CN104558067B

CN104558067B - A kind of method that separating syringin is extracted in the medicinal material from iron holly bark

Info

Publication number: CN104558067B
Application number: CN201410835321.3A
Authority: CN
Inventors: 段迪; 李宇; 杨丽; 钟鸣; 傅玉萍; 李金华
Original assignee: GUANGZHOU HANFANG PHARMACEUTICAL CO Ltd
Current assignee: GUANGZHOU HANFANG PHARMACEUTICAL CO Ltd
Priority date: 2014-12-30
Filing date: 2014-12-30
Publication date: 2017-09-29
Anticipated expiration: 2034-12-30
Also published as: CN104558067A

Abstract

The invention discloses a kind of method that Syringin extract is prepared in medicinal material from iron holly bark.The operating procedure of method is as follows：1) iron holly bark pulverizing medicinal materials are to 20 ~ 50 mesh, and extracting in water, extract solution obtains upper prop liquid after centrifugal concentrating；2) upper prop liquid crosses resin column, is eluted respectively with water, 10 ~ 40% ethanol (v/v), Fractional Collections eluent；3) 10 ~ 40% ethanol (v/v) elution fraction is spray-dried to obtain product after membrane separation concentration.This method technical process is simple, and workable, cost is low, is adapted to industrialized production.

Description

A kind of method that separating syringin is extracted in the medicinal material from iron holly bark

Technical field

The invention belongs to medicinal active ingredient extraction and separation technology field, specifically, it is related in iron holly bark medicinal material purple fourth The extracting and developing method of fragrant glycosides.

Background technology

Iron holly bark for ilexrotunda bark or root skin, main product in areas such as Jiangsu, Anhui, Jiangxi, Fujian, Guangdong, Guangxi, Herbal medicine is commonly used for south China people side.With clearing heat and detoxicating, effect of dampness removing analgesic, it is usually used in treatment summer-heat and damp heating, throat swells Bitterly, damp-heat dysentery, abdominal distention, arthralgia pain due to rheumatism, condyloma, boil, traumatic injury etc..Syringin is called syringin, is that rescue must The main component in active component is answered, with anti-inflammatory, analgesia and antitumor action, available for hemostasis and anti-liver poison.

The method that separating syringin is extracted in the current published medicinal material from iron holly bark is few, the A of patent CN 1010724 The dry silica gel stirring of water extract-alcohol precipitation, medicinal extract, organic solvent extraction, the technique of the method extraction purification Syringin of crystallization are disclosed, Unit operation is excessive, long, and discontinuously, is unfavorable for industrialized production；The A of patent CN 10103534 disclose alcohol extracting-water precipitating, The method that centrifugal filtration prepares general saponin of cortex ilecis rotundae, product total saponin content only reaches 50%, it is difficult to meet exploitation higher purity The demand of product；The A of patent CN 101307079 disclose the side that benzene refluxing extraction, dregs of a decoction acetone reflux are extracted, recrystallized repeatedly Method extracts Syringin, during, consumption of organic solvent is excessive, and environmental pollution is larger；The A of patent CN 102070684 are disclosed Water extraction, concentrate add under the conditions of activated carbon decolorizing, solution acidic under the conditions of filtering, solution neutral with extracting n-butyl alcohol, decompression The method that n-butanol extraction prepares Syringin is reclaimed, the technique consumption of organic solvent is more, and repeatedly concentrates, and energy consumption is big, unfavorable In industrialized production.

Instant invention overcomes consumption of organic solvent in traditional handicraft is big, production cycle length, high energy consumption the shortcomings of, using water Carry-technique of macroporous resin adsorption separation-efficiently NF membrane concentration-spray drying realizes the preparation and successfully of Syringin Realize industrialization.

The content of the invention

The technical problem to be solved in the present invention is to provide a kind of simple, strong operability, efficient, energy consumption is low, be adapted to industrialization The method that separating syringin is extracted from iron holly bark medicinal material of production.

Technical scheme is as follows：

(1) iron holly bark pulverizing medicinal materials are to 20~50 mesh, extracting in water 1~3 time, every time 60~180min, merge extract solution, It is concentrated under reduced pressure into 1.01~1.20g/ml of density and obtains upper prop liquid；

(2) upper prop liquid is entered into macroporous resin column, washed resin to efflux is closely colourless, then with 10~40% ethanol (v/v) Elution, collects eluent, and eluent through nanofiltration membrane is concentrated into total solid content 25~35% and obtains concentrate；

(3) concentrate is spray-dried obtains product.

In above-mentioned preparation method：

In step (1), the consumption of water is 5~20 times, preferably 8~10 times of raw material weight.

In step (2), the macroreticular resin be nonpolar or low pole macroreticular resin, preferably model AB-8, HPD100, D101, D130, SP825 or HP20.

