摘要
以氢氧化镍为镍源,亚磷酸为磷源,TiO2柱撑海泡石(Ti-Sep)为载体,采用浸渍法制备了含磷化镍前驱体的样品,然后采用程序升温还原法制备了Ni质量分数(w)为5%-25%的Ni2P/Ti-Sep催化剂,并考察了其噻吩加氢脱硫性能.采用X射线衍射(XRD)、N2吸附-脱附、热重分析(TGA)、透射电子显微镜(TEM)和傅里叶变换红外(FTIR)光谱对催化剂样品进行了表征.结果表明,海泡石经TiO2柱撑之后层间距增大,比表面积和孔容都明显变大,热稳定性增强,活性组分Ni2P能很好地分散在海泡石层间及表面,并且没有破坏海泡石的层状结构.上述原因导致Ni2P/Ti-Sep催化剂的噻吩加氢脱硫活性明显优于Ni2P/Na-Sep(NaCl改性海泡石)和Ni2P/HCl-Sep(HCl改性海泡石)催化剂.当Ni负载量为15%(w)时,Ni2P/Ti-Sep催化剂具有最好的噻吩加氢脱硫性能;在反应温度为400°C时,噻吩转化率达100%.
Samples containing a nickel phosphide precursor were synthesized by the impregnation method using TiO2-pillared sepiolite （Ti-Sep） as a support, nickel hydroxide as a nickel source, and phosphorous acid as a phosphorus source. From these precursor samples, Ni2P/Ti-Sep catalysts with Ni content ranging from 5%-25% （w, mass fraction） were prepared by temperature-programmed reduction. Thiophene hydrodesulfurization （HDS） was used to investigate the HDS activity of the catalysts. The catalysts were characterized by X-ray powder diffraction （XRD）, N2 adsorption-desorption, thermal gravity analysis （TGA）, transmission electron microscope （TEM）, and Fourier transform infrared spectroscopy （FTIR）. The results demonstrated that the specific surface area and pore volume of Ti-Sep were enlarged and catalyst thermal stability was improved. In addition, the layer spacing of sepiolite was also increased. As a consequence, the active component, Ni2P, can be well dispersed on the interlayer and outer surface of Ti-Sep. Moreover, the layered sepiolite structure remained intact in the Ni2P/Ti-Sep catalysts. Consequently, thiophene conversion on Ni2PFFi-Sep is improved compared with Ni2P/Na-Sep （NaCI-modified sepiolite） and Ni2P/HCl-Sep （HCI-modified sepiolite）, which were prepared on sepiolite without Ti-pillaring. Ni2P/Ti-Sep with a Ni loading of 15% （w） shows the highest activity among all of thestudied catalysts, on which the conversion of thiophene can reach 100% at 400 ℃.
出处
《物理化学学报》
SCIE
CAS
CSCD
北大核心
2012年第12期2924-2930,共7页
Acta Physico-Chimica Sinica
基金
国家自然科学基金(20863006)
南昌大学"赣江"特聘教授启动基金资助项目~~
