Hydroxylation of Benzene over V-HMS Catalysts with the Addition of Fe as the Second Metal Component

被引:14
作者
Feng Su-Jiao [1 ]
Yue Bin [1 ]
Wang Yu [1 ]
Ye Lin [1 ]
He He-Yong [1 ]
机构
[1] Fudan Univ, Dept Chem, Shanghai Key Lab Mol Catalysis & Innovat Mat, Shanghai 200433, Peoples R China
基金
国家高技术研究发展计划(863计划);
关键词
Iron; Vanadium; Mesoporous silica; Benzene; Hydroxylation; Phenol; LIQUID-PHASE OXIDATION; SELECTIVE OXIDATION; AROMATIC-HYDROCARBONS; MESOPOROUS SILICA; HYDROGEN-PEROXIDE; MOLECULAR-OXYGEN; PHENOL SYNTHESIS; OXIDE CATALYSTS; PERFORMANCE; SIEVES;
D O I
10.3866/PKU.WHXB20112881
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Second metals (Fe, Al, Cu, Ni, Co, Mo, Cr) were incorporated into V-HMS catalyst by impregnation to enhance the catalytic activity for the hydroxylation of benzene with hydrogen peroxide as the oxidant. Among the studied second metals, Fe was found to be effective in improving the catalytic performance. Therefore, we synthesized a series of Fe(x)V(x)-HMS catalysts containing different amounts of Fe and V by the co-synthesis method. The catalysts were characterized by powder X-ray diffraction (XRD), N(2), physisorption, transmission electron microscopy (TEM), NH(3) temperature-programmed desorption (NH(3)-TPD), and H(2) temperature-programmed reduction (H(2)-TPR). The characterization results show that the mesoporous structure of HMS is maintained and the addition of Fe creates new acid sites and a stronger redox ability. Catalytic tests show that vanadium species are the active species and that the iron species promote the reaction. Under optimal reaction conditions, the Fe(0.04)V(0.06)-HMS catalyst gives the best catalytic performance with a highest phenol yield of 18.1% by comparison with 13.1% over the Fe-free catalyst Fe(0.00)V(0.06)-HMS. We propose a possible mechanism involving the Fe and V species for the hydroxylation of benzene with H(2)O(2) as the oxidant.
引用
收藏
页码:2881 / 2886
页数:6
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