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European Journal of Applied Sciences – Vol. 12, No. 6

Publication Date: December 25, 2024

DOI:10.14738/aivp.126.17865.

Ma, W., & Wang, C. (2024). Preparation of High-Purity Rutin from Sophora japonica. European Journal of Applied Sciences, Vol -

12(6). 135-147.

Services for Science and Education – United Kingdom

Preparation of High-Purity Rutin from Sophora japonica

Wenjing Ma

School of Chemistry and Chemical Engineering,

Nanjing University of Science and Technology, Nanjing 210094, China

Chuanjin Wang

School of Chemistry and Chemical Engineering,

Nanjing University of Science and Technology, Nanjing 210094, China

ABSTRACT

High-Purity Rutin (HPR) was extracted from Sophora japonica by ultrasonication,

decolorized using activated carbon, separated by polyamide chromatography, and

recrystallized. An orthogonal design of experiment was used to determine the

optimal ultrasonic extraction time, number of ultrasonic extractions, and

ultrasonic extraction temperature to maximize the extraction yield of rutin. The

optimal conditions were determined as follows: 2000 mL of CH3OH were used to

extract 20 g of the dried Sophora japonica flower bud powder for 30 minutes and

the extraction was repeated 2 times under ultrasonic conditions (ultrasound

frequency: 40 KHZ; water temperature: 40 °C). The decolorization of the CH3OH

extract of Sophora japonica using active carbon was studied. The optimal

processes are as follows: The filtrate of CH3OH extract was concentrated to 200 mL

by rotary evaporation; 7.2 g of activated carbon powder was added; and the

mixture was refluxed in an 80 °C water bath for 0.5 hours (twice). The polyamide

chromatography separation conditions for crude rutin were investigated. The

influence of particle size and amount of polyaminde used on extraction yield of

rutin was studied. It was found that best separation results were obtained when

50 g of polyamide with particle size of 0.170~0.210 mm was used to purify 3 g of

crude rutin. The purity of the HPR obtained was 99.8%, the extraction yield of HPR

was 18.6%, and the extraction rate of HPR was 70.8%. The structure of the final

product was identified by elemental analysis, IR, HPLC and 1H NMR. It was

experimentally demonstrated that the proposed process was a safe, mild, low-cost

and waste-free procedure.

Keywords: High-Purity of Rutin (HPR), Ultrasound extraction, Activated carbon

decolorization, Polyamide chromatography separation.

INTRODUCTION

Sophora japonica is the dried flower bud of Sophora japonica L., which is widely cultivated in

China for its favorable medicinal value. It has been reported that Sophora japonica, which has

many active substances, has various biological activities, including antibacterial capacity,

vasodilation, and antioxidation capacity, etc. The dried flower bud of Sophora japonica L. has

been widely applied in health and food products [1]. There is a large amount rutin (Fig. 1) in

the flower buds of Sophora japonica L. Rutin, a flavonoid compound, has many important

physiological activities in the treatment of inflammation, cerebrovascular diseases,

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cardiovascular disorders, cancer, etc., attributed to its anti-inflammatory [2], antiviral [3],

remarkable antioxidation [4], and antifree radical properties [5].

Fig. 1: Chemical structure of rutin

The extraction methods of rutin mainly include alkali extraction and acid precipitation [6, 7],

hot extraction and cold precipitation [8], and organic solvent extraction [9~12]. However,

these methods have some drawbacks, such as thermal degradation of rutin due to prolonged

heat at high temperature, potential effects on human health and the environment through the

use of large amounts of harmful organic solvents. In order to overcome these problems, the

use of environmentally friendly technologies has been highly valued by researchers, including

microwave-assisted extraction [13], ultrasound-assisted extraction [14], enzyme-assisted

extraction [15], supercritical fluid extraction [16], etc. Rutin purification methods mainly

include alkali solubilized acid precipitation method [17], cold water washing method [18],

dextran gel method [19], macroporous adsorption resin method [20], polyamide

chromatography method [21, 22], macroreticular resin method [23], high-pressure liquid

phase preparation method [24], two-step chromatographic process (MCI GEL® CHP20P and

Sephadex® LH-20 columns) method [25], etc. Among them, both cold water washing method

and alkali solubilized acid precipitation method have the problems of low purification rate

and incomplete impurity removal. The latter few methods have the problems of cumbersome

operations, low yields, and high costs. These shortcomings limit the wide application of rutin

in food, cosmetics, and medicine areas.