In step (2), the consumption of water is 2~6 times of resin column volume, and the consumption of 10~40% ethanol (v/v) is resin 2~7 times of column volume.

In step (2), the membrane separation concentration technique, film used is polyamide high temperature NF membrane.

In step (3), in the drying process with atomizing, 170~210 DEG C of EAT, 70 DEG C of temperature of charge, leaving air temp 90~120 DEG C.

Concentration described in the above method is to prepare identical operation in Syringin method using existing.

The present invention using iron holly bark medicinal material as initiation material, using water extraction-macroporous resin adsorption separation-NF membrane concentration- The process route of spray drying, realizes the preparation of Syringin.The invention has the advantages that：

1st, with water level Extraction solvent, cost is low, environmentally safe；

2nd, using macroreticular resin as adsorbent, ethanol water gradient elution, solvent, resin recoverable；

3rd, by membrane separation concentration technique, energy consumption is reduced, production cost is reduced；

3rd, technical process is simple, workable, is adapted to industrialized production.

Brief description of the drawings

Fig. 1 is the process chart that separating syringin is extracted from iron holly bark medicinal material.

Embodiment

Embodiment 1：

After iron holly bark pulverizing medicinal materials, 20 mesh sieves are crossed, claim 220kg to be placed in 3 tons of extractors, the water of 10 times of raw material weights is added 100 DEG C of extractions, extract 120min, filter out decoction for the first time, add the water of 8 times of raw material weights, and refluxing extraction 60min merges Extract solution；

Extract solution is concentrated under reduced pressure into density 1.01g/ml and obtains upper prop liquid；Enter AB-8 macroporous resin columns, be washed to eluent near It is colourless, then eluted with 4 ethanol of column volume 20% (v/v), 20% ethanol (v/v) eluent is collected, it is membrane separation concentrated to be reduced to solid It is spray-dried to obtain product 0.95kg after thing content 30%.

According to the content assaying method of 2010 editions pharmacopeia Syringins, analyze and detect through HPLC, Syringin purity is 78.56%.

Embodiment 2：

After iron holly bark pulverizing medicinal materials, 20 mesh sieves are crossed, claim 220kg to be placed in 3 tons of extractors, the water of 10 times of raw material weights is added 100 DEG C of extractions, extract 180min, filter out decoction for the first time, add the water of 8 times of raw material weights, and refluxing extraction 90min merges Extract solution；

Extract solution is concentrated under reduced pressure into density 1.05g/ml and obtains upper prop liquid；Enter SP825 macroporous resin columns, be washed to eluent near It is colourless, then eluted with 3 ethanol of column volume 20% (v/v), 20% ethanol (v/v) eluent is collected, it is membrane separation concentrated to be reduced to solid It is spray-dried to obtain product 0.86kg after thing content 25%.

According to the content assaying method of 2010 editions pharmacopeia Syringins, analyze and detect through HPLC, Syringin purity is 83.34%.

Embodiment 3

After iron holly bark pulverizing medicinal materials, 30 mesh sieves are crossed, claim 200kg to be placed in 3 tons of extractors, the water of 9 times of raw material weights is added Micro-boiling is extracted, and 120min is extracted for the first time, decoction is filtered out, adds the water of 9 times of raw material weights, refluxing extraction 60min, merging is carried Take liquid；

Extract solution is concentrated under reduced pressure into density 1.04g/ml and obtains upper prop liquid；Enter HP20 macroporous resin columns, be washed to eluent near It is colourless, then eluted with 4 ethanol of column volume 30% (v/v), 30% ethanol (v/v) eluent is collected, it is membrane separation concentrated to be reduced to solid It is spray-dried to obtain product 0.87kg after thing content 25%.

According to the content assaying method of 2010 editions pharmacopeia Syringins, analyze and detect through HPLC, Syringin purity is 76.23%.

Embodiment 4：

After iron holly bark pulverizing medicinal materials, 50 mesh sieves are crossed, claim 200kg to be placed in 3 tons of extractors, the water of 10 times of raw material weights is added Micro-boiling is extracted, and 120min is extracted for the first time, decoction is filtered out, adds the water of 8 times of raw material weights, refluxing extraction 60min, merging is carried Take liquid；

Extract solution is concentrated under reduced pressure into density 1.03g/ml and obtains upper prop liquid；Enter HPD100 macroporous resin columns, be washed to eluent It is near colourless, then eluted with 3 ethanol of column volume 15% (v/v), 15% ethanol (v/v) eluent is collected, it is membrane separation concentrated to be reduced to admittedly It is spray-dried to obtain product 0.84kg after shape thing content 30%.

According to the content assaying method of 2010 editions pharmacopeia Syringins, analyze and detect through HPLC, Syringin purity is 85.27%.

