Research progress in the application of magnetic solid phase extraction based on carbon based magnetic materials in food analysis

doi:10.3724/SP.J.1123.2020.05038

Abstract

Abstract: Trace toxic substances in food pose a serious threat to human health, and need to be detected and analyzed to ensure food safety. However, there are many kinds of toxic substances in food, with small amounts and complex matrices, making it necessary to select an appropriate sample pretreatment technology for extraction and purification. There are some disadvantages to sample pretreatment methods such as solid phase extraction and liquid-liquid extraction, in terms of poor selectivity, significant influence of matrix interference, large sample requirement, long extraction time, use of a large amount of harmful organic solvents, and cumbersome and time-consuming operation. Magnetic solid phase extraction (MSPE) combines the advantages of magnetic separation and traditional SPE technology, avoids time-consuming column loading, and can extract the target analyte efficiently. Because of its advantages, in that it has simple operation, is time-saving and fast, requires no centrifugal filtration, and is environmentally friendly, it is considered an efficient sample pretreatment technology and applied in food analysis. The adsorption capacity and selectivity of the magnetic adsorbent used in MSPE are the key factors affecting the extraction efficiency and selectivity of MSPE, and play a key role in the accuracy of the established method. Carbon-based magnetic materials are a type of new functional magnetic materials prepared by the co-precipitation of carbon-based materials (carbon nanotubes, graphene, metal-organic framework-derived carbon, or activated carbon) and magnetic materials. In order to endow carbon-based magnetic materials with the advantages of both, carbon materials and magnetic materials, while also reflecting the advantages of high specific surface area, good stability, low cost, environmental friendliness, excellent physical and chemical properties, high porosity, and high adsorption capacity, proper functional modification is needed. Carbon-based magnetic materials modified by functionalization can efficiently enrich organic and inorganic analytes with different properties, and have seen significant progress in environmental analysis, biological detection, pollution control, and other fields. In recent years, MSPE technology based on carbon-based magnetic materials has been gradually applied in food analysis and pretreatment, but its use is still in infancy and holds immense application potential. Reference to more than 50 papers published in SCI and Chinese core journals over the past four years reveals that carbon-based materials include carbon nanotubes modified by functional groups, reagents, or materials; graphene, graphene oxide, and reduced graphene oxide; carbon derived from a gold organic framework; activated carbon biochar; and nanodiamond. The harmful substances in food samples include esters, mycotoxins, polycyclic aromatic hydrocarbons, antibiotics, alkaloids, phenols, vitamins, and antibiotics. Based on the classification of carbon-based materials, this review reveals that carbon-based magnetic materials have good preconcentration ability for harmful substances in food samples. MSPE can be combined with GC-MS, liquid chromatography-high resolution mass spectrometry (LC-HRMS), ultra-fast liquid chromatography-tandem mass spectrometry (UFLC-MS/MS), ultra high performance liquid chromatography-Q-Exactive high resolution mass spectrometry (UHPLC-Q-Exactive HRMS), high performance liquid chromatography-diode array detection (HPLC-DAD), gas chromatography micro-electron capture detection (GC-μECD), high performance liquid chromatography fluorescence with post-column photochemical derivatization (HPLC-PCD-FLD), and HPLC-UV to analyze food samples. These combined technologies have high accuracy and recovery. However, the synthesis methods of carbon-based magnetic materials such as carbon nanotubes and graphene, incur high energy consumption and high cost, and involve complex processes, which limit their application. Therefore, a carbon-based magnetic adsorbent with low cost, high selectivity, and high extraction efficiency was developed by further exploring functional modification with biochar as a carbon base. This is a very promising direction to develop MSPE technology utilizing biochar-based magnetic materials for food sample pretreatment. This review provides a theoretical basis and technical support for the wide application of carbon-based magnetic materials in MSPE technology for food analysis.

Key words: magnetic solid phase extraction (MSPE), carbon based magnetic material, adsorbent, food analysis, review

CLC Number:

O658

LIAO Yingmin, HUANG Xiaojia, WANG Zhuozhuo, GAN Rui. Research progress in the application of magnetic solid phase extraction based on carbon based magnetic materials in food analysis[J]. Chinese Journal of Chromatography, 2021, 39(4): 368-375.