Sophora japonica L., which is also widely grown in China, and has become an important source

of rutin. The current upper limit purity of rutin available on the market is about 98%. To meet

higher needs arising in production and scientific research, as well as to control the quality of

rutin products, we have successfully prepared HPR using activated carbon decolorization

method polyamide chromatography method, and recrystallization method. The purity of HPR

was determined using the HPLC method. The structure of rutin was also characterized by IR,

elemental analysis, and 1H NMR. Compared with the extraction and purification processes

reported in the literature, the method for preparing HPR described in this paper has the

advantages of simple process, non-toxic and pollution-free solvents, safety, low cost, and

reusable solvents and polyamides, making it suitable for industrial production.

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Ma, W., & Wang, C. (2024). Preparation of High-Purity Rutin from Sophora japonica. European Journal of Applied Sciences, Vol - 12(6). 135-147.

URL: http://dx.doi.org/10.14738/aivp.126.17865

MATERIALS AND METHODS

Materials and Instruments

Chromatographic methanol and dimethyl sulfoxide (DMSO) were obtained from Sigma

Chemical Co., Ltd. (Shanghai, China). Polyamide (particle size: 0.140 mm-0.575 mm) was

obtained from Jiangsu Changfeng Chemical Co., Ltd. (Changzhou, China). Powdered activated

carbon (particle size: 1.0 μm-150 μm) was obtained from Shanghai Bilang Environmental

Protection Technology Co., Ltd. (Shanghai, China). Sophora japonica was obtained from

Chuzhou, Anhui Province, China.

A Waters e2695 instrument and a 2498UV/Vis detector were obtained from Waters

Corporation of Shanghai (Shanghai, China). A Bruker (500 MHz) NMR and Vector 22 type

infrared spectrometer were obtained from Brooke Company (Karlsruhe, Germany). A CHN-O- Rapid elemental analyzer was obtained from Heraeus Analytical Instruments (Hanau,

Germany). A chromatography column was obtained from Beijing Synthware Glass Instrument

Co., Ltd. (Beijing, China).

Content Determination and Extraction Rate Calculation of Rutin From Sophora japonica

Based on previous research methods [26], 55 mg of rutin standard was weighed and placed in

a 250 mL volumetric bottle; 60% ethanol was added to the scale; and rutin standard solution

was obtained at a concentration of approximately 0.22 mg/mL. A rutin standard solution of

0.22 mg/mL was placed in a 10 mL volumetric flask (0.0, 1.0, 2.0, 3.0, 4.0, and 5.0 mL). Next,

0.5 mL of 5% NaNO2 solution was added and placed for 6 min; 0.5 mL of 10% Al (NO3)3

solution was added and calmly placed for 6 min. Next, added 4 mL of 4% NaOH solution was

added, and the distilled water was diluted to 10 mL, shaken evenly, and then calmly placed for

15 min. Rutin was not added to the blank control group. The absorbance value was measured

at 500 nm. The standard curve was plotted using the standard solution absorbance as the

ordinate Y and the mass concentration of rutin in the standard solution as the abscissa X. The

regressive equation of the curve was Y = 9.5182X-0.0072, R2 = 0.9973. The results showed

that its mass concentration and absorbance were quite linear in the range from 22 μg/mL to

110 μg/mL.

Based on a previous research method [27], Sophora japonica powder (1 g) and ether (120 mL)

were added to a Suo Shi extractor, heated, and refluxed to obtain a colorless extracted liquid.

