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第 39 卷第 6 期Vol. 39 No. 6
2009 年 12 月Dec 2009

所屬欄目:功能材料

Salen-Co配合物在核-殼結構的Silica上的接枝及催化性能的研究
周建波,伏再輝,曾 明,曾小軍,崔小瑩 (長(cháng)沙醫學(xué)院,湖南 長(cháng)沙 410219)
摘 要:分別以球狀納米silica和懸浮聚合法制備的核-殼型silica -苯乙烯與丙烯酸甲酯共聚物雜化體為載體,采用化學(xué)接枝方法,制備了Salen-Co配合物固載型催化劑。采用FT-IR、TG-DTA和TEM對這些催化劑進(jìn)行了表征。結果表明:核-殼型催化劑其殼層性質(zhì)可通過(guò)改變兩個(gè)單體的比例來(lái)調變,隨單體丙烯酸甲酯比例的增加,殼層由聚苯乙烯占優(yōu)逐漸過(guò)渡到以聚丙烯酸甲酯為主,接枝的鈷配合物負載量也相應增加。在以分子氧作氧化劑,異丁醛作犧牲醛,催化環(huán)己烯氧化反應中,核-殼型催化劑在反應速度和環(huán)氧選擇性上均優(yōu)于silica型催化劑;相反,在反式二苯乙烯氧化反應中,則是后者明顯優(yōu)于前者。造成這種差別的原因很可能與殼層表面聚合物與兩個(gè)反應底物的親和力差異顯著(zhù)有關(guān)。
關(guān)鍵詞:納米二氧化硅;核-殼結構;Salen-Co;環(huán)氧化
中圖分類(lèi)號:TQ252.5  文獻標識碼:A  文章編號:1009-9212(2009)06- 0063-06
Chemically Grafting and Catalytic Performances of Salen-Co Complex onto Silica and Core-shell Silica for Epoxidation of Alkene with Oxygen in the Presence of Isobutyraldehyde
ZHOU Jian-bo,FU Zai-hui,ZENG Ming,ZENG Xiao-jun,CUI Xiao-ying (Changsha Medical University,Changsha 410219)
Abstract:By means of chemically grafting method,Salen-Co complex has been successfully bonded onto the surfaces of nano-silica and inorganic-organic hybrid carriers which consist of nano-silica core and styrene and methyl acrylate copolymers shell. The prepared catalysts were characterized by FT-IR,TG-DTA and TEM. The characterization results indicated that the shell layer properties of the core-shell carriers could be adjusted by varying the ratio of the two monomer,the shell with the majority of poly-styrene was gradually transmitted to be characteristic of the poly methyl acrylate with increasing methyl acrylate. In catalyzing the epoxidation of cyclohexene,the Co complexes with the core-shell carriers showed a higher catalytic activity than with nano-silica carriers. This is mainly due to the former has a better affinity to the substrate than the latter. However,in catalyzing the epoxidation of E-stilbene,the reversed results were obtained. This is likely because of affinity differences between the catalysts and the substvates.
Key words:nano-silica;core-shell structure;Salen-co;epoxidation
基金項目:國家自然科學(xué)基金資助項目(20573035)。
作者簡(jiǎn)介:周建波(1979-),女,湖南衡陽(yáng)人,講師,主要從事不對稱(chēng)催化合成。(E-mail:zhoujianbo0603@126.com)
收稿日期: 2009-11-0
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