WO2011051562A1 - Membranes destinées à des dosages à écoulement latéral - Google Patents

Membranes destinées à des dosages à écoulement latéral Download PDF

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Publication number
WO2011051562A1
WO2011051562A1 PCT/FI2010/050852 FI2010050852W WO2011051562A1 WO 2011051562 A1 WO2011051562 A1 WO 2011051562A1 FI 2010050852 W FI2010050852 W FI 2010050852W WO 2011051562 A1 WO2011051562 A1 WO 2011051562A1
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WIPO (PCT)
Prior art keywords
paper
membrane
use according
strip
pulp
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Application number
PCT/FI2010/050852
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English (en)
Inventor
Timo Lappalainen
Tuija Teerinen
Marika Kurkinen
Pia Vento
Tomi Erho
Original Assignee
Valtion Teknillinen Tutkimuskeskus
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Publication of WO2011051562A1 publication Critical patent/WO2011051562A1/fr

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Classifications

    • G—PHYSICS
    • G01—MEASURING; TESTING
    • G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N33/00—Investigating or analysing materials by specific methods not covered by groups G01N1/00 - G01N31/00
    • G01N33/48—Biological material, e.g. blood, urine; Haemocytometers
    • G01N33/50—Chemical analysis of biological material, e.g. blood, urine; Testing involving biospecific ligand binding methods; Immunological testing
    • G01N33/53—Immunoassay; Biospecific binding assay; Materials therefor
    • G01N33/543—Immunoassay; Biospecific binding assay; Materials therefor with an insoluble carrier for immobilising immunochemicals
    • G01N33/54366—Apparatus specially adapted for solid-phase testing
    • G01N33/54386—Analytical elements
    • G01N33/54387—Immunochromatographic test strips
    • G01N33/54388—Immunochromatographic test strips based on lateral flow
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D39/00—Filtering material for liquid or gaseous fluids
    • B01D39/14—Other self-supporting filtering material ; Other filtering material
    • B01D39/16—Other self-supporting filtering material ; Other filtering material of organic material, e.g. synthetic fibres
    • B01D39/1607—Other self-supporting filtering material ; Other filtering material of organic material, e.g. synthetic fibres the material being fibrous
    • B01D39/1615—Other self-supporting filtering material ; Other filtering material of organic material, e.g. synthetic fibres the material being fibrous of natural origin