The extracted liquid of ether was discarded after being cooled. Methanol (90 mL) was added

to the Suo Shi extractor once again, heated, refluxed to colorless extracted liquid, and

transferred to a 100 mL volumetric flask. Methanol was added to the scale, and methanol

extract solution was obtained. Five milliliters of methanol extract solutions were placed in a

50 mL volumetric flask, and distilled water was added to the scale. Two milliliters were

removed from the previously prepared solution and placed in a 10 mL volumetric flask, and

the absorbance was measured according to the standard curve method. The mass fraction (c)

of rutin in Sophora japonica was calculated as 25.4% based on the concentration-absorbance

of the standard sample.

In the subsequent ultrasonic extraction and decolorization process, each extract or

decolorization liquid was transferred to a 100 mL volumetric bottle, methanol was added to

the scale, and a methanol extract solution was obtained. Five milliliters of methanol extract

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solutions were placed in a 50 mL volumetric flask, and distilled water was added to the scale

and used as the test solution. In the polyamide column layer separation process study, 100 mL

of eluate was taken each time. Two milliliters of eluate were transferred to a 50 mL

volumetric flask, and 50% ethanol was added to the scale and used as the test solution.

Two milliliters were removed from each test solution and placed in a 10 mL volumetric flask,

and the absorbance was measured according to the standard curve method. The mass fraction

(c') of rutin in the test solution was calculated according to the standard linear equation of

concentration-absorbance of the standard sample, and the extraction rate of rutin was

calculated according to the following formula:

Extraction rate of rutin (%) = (c'/c) × 100%

Polyamide Pretreatment and Packing

Polyamide (140 g) mixed with an appropriate amount of anhydrous ethanol was added to a

1000 mL round bottom flask, heated under reflux in a constant temperature water bath (90

°C), filtered and washed with distilled water more than three times after 2 h. The filter cake

was transferred to a 1000 mL beaker filled with distilled water (500 mL), stirred well, and

then soaked overnight. The next day, the polyamide powders that removed some bubbles in

the beaker were poured into the chromatography column filled with absorbent cotton at the

bottom of the column and naturally settled. Excess water is released from the

chromatography column and then stopped by closing the piston at the bottom of the column

until the water surface is slightly higher than the surface of the polyamide powder. The

chromatography column was installed and used for the separation and purification of rutin.

Extraction and Isolation

The dried flower bud powders of Sophora japonica (20.0 g) were loaded into a flask (5000

mL) and extracted with CH3OH (2000 mL × 2) under ultrasonic conditions (ultrasound

powder: 40 KHZ; water temperature: 40 °C). Each extraction time was 30 min. The solutions

were filtered and merged. The filtrate was concentrated to 200 mL by rotary evaporation; 7.2

g of activated carbon powder was added; and the mixture was refluxed in an 80 °C water bath

for 0.5 h (two times), filtered and merged to obtain a brown-yellow liquid. As previously

mentioned, the brown‒yellow liquid was concentrated and dried under vacuum to obtain a

crude extract of rutin (6.2 g). The crude rutin (3.0 g) was separated on a with polyamide

chromatographic column using elution solvent with H2O-C2H5OH (V/V, 1:1) to afford 30

fractions (F1-F30, 100 mL/fraction). Fractions F6–F20 were merged, concentrated, dried in

vacuum and further recrystallized from 400 mL H2O to obtain HPR (1.8 g) with a yield of

approximately 18.6% from Sophora japonica.

