低碳化学与化工2024，Vol.49Issue(11)：43-49,69,8.DOI:10.12434/j.issn.2097-2547.20240119
Ru@Alx-mSiO2中空介孔核壳型催化剂苯酚加氢脱氧制苯性能研究
Study on performances of Ru@Alx-mSiO2 hollow mesoporous core-shell catalysts for phenol hydrodeoxygenation to benzene
摘要
Abstract
In order to address the issue of poor stability of loaded Ru catalysts in the hydrodeoxygenation reaction of phenolic compounds,a series of hollow mesoporous core-shell catalysts,Ru@Alx--mSiO2(x=0.5,1.0,1.5 or 2.0),with varying Al loadings(mass fractions)were prepared by selective etching under alkaline conditions with Ru-containing silica microspheres(Ru@SiO2)as the precursor and sodium meta-aluminate(NaAlO2)as the aluminum source.The microstructures and physicochemical properties of the catalysts were characterized by TEM,HAADF-STEM,XRD,N2 adsorption/desorption,NH3-TPD and H2-TPD.The catalytic performances of Ru@Alx-mSiO2 catalysts were investigated using phenol hydrodeoxygenation to prepare benzene as a model reaction.The results show that the incorporation of Al into Ru@mSiO2 under the reaction conditions of 60 ℃ and 2.0 MPa can significantly improve the selectivity of benzene.This is attributed to the fact that the Al loading provideds abundant acidic sites,which can not only assist the dissociation of HI2 from the metal Ru to increase the phenol hydrogenation activity,but also enhance the deoxygenation of phenol and thus improve the benzene selectivity.Among all the catalysts,Ru@Al1.0-mSiO2 exhibits the highest phenol conversion(80.5％)and benzene selectivity(96.5％),which is attributed to the synergistic effect between the Ru metal and the silicoaluminate shell layer.Furthermore,the hollow mesoporous silica-aluminate shell layer exhibites a domain-limiting protective effect,and Ru@Al1.0-mSiO2 still exhibits excellent stability in multiple catalytic cycle hydrodeoxygenation experiments.关键词
酚类化合物/Ru基核壳型催化剂/苯酚/加氢脱氧/苯Key words
phenolic compound/Ru-based core-shell catalysts/phenol/hydrodeoxygenation/benzene分类
化学化工引用本文复制引用
钟梦宇,于洪波,周永柱,尹宏峰..Ru@Alx-mSiO2中空介孔核壳型催化剂苯酚加氢脱氧制苯性能研究[J].低碳化学与化工,2024,49(11):43-49,69,8.基金项目
国家自然科学基金(22072171) （22072171）
天津市教委科研计划项目(2017KJ064). （2017KJ064）
