| 第 46 卷第 5 期 |  | Vol. 46 No. 5 | | 2016 年 10 月 | Oct 2016 |
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所屬欄目：功能材料
Zn-EDTA-2Na配合物催化環(huán)氧丙烷與CO2反應合成碳酸丙烯酯的研究 |
| 陳 盛2，唐靈生2，蘭東輝1*
（1. 湖南大學(xué) 化學(xué)化工學(xué)院，湖南 長(cháng)沙 410082；2. 雅禮中學(xué)，湖南 長(cháng)沙 410007） |
| 摘 要：以水為溶劑，利用無(wú)毒、穩定、廉價(jià)易得且具有強配位能力的乙二胺四乙酸鈉鹽（EDTA-nNa）與金屬鹵化物配位，構建了多種配合物MX2-EDTA-nNa（M=Zn、Fe、Co、Ni；X=Cl、Br、I、NO3；n=0、2、4）。配合物催化環(huán)氧丙烷與CO2反應合成碳酸丙烯酯研究表明，配合物中金屬中心Lewis酸性和陰離子離去能力越強，其催化活性越高；其中ZnBr2-EDTA-2Na表現出最優(yōu)異的催化性能，碳酸丙烯酯的收率和選擇性分別為96.9%和99.3%，TOF達96.9 h-1。通過(guò)復合氧化石墨烯，可以進(jìn)一步提高ZnBr2-EDTA-2Na的耐水性。另外，結合Redlich-Kwong方程和實(shí)驗結果探討了溶于反應液中CO2的量，在25℃和1.25 MPa下溶于反應液中的CO2量超過(guò)9.3 mmol，將有利于CO2轉化為碳酸丙烯酯。 |
| 關(guān)鍵詞：Zn-EDTA-2Na配合物；催化；二氧化碳；碳酸丙烯酯；環(huán)加成反應 |
| 中圖分類(lèi)號：O621.3 文獻標識碼：A 文章編號：1009-9212（2016）05-0056-07 |
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| Synthesis of Propylene Carbonate from CO2 and Propylene Oxide Using Zn-EDTA-2Na Complexes as Catalysts |
| CHEN Sheng2, TANG Ling-sheng2, LAN Dong-hui1*
(1. College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China; 2. Yali Middle School, Changsha 410007, China) |
| Abstract：A series of novel MX2-EDTA-nNa(M=Zn, Fe, Co, Ni; X=Cl, Br, I, NO3; n=0, 2, 4) complexes were prepared through the coordination of metal halides with ethylenediaminetetraacetic acid sodium salts (EDTA-nNa) in aqueous solution. These prepared complexes were non-toxic, cheap, and stable. Based on the activities of MX2-EDTA-nNa, it was deduced that a strong acidity of metal and a strong leaving ability of anion were favorable for the cycloaddition reaction of CO2 with propylene oxide. In the case of using ZnBr2-EDTA-2Na as the catalyst, propylene carbonate(PC) selectivity and yield are 99.3% and 96.9%, respectively, showing a turnover frequency of 96.9 h-1. The stability of ZnBr2-EDTA-2Na could be improved by graphene oxide. Furthermore, the mount of CO2 dissolved in the liquid phase was calculated using the Redlich-Kwong equations on the basis of PC yield. It was found that the amount of CO2 dissolved in the reaction solution was higher than 9.3 mmol at a temperature of 25℃ and a pressure of 1.25 MPa. The good solubility of CO2 in the reaction liquid was favorable for CO2 conversion. |
| Key words：Zn-EDTA-2Na complex; catalyst; carbon dioxide; propylene carbonate; cycloaddition |
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作者簡(jiǎn)介：陳 盛（1999-），男，湖南長(cháng)沙人，主要從事功能材料研究。
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聯(lián) 系 人： 蘭東輝，講師，博士，研究方向：二氧化碳資源化利用、功能材料研究。
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收稿日期：2016-09-1
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