Figures/Tables 2

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Carbon base	Carbon based magnetic composite material	Analyte	Samples	Method	LOD	Recovery/ %		RSD/ %	Ref.
CNTs	Fe₃O₄/AMWNTs	pyrethroid pesticides	honey	GC	0.07-0.20 μg/L	78.4	-94.8	3.8-8.1	[10]
	MWCNT-Fe₃O₄	phthalate acid esters	yogurt-based drinking	GC-MS	10.00-24.00 ng/L		-	0.3-7.4	[11]
	MWCNT-MNP	polycyclic aromatic hydrocarbons	milk, milk powder	GC-MS	0.040-0.075 μg/kg	86.1	-100.3	3.2-10.1	[12]
	Tol-MCNT	sulfonamides	milk	LC-HRMS	2.00-10.00 ng/L	86.6	-98.3	0.9-6.2	[13]
	M-N-CNTs	bisphenols	fruit juices	UHPLC-MS/MS	0.43-2.47 ng/L	90.6	-101.0	1.2-5.8	[14]
	PAMAM@Mag-CNTs	toxic alkaloids	meat, vegetable	UFLC-MS/MS	0.011-0.329 ng/g	83.4	-125.0	1.3-8.0	[15]
	PEG-MWCNTs-MNP	mycotoxins	real liquid milk	UHPLC-Q-Exactive HRMS	0.005-0.050 μg/kg	81.8	-106.4	2.1-8.5	[16]
	HCSs@Fe₃O₄- MWCNT-COOH	herbicides	wheat flour	HPLC-DAD	0.24-0.68 ng/g	88.8	-96.6	1.6-6.2	[17]
	Fe₃O₄/MWCNT@ND	vitamin B12	infant formula powder, cereal	HPLC-DAD	2.85 ng/mL	97.8	-103.1	4.3-6.1	[18]
	N-CNTCs	okadaic acid	mussel, oyster	HPLC-MS/MS	1.30 pg/mL	82.0	-107.0	1.8-2.5	[19]
	mMWCNT-ZrO₂-C18	polycyclic aromatic hydrocarbons	edible oils	HPLC-DAD	0.06-0.55 ng/g	93.9	-113.3	3.9-6.0	[20]
G	Fe₃O₄@SiO₂@G	preservative	vegetables	GC-MS	0.21-11.50 μg/kg	78.3	-116.7	1.4-11.9	[21]
	MG@SiO₂-TMSPED	pesticides	tomato, grape	GC-μECD	0.23-0.30 μg/kg	82.0	-113.0	5.1-8.1	[22]
	mNi@N-GrT	tetracyclines	milk	HPLC	1.29-2.31 ng/mL	91.6	-109.7	2.2-5.7	[23]
	3D-G-Fe₃O₄	caffeine	food	GC-FID	0.10 μg/mL	93.1	-97.7	5.9-7.1	[24]
	3D-G-Fe₃O₄	organophosphorus pesticides	juice	GC-NPD	1.20-5.10 ng/L	86.6	-107.5	2.5-7.4	[25]
	3D-G-Fe₃O₄	chlorophenols	honey	HPLC-UV	1.00-1.50 ng/g	93.2	-98.9	4.1-4.6	[26]
GO	Fe₃O₄@GO	sulfonamides	milk	HPLC-MS/MS	0.02-0.13 μg/L	73.4	-97.4	1.0-8.2	[27]
	Fe₃O₄@SiO₂-GO/ MIL-101(Cr)	triazine herbicides	rice	HPLC	0.01-0.08 μg/kg	83.9	-103.5	0.5-8.7	[28]
	MGO	phthalate esters	bottled water	HPLC	0.004-0.013 mg/L	65.0	-126.0	0.6-6.0	[29]
	Fe₃O₄/GO	melamine	dairy products	HPLC	0.03 μg/L	97.2	-103.1	1.1-5.0	[30]
	Fe₃O₄/rGO	aflatoxins	vegetable oils	HPLC-PCD-FLD	0.01-0.02 μg/kg	80.4	-106.0	1.3-10.5	[31]
	rGO/ZnFe₂O₄	estrogens	fish	HPLC-DAD	0.01-0.02 ng/mL	73.5	-104.1	1.7-8.3	[32]
MOFs	MNPCs	organophosphorus pesticides	fruit	GC-FPD	0.018-0.045 μg/L	84.0	-116.0	3.5-9.7	[33]
AC	MBAC	phenylurea herbicides	juice	HPLC-UV	0.10-0.80 ng/mL	86.1	-104.1	4.0-6.8	[34]
BC	C/Fe₃O₄ NCs	triazole fungicides	fruit	GC-MS	0.12-0.55 μg/kg	82.1	-109.9	2.1-8.4	[35]
GC	YS-Fe₃O₄@GC	sulfonamides	milk, meat	HPLC	0.11-0.25 μg/L	77.2	-118.0	1.4-9.2	[36]

