摘要
采用无酸性的α-Al_(2)O_(3)为载体,预先沉积WO_(3)然后浸渍法负载Pt物种,合成了系列Pt-WO_(3)/α-Al_(2)O_(3)催化剂用于萘深度加氢反应,系统地研究了氧化钨物种在萘加氢反应中的作用。通过XRD、Raman、HRTEM、XPS和H2-TPR技术表征了Pt和WO_(3)物种在载体表面的分散情况和状态,并利用Py-IR研究了载体负载氧化钨和Pt前后的酸性质变化。在温和的反应条件下(70℃、3 MPa、1 h)Pt-WO_(3)/α-Al_(2)O_(3)催化剂表现出优异的萘深度加氢活性,萘的转化率和十氢萘的选择性均达到100%。结果表明,预先在载体表面引入的WO_(3)和Pt产生了强相互作用,WO_(3)提高了Pt物种的分散程度,催化剂的酸性来源于氧化钨物种的引入且和负载量成正比关系。催化剂较强的酸性和较高的Pt分散程度是Pt-WO_(3)/α-Al_(2)O_(3)在低温条件下能够使萘深度加氢的关键因素,对于十氢萘作为储氢介质工艺具有重要的意义。
Pt-WO_(3)/α-Al_(2)O_(3) catalysts were prepared with sequential impregnation of WO_(3) and then Pt inα-Al_(2)O_(3) supports without acid sites.The as-prepared were investigated the promotion of WO_(3) catalysts in the reaction of hydrogenation of naphthene at mild reaction conditions.XRD,Raman,HRTEM,XPS,and H2-TPR analyses reveal the basic structure and distribution of Pt and WO_(3) species.Py-IR analyses reveal that the changing of acid sites after loading Pt and WO_(3) species.Pt-WO_(3)/α-Al_(2)O_(3) catalysts have shown excellent catalytic performance for the hydrogenation of naphthalene to decalin at mild reaction conditions(70℃,3 MPa,1 h)with the conversion and selectivity of decalin are 100%.Combined with the characterization and catalytic performance,the pre-introduced Pt and WO_(3) species caused the strong interaction between Pd sites and WO_(3) and the efficient distribution of Pt by WO_(3) species.The strong acidity of the catalyst and the high degree of Pt dispersion are the key factors for the deep hydrogenation of naphthalene by Pt-WO_(3)/α-Al_(2)O_(3) under low temperature conditions,which is of great significance for the process of decalin as a hydrogen storage medium.
作者
梁瑜
赵彤
赵斌彬
刘雷
董晋湘
唐明兴
李学宽
LIANG Yu;ZHAO Tong;ZHAO Binbin;LIU Lei;DONG Jinxiang;TANG Mingxing;LI Xuekuan(College of Chemistry and Chemical Engineering,Taiyuan University of Technology,Taiyuan 030024,Shanxi,China;Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,Shanxi,China)
出处
《化工学报》
EI
CAS
CSCD
北大核心
2021年第11期5643-5652,共10页
CIESC Journal
基金
国家自然科学基金项目(U1910202,21978194)
山西省“1331工程”项目
山西省青年三晋学者支持计划项目。
关键词
萘
十氢萘
载体
氧化钨
加氢
催化剂
naphthalene
decalin
support
tungsten oxide
hydrogenation
catalyst
