摘要
以UiO-66为前体,在N_(2)气氛下焙烧制备了ZrO_(2)@C,以其为载体,利用浸渍法制备了Pd/ZrO_(2)@C催化剂。以Pd/ZrO_(2)@C+SO_(4)^(2-)/ZrO_(2)为催化剂,对以甲酸(FA)为氢源、硝基苯(NB)转移加氢合成对氨基苯酚(PAP)的反应进行了研究。通过表征发现,Pd/ZrO_(2)@C载体中的ZrO_(2)为四方相ZrO_(2),包埋在无定形C中。随着ZrO_(2)@C在空气中焙烧温度的升高和焙烧时间的增加,其C含量和比表面积随之下降,同时Pd颗粒尺寸变大。Pd/ZrO_(2)@C催化剂中Pd以Pd^(0)和Pd^(2+)两种形式存在,且随着C含量的减少,Pd^(0)含量增加,Pd^(2+)含量减少;当Pd^(0)含量明显高于Pd^(2+),其对PAP的选择性明显下降。在140℃、反应6h的条件下,Pd/ZrO_(2)@C-200-4+SO_(4)^(2-)/ZrO_(2)具有较好的催化性能,NB转化率为63.7%,PAP选择性为42.3%。
With UiO-66 as the precursor,ZrO_(2)@C was prepared by calcination in N_(2) atmosphere.Then,Pd/ZrO_(2)@C was prepared by impregnation method.In this paper,the catalytic transfer hydrogenation of nitrobenzene(NB)to p-aminophenol(PAP)over Pd/ZrO_(2)@C+SO_(4)^(2-)/ZrO_(2)was studied with formic acid(FA)as hydrogen source.Characterization results showed that tetragonal ZrO_(2)was present in ZrO_(2)@C and was embedded in amorphous C.With the increase of calcination temperature and time in the air,the C content and specific surface area of ZrO_(2)@C decreased accordingly,while the Pd particle size became larger.Pd in the Pd/ZrO_(2)@C catalyst was in the form of Pd^(0)and Pd^(2+).The content of Pd^(2+)decreased with C content,While the content of Pd^(0)increased.When the content of Pd^(0)was higher than that of Pd^(2+),PAP selectivity decreased obviously.Pd/ZrO_(2)@C-200-4+SO_(4)^(2-)/ZrO_(2)exhibited good catalytic activity at 140℃for 6h.The conversion of NB was 63.7%and the selectivity of PAP was 42.3%.
作者
王雨菲
贾宇
张议升
薛伟
李芳
王延吉
WANG Yufei;JIA Yu;ZHANG Yisheng;XUE Wei;LI Fang;WANG Yanji(Hebei Provincial Key Laboratory of Green Chemical Technology and High Efficient Energy Saving,School of Chemical Engineering and Technology,Hebei University of Technology,Tianjin 300400,China;Tianjin Key Laboratory of Chemical Process Safety,Tianjin 300400,China;Hebei Industrial Technology Research Institute of Green Chemical Industry,Cangzhou 061000,Hebei,China)
出处
《化工进展》
EI
CAS
CSCD
北大核心
2024年第8期4421-4431,共11页
Chemical Industry and Engineering Progress
基金
国家自然科学基金(U21A20306,U20A20152)
河北省自然科学基金(B2022202077)。
关键词
催化
加氢
载体
对氨基苯酚
甲酸
硝基苯
catalysis
hydrogenation
support
p-aminophenol
formic acid
nitrobenzene