Carbon base	Carbon based magnetic composite material	Analyte	Samples	Method	LOD	Recovery/ %		RSD/ %	Ref.
CNTs	Fe₃O₄/AMWNTs	pyrethroid pesticides	honey	GC	0.07-0.20 μg/L	78.4	-94.8	3.8-8.1	[10]
	MWCNT-Fe₃O₄	phthalate acid esters	yogurt-based drinking	GC-MS	10.00-24.00 ng/L		-	0.3-7.4	[11]
	MWCNT-MNP	polycyclic aromatic hydrocarbons	milk, milk powder	GC-MS	0.040-0.075 μg/kg	86.1	-100.3	3.2-10.1	[12]
	Tol-MCNT	sulfonamides	milk	LC-HRMS	2.00-10.00 ng/L	86.6	-98.3	0.9-6.2	[13]
	M-N-CNTs	bisphenols	fruit juices	UHPLC-MS/MS	0.43-2.47 ng/L	90.6	-101.0	1.2-5.8	[14]
	PAMAM@Mag-CNTs	toxic alkaloids	meat, vegetable	UFLC-MS/MS	0.011-0.329 ng/g	83.4	-125.0	1.3-8.0	[15]
	PEG-MWCNTs-MNP	mycotoxins	real liquid milk	UHPLC-Q-Exactive HRMS	0.005-0.050 μg/kg	81.8	-106.4	2.1-8.5	[16]
	HCSs@Fe₃O₄- MWCNT-COOH	herbicides	wheat flour	HPLC-DAD	0.24-0.68 ng/g	88.8	-96.6	1.6-6.2	[17]
	Fe₃O₄/MWCNT@ND	vitamin B12	infant formula powder, cereal	HPLC-DAD	2.85 ng/mL	97.8	-103.1	4.3-6.1	[18]
	N-CNTCs	okadaic acid	mussel, oyster	HPLC-MS/MS	1.30 pg/mL	82.0	-107.0	1.8-2.5	[19]
	mMWCNT-ZrO₂-C18	polycyclic aromatic hydrocarbons	edible oils	HPLC-DAD	0.06-0.55 ng/g	93.9	-113.3	3.9-6.0	[20]
G	Fe₃O₄@SiO₂@G	preservative	vegetables	GC-MS	0.21-11.50 μg/kg	78.3	-116.7	1.4-11.9	[21]
	MG@SiO₂-TMSPED	pesticides	tomato, grape	GC-μECD	0.23-0.30 μg/kg	82.0	-113.0	5.1-8.1	[22]
	mNi@N-GrT	tetracyclines	milk	HPLC	1.29-2.31 ng/mL	91.6	-109.7	2.2-5.7	[23]
	3D-G-Fe₃O₄	caffeine	food	GC-FID	0.10 μg/mL	93.1	-97.7	5.9-7.1	[24]
	3D-G-Fe₃O₄	organophosphorus pesticides	juice	GC-NPD	1.20-5.10 ng/L	86.6	-107.5	2.5-7.4	[25]
	3D-G-Fe₃O₄	chlorophenols	honey	HPLC-UV	1.00-1.50 ng/g	93.2	-98.9	4.1-4.6	[26]
GO	Fe₃O₄@GO	sulfonamides	milk	HPLC-MS/MS	0.02-0.13 μg/L	73.4	-97.4	1.0-8.2	[27]
	Fe₃O₄@SiO₂-GO/ MIL-101(Cr)	triazine herbicides	rice	HPLC	0.01-0.08 μg/kg	83.9	-103.5	0.5-8.7	[28]
	MGO	phthalate esters	bottled water	HPLC	0.004-0.013 mg/L	65.0	-126.0	0.6-6.0	[29]
	Fe₃O₄/GO	melamine	dairy products	HPLC	0.03 μg/L	97.2	-103.1	1.1-5.0	[30]
	Fe₃O₄/rGO	aflatoxins	vegetable oils	HPLC-PCD-FLD	0.01-0.02 μg/kg	80.4	-106.0	1.3-10.5	[31]
	rGO/ZnFe₂O₄	estrogens	fish	HPLC-DAD	0.01-0.02 ng/mL	73.5	-104.1	1.7-8.3	[32]
MOFs	MNPCs	organophosphorus pesticides	fruit	GC-FPD	0.018-0.045 μg/L	84.0	-116.0	3.5-9.7	[33]
AC	MBAC	phenylurea herbicides	juice	HPLC-UV	0.10-0.80 ng/mL	86.1	-104.1	4.0-6.8	[34]
BC	C/Fe₃O₄ NCs	triazole fungicides	fruit	GC-MS	0.12-0.55 μg/kg	82.1	-109.9	2.1-8.4	[35]
GC	YS-Fe₃O₄@GC	sulfonamides	milk, meat	HPLC	0.11-0.25 μg/L	77.2	-118.0	1.4-9.2	[36]