A High-performance liquid chromatography (HPLC) system of (Waters) was selected to

determine the purity of rutin. The analytical chromatography conditions are listed as follows:

rutin (5 mg) was dissolved in methanol in a 100 mL volumetric flask. After filtration with a

0.22 μm filter, purity analysis of rutin was carried out with a C18 column (4.6 mm i.d ×250

mm, particle size of 5 μm). The mobile phases were H2O and CH3OH (70:30, V/V), the flow

rate was 1.0 mL/min, and the sample volume was 10 μL. The temperature of the column was

maintained at 30 °C, and the UV detection wavelength was set to 254 nm. Identification of

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Ma, W., & Wang, C. (2024). Preparation of High-Purity Rutin from Sophora japonica. European Journal of Applied Sciences, Vol - 12(6). 135-147.

URL: http://dx.doi.org/10.14738/aivp.126.17865

rutin was performed by IR, elemental analysis and 1H NMR spectroscopy. IR was performed

using a Vevtor 22 infrared spectrometer. The 1H NMR experiment was carried out using a

Bruker DR×500 NMR spectrometer. Elemental analysis was performed by a CHN-O-Rapid

elemental analyzer.

RESULTS AND DISCUSSION

Identification of rutin Isolated from Sophora japonica

The structure of the final product separated was identified by IR, elemental analysis, HPLC

and NMR spectroscopy as follows: Purity (HPLC): 99.8% (Fig. 2); appearance: light yellow

powder; mp: 195-196 °C. In the infrared spectrum (Fig. 3), the strong and wide absorption

peak at 3427.3 cm-1 resulted from the -OH stretching vibration.

Fig. 2: HPLC spectrogram of rutin isolated methanol solution

Fig. 3: Infrared spectrum of rutin

The weak absorption peak of 2923.7 cm-1 resulted from CH3- and -CH2- stretching vibrations.

The strong and wide absorption peak of 1652.8 cm-1 indicated the presence of a conjugated

carbonyl group. The peaks at 1604.6 cm-1, 1506.2 cm-1, 937.3 cm-1, 877.5 cm-1 and 811.9 cm-1

were caused by aromatic ring skeletons and aromatic ring substitutions. The absorption peak

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of 1361.5 cm-1 showed the presence of methyl group in this compound. The absorption peak

of 1456.1 cm-1 was caused by C-H bending vibration of methylene. 1297.9 cm-1, 1243.9 cm-1,

1205.3 cm-1, 1164.8 cm-1 and 1062.3 cm-1 were attributed to various hydroxyl groups in

flavonoid glycosides.

The results of element analysis according to C27H30O16 were the measured values (calculated

values)/%: C, 53.10 (53.07); H, 4.88 (4.91). The structure of the isolated compound and rutin

are identical.

The chemical shifts of different types of protons are shown in the 1H NMR spectra (DMSO, 500

MHz) (Fig. 4). Apart from the sharp peak of δ 12.58 (1H, S, 5-OH), the remaining three peaks

of 10.83 (1H, S, 7-OH), 9.67 (1H, S, 4′-OH), and 9.18 (1H, S, 3′-OH) hydroxyl protons on the

aromatic ring are wide and flat, and all four hydroxyl protons appear in the low field (δ>9.0).

The five protons on the aromatic ring are 7.52 (1H, S, 6′-H), 7.51 (1H, S, 2′-H), 6.83 (1H, S, 5′-

H), 6.37 (1H, S, H-8), and 6.17 (1H, S, H-6). These protons appear in the field (9.0>δ>6.0).

The six –OH proton glycosides are 5.28 (1H, S, 2′′-OH), 5.11 (1H, S, 3′′-OH), 5.08 (1H, S, 4′′-

OH), 5.07 (1H, S, 2′′′-OH), 4.53 (1H, S, 3′′′-OH), and 4.35 (1H, S, 4′′′-OH). The three hydroxyl

glucose group appear in the lower field because the glucose groups is near the mother nucleus

of the flavonoid. The chemical shifts of two hydrogen atoms on the first carbon of

glucosylrhamnose are 5.31 (1H, S, H-1′) and 4.39 (1H, S, H-1′′′). The peaks of 0.97, and 0.96

are typical proton-induced chemical shift of rhamnose methyl. The chemical shifts of ten

hydrogen atoms on the glucose and pyran ring of rhamnose are located between 3.0 and 4.0,

forming overlapping multiple peaks. All data were identical to those of rutin [28].

