Bai Jingyao, Ou Junjie, Zhang Haiyang, Ma Shujuan, Shen Yehua, Ye Mingliang
CAS Key Laboratory of Separation Sciences for Analytical Chemistry, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China; Key Laboratory of Synthetic and Natural Function Molecule Chemistry of Ministry of Education, College of Chemistry and Materials Science, Northwest University, Shaanxi Alcohol Ether and Biomass Energy Engineering Research Center, Key Laboratory of Yulin Desert Plants Resources, Xi'an, 710069, China.
CAS Key Laboratory of Separation Sciences for Analytical Chemistry, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
J Chromatogr A. 2017 Sep 8;1514:72-79. doi: 10.1016/j.chroma.2017.07.070. Epub 2017 Jul 26.
One-step thiol-maleimide polymerization reaction was firstly adopted for direct preparation of polymeric monoliths via alkaline-catalyzed reaction of 4,4'-bis(maleimidophenyl)methane (BMI) and trimethylolpropane tris(3-mercaptopropionate) (3SH)/pentaerythriol tetra(3-mercaptopropionate) (4SH) in the presence of a small amount of triethylamine (TEA). The polymerization could be performed within 3h, which was faster than thermal-initiated free radical polymerization. Two kinds of monoliths, poly(BMI-co-3SH) (marked as I) and poly(BMI-co-4SH) (marked as II), were characterized with scanning electron microscopy (SEM), attenuated total reflection Fourier-transformed infrared spectroscopy (ATR-FTIR), thermal gravimetric analysis (TGA) and mercury intrusion porosimetry (MIP). Satisfactory chromatographic separation ability and column efficiency were gained for analysis of small molecular compounds such as alkylbenzenes, polynuclear aromatic hydrocarbons (EPA 610) and phenols in reversed-phase capillary liquid chromatography (cLC). High column efficiency (180,500N/m) for butylbenzene was acquired on poly(BMI-co-3SH) column I-2, which was higher than those on most reported polymeric monoliths. A retention-independent efficient performance of small molecules was obtained by plotting of plate height (H) of alkylbenzenes versus the linear velocity (u). A term values in van Deemter equation of I-2 (1.72-0.24μm) and poly(BMI-co-4SH) column II-2 (5.28-4.14μm) were smaller than those of traditional organic/hybrid monoliths. Finally, as a practical application, 53 and 2184 unique peptides from the tryptic digests of bovine serum albumin (BSA) and HeLa cell proteins were positively identified with poly(BMI-co-3SH) monolith in cLC-MS.
首次采用一步硫醇-马来酰亚胺聚合反应,通过4,4'-双(马来酰亚胺基苯基)甲烷(BMI)与三羟甲基丙烷三(3-巯基丙酸酯)(3SH)/季戊四醇四(3-巯基丙酸酯)(4SH)在少量三乙胺(TEA)存在下的碱催化反应直接制备聚合物整体柱。聚合反应可在3小时内完成,比热引发自由基聚合更快。用扫描电子显微镜(SEM)、衰减全反射傅里叶变换红外光谱(ATR-FTIR)、热重分析(TGA)和压汞法(MIP)对两种整体柱,即聚(BMI-co-3SH)(标记为I)和聚(BMI-co-4SH)(标记为II)进行了表征。在反相毛细管液相色谱(cLC)中分析小分子化合物如烷基苯、多环芳烃(EPA 610)和酚类时,获得了令人满意的色谱分离能力和柱效。在聚(BMI-co-3SH)柱I-2上对丁基苯获得了高柱效(180500N/m),高于大多数报道的聚合物整体柱。通过绘制烷基苯的板高(H)与线速度(u)的关系图,获得了小分子的保留无关高效性能。I-2(1.72-0.24μm)和聚(BMI-co-4SH)柱II-2(5.28-4.14μm)的范德姆特方程中的A项值小于传统有机/混合整体柱。最后,作为实际应用,在cLC-MS中用聚(BMI-co-3SH)整体柱对牛血清白蛋白(BSA)和HeLa细胞蛋白的胰蛋白酶消化产物中的53种和2184种独特肽进行了阳性鉴定。