磁各向异性催化剂制备及其磁稳定床加氢催化研究

Magnetic catalyst holds important interest and potential application value in both environmental protection and green catalysis areas. However, there are problems of low magnetization and low working temperature for the magnetic isotropic catalyst. In this project we will synthesize well dispersed rod shape γ-Fe2O3 with shape anisotropic core by surface modification and surface coating, and analyze the orientation behavior by oil column method combination with magnetic field, then build the orientation mechanisms between magnetic anisotropy of carrier and the forming temperature, sol viscosity, gelling speed in order to improve magnetic and thermal properties. The final magnetic anisotropic carrier has excellent temperature magnetic properties, chemical stability and easy to magnetic separation, owning doubled residual magnetization and enhanced magnetic susceptibility. Moreover, hydrogenation of benzene to cyclohexane in magnetically stabilized bed will be studied to settle overheating of fixed reaction bed, and explore the matching laws between the magnetic anisotropic carrier and bed operating conditions (magnetic field, liquid space velocity, ratio of hydrogen to benzene). This work not only explores a new method for the preparation of the high response magnetic carrier, but also builds foundation for further development of magnetic catalyst. This study should be also valuable for vital application and academic significance.

磁性催化剂具有优异的催化和磁响应特性，越来越多的受到研究者关注，但目前这类催化剂普遍为磁各向同性催化剂。本项目采用具有形状各向异性的棒状γ-Fe2O3作为磁核，经表面改性、包覆后，通过自制的磁场油柱成型装置，利用纵向磁场控制载体的成型过程，建立磁各向异性载体与溶胶粘度、油柱成型温度、胶凝速度等参数的对应调控机制，进而获得磁各向异性催化剂载体，与磁各向同性载体相比剩余磁化强度可提高近一倍。将该高磁响应特性载体负载活性组分，在磁稳定床中进行苯加氢制环己烷催化，研究与该载体相匹配的磁床加氢参数（磁场强度、液体空速、氢苯比等）控制机制，解决固定床反应床层局部过热问题，提高催化剂寿命，同时高磁响应催化剂也可降低磁场能耗。该磁各向异性载体具有出色的磁响应特性和化学稳定性，易于磁分离、磁控制。该研究为制备高磁响应催化剂提供了新的方法，也为磁性催化剂的进一步发展奠定基础，具有较重要应用价值和学术意义

磁性催化剂被广泛应用于工业催化领域，但也存在着载体磁化强度较小、适用催化反应温度偏低的问题。本项目采用具有耐高温的形状各向异性棒状γ-Fe2O3作为磁核，对其进行表面氧化硅的改性、包覆，然后通过自制磁场油柱成型装置控制载体的成型过程，分析磁核取向行为的影响机制，进而获得了磁各向异性球形氧化铝载体的制备方法，其比饱和磁化强度高温下达到12.3 emu/g，易于回收。该载体负载活性组分Ni-B后，在磁稳定床中进行苯加氢制环己烷催化研究，使其产率提高，解决了床层局部过热问题，避免了停车，并提高催化剂寿命，方便磁场回收利用。该载体的剩余磁化强度提高了一倍，磁化率大幅提升，具有出色的耐高温磁特性和化学稳定性，也易于磁分离、磁控制。该工作为制备高温度磁响应特性载体提供了新的方法，也为磁性催化剂的发展奠定基础，具有重要应用价值和学术意义。项目发表文章19篇，其中被SCI收录 14篇，EI收录2篇，一区top 期刊3篇，二区 3篇，授权国家发明专利10项。获青岛市技术发明二等奖，青岛市青年科技奖，青岛西海岸新区优秀青年人才称号。