programmed desorption,and in-situ diffuse reflectance infrared Fourier transform spectroscopy were used to characterize the physicochemical properties and surface reaction intermediates of Cu_(5)/TiO_(2)catalyst,and the relevant catalytic reaction mechanisms were discussed in depth from multiple perspectives.The characterization results show that compared with other Cu_(x)/TiO_(2)catalysts,Cu_(5)/TiO_(2)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 Cu_(5)/TiO_(2)catalyst are Cu^(2+)and Cu^(+) species,and the adsorption and deionization of N_(2)O is a key step in the catalytic reaction.
作者
高宇
李坤
GAO Yu;LI Kun(China Waterborne Transport Research Institute,Beijing 100088,China)
出处
《科学技术与工程》
北大核心
2025年第13期5681-5688,共8页
Science Technology and Engineering
基金
国家重点研发计划(2021YFB2601601)
交通运输部水运科学研究院基本科研业务费项目(72404)。
作者简介
第一作者:高宇(1993-),男,汉族,内蒙古鄂尔多斯人,博士,助理研究员。研究方向:新能源清洁能源船舶。E-mail:gaoyu@wti.ac.cn。;通信作者:李坤(1987-),男,汉族,河南商丘人,硕士,副研究员。研究方向:新能源清洁能源船舶。E-mail:likun@wti.ac.cn。
