| 项双龙,杨小俊,张育莲,熊春荣.椰壳活性炭共价固载钯离子有机络合物催化剂的制备与应用[J].分子催化,2013,(1):55-62 |
| 椰壳活性炭共价固载钯离子有机络合物催化剂的制备与应用 |
| Preparation and Application of Coconut Shell Activated Carbon Covalently Immobilized Palladium Complexes |
| 投稿时间：2012-12-14 修订日期：2013-01-19 |
| DOI： |
| 中文关键词: 椰壳活性炭 共价固载 钯离子有机络合物 氧化羰基化 碳酸二苯酯 |
| 英文关键词:Coconut shell activated carbon Covalently immobilize Palladium ions complex Oxidative carboxylation Diphenyl carbonate |
| 基金项目:国家自然科学基金, 国家教育部和国家人事部留学回国人员基金 |
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| 中文摘要: |
| 采用椰壳活性炭为载体, 通过20% HNO3氧化处理, Boehm滴定表明活性炭表面羟基含量达到0.376 mmol/g. 之后分别接枝(MeO)3Si(CH2)3NH2和(MeO)3Si(CH2)3Cl, 并成功合成了两种不同类型的含氮双齿配体用来络合钯离子, 以FT-IR、XPS、1H NMR、ICP及N2吸附-脱附等手段表征了催化剂制备过程中的各种中间体. 在高压反应釜中以苯酚氧化羰基化反应考察了所制催化剂的催化性能. 结果表明, 在100 ℃, 7.0 MPa及p(CO)/p(O2)=10/1下, 二氯甲烷为溶剂, 以环庚二胺配体络合的钯离子为催化剂, 苯酚转化率及产物碳酸二苯酯(DPC)选择性分别为11.91%、86.82%, 对于双氰基配体络合的催化剂, 苯酚转化率及产物DPC选择性分别为6.22%及81.02%. |
| 英文摘要: |
| Coconut shell activated carbon (AC) was used as carrier to covalently immobilize Pd2 complexes. Boehm titration showed that hydroxyl content of the carbon surface reached 0.376 mmol/g after 20% HNO3 oxidation treatment. Two types of nitrogen-containing bidentate ligands were subsequently synthesized by grafting the oxidized AC with (MeO)3Si(CH2)3NH2 or (MeO)3Si(CH2)3Cl. The samples were characterized by FT-IR, XPS, 1H NMR, ICP and N2 adsorption-desorption. CH2Cl2 was used as solvent, oxidative carbonylation of phenol was investigated in a high pressure reaction vessel at 100 ℃, 7.0 Mpa and p(CO)/p(O2) = 10/1 over the immobilized Pd2 complexes. The results show that the conversion rate of phenol was 11.91%, and the diphenyl carbonate (DPC) selectivity was 86.82% for the cycloheptyl diamine ligand-complexed palladium ions. Comparatively, the bis-nitrile ligand-complexed ones displayed a phenol conversion rate of 6.22% and a DPC selectivity of 81.02%. |
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