氟化铵对CoMoS/ZrO_(2)催化4-甲基酚加氢脱氧性能的影响  

Effect of ammonium fluoride on performance of CoMoS/ZrO_(2)in catalyzing hydrodeoxygenation of 4-methylphenol

作　　者：李志勤[1] 任枭雄 李宗轩 邱泽刚[1] LI Zhi-qin;REN Xiao-xiong;LI Zong-xuan;QIU Ze-gang(Xi'an Shiyou University,Xi'an 710065,China)

机构地区：[1]西安石油大学,陕西西安710065

出　　处：《现代化工》2022年第10期135-139,144,共6页Modern Chemical Industry

基　　金：国家自然科学基金(21878243);陕西省重点研发计划(2022GY-153);省部共建煤炭高效利用与绿色化工国家重点实验室开放课题(2022-K50)。

摘　　要：芳环直接加氢脱氧(DDO)制芳烃是低价值酚类高值利用的重要途径,而CoMoS/ZrO_(2)可促进酚类DDO反应。利用不同制备方法和引入NH_(4)F来调节CoMoS/ZrO_(2)的结构和性质。结果表明,引入NH_(4)F并通过F^(-)、Zr^(4+)和OH^(-)协同作用,可诱导催化剂形貌有序变化,提高m-ZrO_(2)(单斜相)结晶度和表面Co、Mo质量分数,使颗粒变均匀、孔分布集中。F^(-)与Zr^(4+)摩尔比为1.3时,CoMoS/ZrO_(2)为均匀规则梭状颗粒且表面平滑,具有较高结晶度、活性组分质量分数和适宜孔分布,使4-甲基酚转化率高达99.7%,甲苯选择性高达92.4%。Direct hydrodeoxygenation(DDO)of aromatic ring to aromatics is an important way for high-value utilization of low-value phenols.CoMoS/ZrO_(2) can promote the DDO reaction of phenols.The structure and properties of CoMoS/ZrO_(2) are regulated by means of different preparation methods and the addition of ammonium fluoride.It is indicated that the addition of ammonium fluoride together with the synergistic effect among F^(-),Zr^(4+)and OH^(-)can induce the morphology of catalyst to change orderly,which improves the crystallinity of m-ZrO_(2)(monoclinic phase)and the contents of Co and Mo on the catalyst surface.Furthermore,the particles of catalyst become uniform and the pore distribution becomes more concentrated.As the molar ratio of F^(-)to Zr^(4+)is 1.3,CoMoS/ZrO_(2) appears as uniform and regular shuttle particles,and has smooth surface,high crystallinity,high active component content and suitable pore distribution,over which the conversion of 4-methylphenol can reach as high as 99.7%and the selectivity of toluene achieves as high as 92.4%.

关 键 词：酚 加氢脱氧 水热法 二氧化锆 COMO 氟化铵 

分 类 号：TQ032[化学工程]