Fig. 4:

1H NMR spectrogram of rutin

Factors Influencing the Separation and Purification of Rutin

Factors Influencing Ultrasonic Extraction:

The ultrasonic extraction process has shown many advantages, including a faster extraction

rate, lower energy input, lower solvent consumption, and lower temperature in the extraction

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of natural products [29]. This extraction technology is widely utilized in industry. Ultrasound

waves cause cell destruction and ultrasonic jets and reduce the particle size, improving the

contact area of the solid-liquid phase and producing more active substances in the extraction

solvent. The increasing extraction yield of natural products is devoted to acoustic cavitation

phenomena under ultrasound conditions. The expansion cycle could produce numerous

microbubbles or cavities in the liquid phase at sufficient ultrasound intensity. These formed

bubbles could absorb the energy from ultrasonic waves and increase during the expansion

cycles. The pressure and temperature increased due to compression, making the bubbles

break up, which produces a shock wave that traversed the solvent, improving the mass

transfer effect within the ultrasound extraction system [30].

Rutin is an alcohol-soluble component that is extracted with methanol as the solvent. A three- factor and three-level orthogonal experiment was established with ultrasonic extraction times

(A) of 20 min, 30 min and 40 min, ultrasonic extraction times (B) of 1 time, 2 times and 3

times, and ultrasonic extraction temperatures (C) of 20 °C, 40 °C and 60 °C (Table 1). The

ultrasonic extraction technology of rutin from Sophora japonica was investigated. The

extraction rate of rutin was used as a marker. The dried flower bud powders of Sophora

japonica (1.0 g) were loaded into a flask (50 mL) and extracted with CH3OH (10 mL) under

ultrasonic conditions (ultrasound powder: 40 KHZ) every time. The experimental results are

shown in Table 2.

Table 1: Factors and levels of orthogonal experiments for ultrasonic extraction

Levels Factors

Time/A(min) Times/B(Times) Temperature/C (°C)

1 20 1 20

2 30 2 40

3 40 3 60

Table 2: Results of ultrasonic extraction orthogonal experiment

No

Factors and levels The extraction rate of rutin (%)

A B C D(Blank)

1 1 1 1 1 64.5

2 1 2 2 2 72.4

3 1 3 3 3 77.1

4 2 1 2 3 84.6

5 2 2 3 1 85.1

6 2 3 1 2 81.2

7 3 1 3 2 79.3

8 3 2 1 3 86.2

9 3 3 2 1 85.7

I 214.0 228.4 231.9 235.3

II 250.9 243.7 242.7 232.9

III 251.2 244.0 241.5 247.9

R 37.2 15.6 10.8 15.0

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As shown in Table 2, the A3B3C2 method (ultrasonic extraction time of 40 minutes, 3 ultrasonic

extraction times, and ultrasonic extraction temperature of 40 °C) was the optimal ultrasonic

extraction method for rutin from Sophora japonica.

With the extended ultrasound time, the extraction rate of rutin gradually increased. When the

time exceeded 30 minutes, the effect of time on the extraction rate of rutin was not obvious.

As shown in Table 2, the rutin extraction rate was nearly unchanged by ultrasound time at 30

minutes and 40 minutes. The concentration gradient of rutin inside and outside the plant cells

tended to 0 in a short time, and the rutin extraction rate exhibited minimal change with

increasing extraction time. Under the conditions of constant extraction time and extraction

temperature, the ultrasonic extraction time had a significant effect on the extraction rate of

rutin. If the number of extractions is too small, rutin leaching will be incomplete. With an

increase in extraction times, rutin leaching becomes relatively more complete; however, the

production cost is increased. Comprehensive consideration shows that the 2 extraction times

yields better results. The increase in ultrasonic extraction temperature can improve the

solubility and diffusion coefficient of rutin in the solvent and enhance the extraction rate.