Embodiment 5：

After iron holly bark pulverizing medicinal materials, 20 mesh sieves are crossed, claim 220kg to be placed in 3 tons of extractors, the water of 11 times of raw material weights is added 100 DEG C of extractions, extract 180min, filter out decoction for the first time, add the water of 9 times of raw material weights, and refluxing extraction 90min merges Extract solution；

Extract solution is concentrated under reduced pressure into density 1.03g/ml and obtains upper prop liquid；Enter AB-8 macroporous resin columns, be washed to eluent near It is colourless, then eluted with 4 ethanol of column volume 20% (v/v), 20% ethanol (v/v) eluent is collected, it is membrane separation concentrated to be reduced to solid It is spray-dried to obtain product 1.01kg after thing content 25%.

According to the content assaying method of 2010 editions pharmacopeia Syringins, analyze and detect through HPLC, Syringin purity is 76.33%.

Embodiment 6：

After iron holly bark pulverizing medicinal materials, 20 mesh sieves are crossed, claim 220kg to be placed in 3 tons of extractors, the water of 9 times of raw material weights is added 100 DEG C of extractions, extract 120min, filter out decoction for the first time, add the water of 8 times of raw material weights, and refluxing extraction 90min merges Extract solution；

Extract solution is concentrated under reduced pressure into density 1.05g/ml and obtains upper prop liquid；Enter SP825 macroporous resin columns, be washed to eluent near It is colourless, then eluted with 4 ethanol of column volume 20% (v/v), 20% ethanol (v/v) eluent is collected, it is membrane separation concentrated to be reduced to solid It is spray-dried to obtain product 0.93kg after thing content 25%.

According to the content assaying method of 2010 editions pharmacopeia Syringins, analyze and detect through HPLC, Syringin purity is 78.37%.

Embodiment 7：

After iron holly bark pulverizing medicinal materials, 30 mesh sieves are crossed, claim 200kg to be placed in 3 tons of extractors, the water of 9 times of raw material weights is added Micro-boiling is extracted, and 180min is extracted for the first time, decoction is filtered out, adds the water of 8 times of raw material weights, refluxing extraction 90min, merging is carried Take liquid；

Extract solution is concentrated under reduced pressure into density 1.01g/ml and obtains upper prop liquid；Enter HP20 macroporous resin columns, be washed to eluent near It is colourless, then eluted with 5 ethanol of column volume 30% (v/v), 30% ethanol (v/v) eluent is collected, it is membrane separation concentrated to be reduced to solid It is spray-dried to obtain product 0.83kg after thing content 30%.

Embodiment 8：

After iron holly bark pulverizing medicinal materials, 50 mesh sieves are crossed, claim 200kg to be placed in 3 tons of extractors, the water of 10 times of raw material weights is added Micro-boiling is extracted, and 180min is extracted for the first time, decoction is filtered out, and adds the water of 8 times of raw material weights, and refluxing extraction 120min merges Extract solution；

Extract solution is concentrated under reduced pressure into density 1.01g/ml and obtains upper prop liquid；Enter HPD100 macroporous resin columns, be washed to eluent It is near colourless, then eluted with 4 ethanol of column volume 15% (v/v), 15% ethanol (v/v) eluent is collected, it is membrane separation concentrated to be reduced to admittedly It is spray-dried to obtain product 0.85kg after shape thing content 30%.

Claims

1. the method for separating syringin is extracted in a kind of medicinal material from iron holly bark, it is characterised in that comprise the following steps：

（1）Iron holly bark pulverizing medicinal materials are to 20 ~ 50 mesh, extracting in water 1 ~ 3 time, every time 60 ~ 180 min, merge extract solution, depressurize dense It is reduced to the g/ml of density 1.01 ~ 1.20 and obtains upper prop liquid；

（2）Upper prop liquid is entered into macroporous resin column, washed resin to efflux is closely colourless, then eluted with 10 ~ 40% ethanol (v/v), received Collect eluent, eluent through nanofiltration membrane is concentrated into total solid content 25 ~ 35% and obtains concentrate；

The macroreticular resin is nonpolar or low pole macroreticular resin；

Model AB-8, HPD100, D101, D130, SP825 or HP20 of the macroreticular resin；

The consumption of water is 2 ~ 6 times of resin column volume, and the consumption of 10 ~ 40% ethanol (v/v) is 2 ~ 7 times of resin column volume；

The membrane separation concentration technique, film used is polyamide high temperature NF membrane；

（3）Concentrate is spray-dried to obtain product；

Step（1）In, the consumption of water is 5 ~ 20 times of raw material weight；

Step（3）In, in the drying process with atomizing, 170 ~ 210 DEG C of EAT, 70 DEG C of temperature of charge, leaving air temp 90 ~ 120℃。