SiW11掺杂二氧化硅纳米纤维(SiW11/SiO2)的制备及对拟南芥叶中多胺的萃取分析

doi:10.7503/cjcu20180531

摘要/Abstract

摘要：

采用静电纺丝技术制备了SiW₁₁掺杂的二氧化硅纳米纤维(SiW₁₁/SiO₂)材料, 其中掺杂的SiW₁₁质量占纤维质量的7.83%, 制备的SiW₁₁/SiO₂材料尺寸均一, 在考察的pH范围内带负电, 与未掺杂SiW₁₁的二氧化硅纳米纤维相比, SiW₁₁/SiO₂材料表现出强阳离子交换作用, 能有效萃取尸胺和腐胺. 在最优条件下, 建立了注射器分散固相萃取(In syringe dSPE)-超高效液相色谱-串联质谱联用(UHPLC-MS/MS)检测拟南芥样品中多胺的方法. 结果表明, 尸胺和腐胺分别在10~1000和20~1000 ng/mL浓度范围内具有良好的线性关系(R²≥0.9950), 检出限和定量限分别为0.5~0.9和1.6~3.0 ng/mL. 将该方法应用于拟南芥样品中尸胺和腐胺的检测, 加标回收率在87.5%~111.3%之间, 相对标准偏差RSD<5.0%. 建立的SiW₁₁/SiO₂制备方法解决了多金属氧酸盐(POM)在修饰改性过程中存在的制备繁琐、固载量少的问题, 拓宽了POM在分离领域中的应用.

关键词: 多金属氧酸盐, SiW₁₁/SiO₂, 静电纺丝, 注射器分散固相萃取, 多胺

Abstract:

SiW₁₁ incorporated SiO₂ nanofibers(SiW₁₁/SiO₂) was prepared by electrospinning technology. The mass of incorporated SiW₁₁ accounted for 7.83% of nanofibers. SiW₁₁/SiO₂ nanofiber possessed uniform structure with the diameter about 450 nm, and was negative charged in the pH range of 1.0—11.0. Compared with SiO₂ nanofibers, the SiW₁₁/SiO₂ nanofiber exhibited stronger cation-exchange interactions to extract PUT and CAD. Under the optimized condition, an in-syringe dSPE-UHPLC-MS/MS method for rapid and selective detection of polyamines from plants was established. The limits of detection(LODs) for the target CAD and PUT ranged from 0.5 ng/mL to 0.9 ng/mL, and the linear range was 10—1000 ng/mL and 20—1000 ng/mL with determination coefficients(R²) higher than 0.9950. The recoveries ranged from 87.5% to 111.3% with relative standard deviations(RSDs) of 1.9%—7.2%. The proposed method can be used to detect the trace CAD and PUT in Arabidopsis.

Key words: Polyoxometalate(POM), SiW₁₁/SiO₂, Electrospinning technology, Insyringe dSPE, Amine compound

中图分类号:

O652

TrendMD:

蔡娇, 余琼卫, 何小梅, 许静, 丁琼, 冯钰锜. SiW₁₁掺杂二氧化硅纳米纤维(SiW₁₁/SiO₂)的制备及对拟南芥叶中多胺的萃取分析. 高等学校化学学报, 2019, 40(5): 901.

CAI Jiao,YU Qiongwei,HE Xiaomei,XU Jing,DING Qiong,FENG Yuqi. Preparation of SiW₁₁ Incorporated SiO₂ Nanofibers(SiW₁₁/SiO₂) and Its Application in the Analysis of Polyamines in Arabidopsis^†. Chem. J. Chinese Universities, 2019, 40(5): 901.

图/表 11

Scheme 1 Chemical structure of CAD and PUT

Table 1 Optimized parameters of multiple reaction monitoring(MRM) mode for analysis of polyamines*

Compound	Scan mode	Precursor ion, m/z	Product ion, m/z	Q1 pre bias/V	CE/V	Q3 pre bias/V
CAD	+	103.2	86.2	-22	-13	-15
PUT	+	89.2	72.2	-13	-13	-27
IS	+	117.2	100.2	-10	-15	-23

Scheme 2 Preparation of SiW11/SiO2 nanofibers(A) and the procedure of insyringe dSPE for the extraction of polyamines(B)

Fig.1 SEM image of SiW11/SiO2 nanofibers

Fig.2 Zeta potentials of SiW11/SiO2 nanofibers ith different pH

Fig.3 Effect of extraction conditions on the extraction efficiencies of two polyaminesExtraction conditions: (A) sorbent amount; (B) pH value; (C) extraction time; (D) the content of formic acid in desorption solvent; (E) desorption volume; (F) desorption time.

Fig.4 Exraction efficiencies of CAD and PUT on SiO2 nanofibers and SiW11/SiO2 nanofibers

Table 2 Linear regression and LOD, LOQ date of polyamines from plant samples

Compound	Linear range/ (ng·mL^-1)	Regression date(n=3)			LOD/ (ng·mL^-1)	LOQ/ (ng·mL^-1)
		Slope	Intercept	R²
		CAD	10.0—1000	12.9			0.632	0.9970	0.9	3.0
PUT	20.0—1000	43.1	2.951	0.9950	0.5	1.6

Table 3 Method reproducibility assessed by intra- and inter-day precisions at three different concentrations of polyamines in spiked plant samples

Compound	Intraday presicion, RSD(%, n=3)			Interday precision, RSD(%, n=3)
Compound	20 ng/mL	100 ng/mL	500 ng/mL	20 ng/mL	100 ng/mL	500 ng/mL
CAD	2.1	2.6	3.4	0.5	1.9	6.0
PUT	0.5	6.8	3.0	12.0	4.8	6.3

Table 4 Method recoveries of polyamines at three different concentrations from spiked plant samples

Compound	Recovery(%)			RSD(%, n=3)
Compound	20 ng/mL	100 ng/mL	500 ng/mL	20 ng/mL	100 ng/mL	500 ng/mL
CAD	87.5	106.6	101.3	3.0	7.2	2.0
PUT	98.2	103.5	111.3	1.9	5.7	3.5

Fig.5 MRM chromatograms of PUT[(47.1±5.8) μg/g](A) and CAD(not detected)(B) detected in plant samples

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SiW₁₁掺杂二氧化硅纳米纤维(SiW₁₁/SiO₂)的制备及对拟南芥叶中多胺的萃取分析

Preparation of SiW₁₁ Incorporated SiO₂ Nanofibers(SiW₁₁/SiO₂) and Its Application in the Analysis of Polyamines in Arabidopsis^†

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