Highly Dispersed Copper Species within SBA-15 Introduced by the Hydrophobic Core of a Surfactant Micelle as a Carrier and Their Enhanced Catalytic Activity for Cyclohexane Oxidation

被引:42
作者
Gu, Jinlou [1 ]
Huang, Ying [1 ]
Elangovan, S. P. [2 ]
Li, Yongsheng [1 ]
Zhao, Wenru [1 ]
Toshio, Iijima [2 ]
Yamazaki, Yasuo [2 ]
Shi, Jianlin [1 ,3 ]
机构
[1] E China Univ Sci & Technol, Sch Mat Sci & Engn, Minist Educ, Key Lab Ultrafine Mat, Shanghai 200237, Peoples R China
[2] Nippon Chem Ind Co Ltd, Koto Ku, Tokyo 1368515, Japan
[3] Chinese Acad Sci, Shanghai Inst Ceram, State Key Lab High Performance Ceram & Superfine, Shanghai 200050, Peoples R China
关键词
ORDERED MESOPOROUS MATERIALS; AEROBIC OXIDATION; SELECTIVE OXIDATION; LIQUID-PHASE; SILICA; BEHAVIOR; HYDROGENATION; PHENOL; OXYGEN; EPOXIDATION;
D O I
10.1021/jp206132a
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
Highly dispersed copper species were successfully coated onto the inner surface of the rodlike mesoporous SBA-15 silica by a newly developed strategy. The hydrophobic core of the surfactant micelle in the as-synthesized SBA-15 was effectively employed as a carrier for the hydrophobic precursors of copper acetyl acetonate (Cu(acac)(2)) during hydrothermal treatment (HT) before surfactant removal, and the copper-derivated catalysis centers within SBA-15 were strategically generated on pyrolysis. Characterizations of the synthesized samples by a series of techniques such as X-ray diffraction (XRD), transmission electron microscopy (TEM), Brunauer-Emmett-Teller (BET), electron paramagnetic resonance (EPR), temperature-programmed reduction (TPR), UV-vis, X-ray photoelectron spectroscopy (XPS), and inductively coupled plasma atomic emission spectroscopy (ICP-AES) manifested that about 0.19-0.85 wt % copper was directly introduced and dispersed into the inner surface of the SBA-15 pore network. While there were few studies, if any, to utilize synthetic copper catalysts for the selective oxidation of cyclohexane oxidation, it was found that currently synthesized Cu-SBA-15 demonstrated very interesting catalytic properties for this industrially important reaction. Under the optimized reaction condition at an oxygen pressure of 1 MPa and a temperature of 120 degrees C for 7 h, the conversion of cyclohexane to the target products was higher than 11%; meanwhile, the total selectivity to cyclohexanol and cyclohexanone satisfactorily reached ca. 80%.
引用
收藏
页码:21211 / 21217
页数:7
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