However, when the temperature is too high, ultrasonic cavitation may be weakened, which is

not conducive to the extraction of rutin [31]. Overall, an ultrasound temperature of 40 °C was

selected for subsequent experiments. The method of A2B2C2 (ultrasonic extraction time: 30

minutes; number of ultrasonic extractions: 2 times; ultrasonic extraction temperature: 40 °C)

was determined as the method of ultrasound extraction. The test was repeated three times

according to the optimized process conditions, and the average extraction rate of rutin was

88.6%. The result was better than that of any group in the orthogonal trials. The results

showed that the optimal extraction method that was selected was convenient and reliable,

had a high extraction rate and was suitable for extracting rutin from Sophora japonica.

Factors Influencing Activated Carbon Decolorization:

The methanol ultrasonic extract of Sophora japonica contains more chlorophyll, which should

be decolorized with activated carbon. Systematic research on the method of decolorization of

methanol ultrasonic extract of Sophora japonica was carried out. The dried flower bud

powders of Sophora japonica (9.0 g) were loaded into a flask (500 mL) and extracted with

CH3OH (90 mL) under ultrasonic conditions (ultrasound powder: 40 KHZ) according to the

optimal methanol ultrasonic extraction process A2B2C2 (ultrasonic extraction time: 30

minutes; ultrasonic extraction: 2 times; ultrasonic extraction temperature: 40 °C). The two

extracts were filtered, merged, concentrated to 90 mL by rotary evaporation, evenly divided

into nine aliquots, and decolorized according to the orthogonal experiment method (Table 3).

The extraction rates of rutin, chlorophyll A (at 663 nm) and chlorophyll B (at 645 nm)

absorption in decoloring solution were selected as the comprehensive marker, and the L9 (34)

orthogonal table was arranged for the experiment. The experimental results are shown in

Table 4.

Comprehensive marker (CM) = 25% (X̅/X) + 25% (Y̅/Y) + 50% (Z̅/Z)

X is the absorption of chlorophyll A in 9 parts of the decolorization solution; X̅ is the mean of

chlorophyll A absorption in 9 decolorization solutions; Y is the absorption of chlorophyll B in

9 parts of the decolorization solution; Y̅ is the mean of chlorophyll B absorption in 9

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Ma, W., & Wang, C. (2024). Preparation of High-Purity Rutin from Sophora japonica. European Journal of Applied Sciences, Vol - 12(6). 135-147.

URL: http://dx.doi.org/10.14738/aivp.126.17865

Table 6: Influence of the sample amount to the polyamide amount

M sample /M polyamide (g/g) Extracting rate of rutin/%

1:40 55.7

1:45 65.3

1:50 76.6

1:55 76.8

1:60 77.5

As show in Table 6, when the mass ratio of the crude rutin to polyamide used was 1:50, the

extraction rate of rutin did not increase. Therefore, the ratio of 1:50 is selected.

CONCLUSIONS

In recent years, natural products have been increasingly investigated as anticancer drugs. In

this study, HPR (HPLC: 99.8%) was successfully separated from Sophora japonica by

ultrasonic extraction, activated carbon decolorization, polyamide column chromatography,

and recrystallization. The extraction yield of HPR was 18.6%. The chemical structure of the

final product separated was identified by IR, element analysis and 1H NMR. Compared with

the traditional separation process, optimized extraction process of HPR in this paper has the

advantages of simple process, environmentally friendly solvent, safe and cheap, and

polyamide can be reused. so optimized extraction process is suitable for industrial

production. The extraction yield and purity of rutin increased significantly. The research

results have provided a strong foundation for the further development and utilization of

Sophora japonica resources.

ACKNOWLEDGMENTS

The author appreciates Lei Sun, Fu Da Testing Center, for the help with FT-IR and HNMR

characterizations.

Conflict of Interest

The authors declare no conflict of interest.

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