Definitions

  • the present invention relates to membrane strips for lateral flow assays and to the production of the same. Description of Related Art
  • LFA tests are based on a highly sensitive and selective binding reaction between the target molecule (antigen) and the corresponding receptor (e.g.
  • LFA tests are widely used for diagnostic purposes.
  • LFA test is the human pregnancy test. Other applications are in the detection of toxic compounds on food, infectious diseases, allergens, chemical contaminants and in the testing of drugs of abuse etc. LFA tests are particularly useful in the area of point-of-care testing (POC), which eliminates the need of laboratory work conducted by trained personnel.
  • POC point-of-care testing
  • the liquid sample such as urine, blood, saliva, water or milk is placed on a test device and the test result can be detected visually in 5-30 minutes.
  • a conventionally designed lateral flow strip test is shown in Figure 1. It is composed of a reaction membrane 1, a sample pad 2, a conjugate pad 3 and an absorbent pad 6. The parts overlap onto one another and are laminated to the backing material 7 using a pressure-sensitive adhesive. From the sample pad 2, liquid is transferred onto the conjugate pad 3. The primary function of the conjugate pad 3 is to hold the detector particles in a dry state so that they are functionally stable until resuspended by the sample.
  • the absorbent pad 6 is placed at the distal end of the test strip. It absorbs excess liquid from the lateral flow membrane and holds it for the duration of the test. The absorbent pad 6 is often made out of cellulosic paper.
  • Backing 7 improves physical strength of the test strip and also prevents liquid flow out through the bottom of the components.
  • LFIA lateral flow immunoassay tests
  • antibodies to the analyte are used for recognition. Immunoglobulin loaded label particles are utilized to make antigens visible to the eye.
  • the two main formats of the LFIA test are competitive and direct (i.e. sandwich) formats.
  • sandwich In a direct LFIA test, an antibody specific for the analyte is immobilised on the membrane at the test line 4.
  • the detector reagent typically an antibody coupled to coloured latex or colloidal gold particles is deposited and dried on the conjugate pad 3.
  • a liquid sample which contains the analyte of interest e.g. an antigen
  • the analyte of interest e.g. an antigen
  • the liquid sample migrates to the next zone, the conjugate pad 3, where it re-mobilizes the dried labelled conjugate.
  • the analyte of interest e.g. the antigen
  • the reaction matrix is conventionally made out of nitrocellulose.
  • the analyte-detector reagent is trapped and the accumulation of coloured label particles results in the appearance of specific colour lines.
  • the colour intensity of the test line is normally directly proportional to the amount of analyte present in the sample.
  • the control line 5 which is usually deposited after the test line in the direction of flow, confirms correct test development. If the test is performed properly a control line should form, irrespective of the result on the test line.
  • LFA membrane strips for lateral flow assays
  • synthetic polymeric materials such as nitrocellulose, nylon, polyethersulfone and polyethylene, or from fused silica, nitrocelluose (in the following abbreviated NC) being the most widely used material.
  • NC fused silica
  • Nitrocelluloce is in use in very commercially available LFA tests.
  • NC membranes The manufacture of NC membranes has been developed for several decades.
  • NC membranes Commercially useful in LFA applications include relatively low cost, true capillary flow characteristics and high protein binding capacity.
  • a lateral flow assay test strip which comprises in the flow direction a selectively activated membrane for a test reaction and an absorption pad, wherein both the selectively activated membrane and the absorption pad are made from a paper strip material produced from bleached, short-fibered pulp of deciduous tree.
  • the lateral flow assay test strip is characterized by what is stated in the characterizing part of claim 20.
  • Considerable advantages are provided by the present invention.
  • use of bleached cellulose papers, optionally modified to improve wet strength and porosity, as membranes allows for the manufacture of a new type of LFA products, because paper is mechanically much stronger than unbacked membranes made of nitrocellulose and manufacturing of paper in large scale is much more inexpensive than that of nitrocellulose.
  • Protein binding capacity of fibrous structure can be increased to the sufficient level by
  • the present technology can also be used to assays employing the lateral flow principle, e.g. in enzyme or nucleic acid based assays, and in assays based on chemical reaction.
  • a cellulose paper when additionally and optionally treated with chemicals for modifying its properties, and manufactured to a suitable grammage, has properties which are similar to those of a nitrocellulose membrane.
  • the properties of a cellose paper which are of importance for its present use are tailored by the selection criteria and treatment step discussed below such that they do not deviate from those of a nitrocellulose membrane by more than about ⁇ 20 %.
  • a cellulose paper allows for its use as a replacement of a conventional nitrocellose membrane.
  • the cellulose paper can be used as such or provided with a backing layer.
  • the present invention provides cost effective, mass manufacturable, disposable systems, which exploit the benefits of paper or fibrous structure; e.g.
  • Figure 1 shows, in a schematic, perspective depiction, the main parts of a lateral flow assay strip
  • Figure 2 shows, similarly in a schematic, perspective depiction, an embodiment wherein a part of the paper membrane is used as a lateral flow membrane and the distal end of the strip is modified to work as an absorbent pad;
  • Figure 3 is a digital image of the visual tests for hemoglobin.
  • Figure 4 shows a photograph of the hydrophilic channel on 80 g/m 2 eucalyptus paper.
  • the present invention provides for the use as membrane strips in laminar flow assay of paper, in particular paper produced from bleached, short-fibered pulp of deciduous trees.
  • Blocking of the fibrous network Blocking of the membrane is used to prevent nonspesific binding of the detector particles and analyte. Immersion methods are often in use, when blocking membranes.
  • the addition of of blocking agents has to be done on dry web, because blocking agents are normally applied after the addition of antibodies on the test line. Therefore the wet strength of paper membrane must be good.
  • paper based on short-fibered pulp of deciduous tree is capable of meeting a number of the listed properties. Firstly, formation of the paper is good.
  • this kind of paper has consistent flow characteristics and modification of wicking rate is easy.
  • wet strength of paper membrane is also good, which is important because some of the functionalization treatments and blocking of paper membrane are done to dry paper.
  • the mass-manufacturability using roll-to-roll printing or printing like methods gravure, flexo, inkjet or screen printing, coating and soaking) of the final LFA assay, a highly valuable property, is also present.
  • the present paper has a good and uniform optical and surface quality of the fibrous network, which provides for a clear test result.
  • Cellulose papers are commonly used for sample and adsorption pads.
  • the present technology describes how fibrous network can be further modified in order to allow for efficient use of paper as a membrane material.
  • Pulp type affects formation, brightness, wet strength and lateral flow speed of the membrane. Formation is an extremely important property of the paper membrane. If the paper formation is poor there can be large local variations in several paper properties causing variation between test strips. Therefore the reproducibility of performance can be poor.
  • a pulp is selected having a specific formation index (Sfi) of the paper membrane of about 0.2 to 1.2 Vg/m 2 , in particular (for handsheets) about 0.2 to about 0.5 Vg/m 2 , for example about 0.40 Vg/m 2 ⁇ 20 %.
  • the specific formation index (Sfi) of a paper membrane made of unbeaten, bleached, eucalyptus pulp, in particular one having a grammage of 80 g/m 2 is 0.40 Vg/m 2 .
  • the brightness of the paper used as a membrane should be good, in general higher than about 88.5 %, in particular higher than about 90 % (ISO).
  • ISO 90 %
  • pulp of bleached, unbeaten eucalyptus is about 91 %. This value is only slightly smaller than that of nitrocellulose (94-95 %).
  • one embodiment comprises selecting a pulp which has been produced by a chemical pulping method, in particular an alkaline pulping method, preferably an alkaline pulping method capable of removing lignin from the pulp.
  • a chemical pulping method in particular an alkaline pulping method, preferably an alkaline pulping method capable of removing lignin from the pulp.
  • a specific example of a suitable pulping method is the traditional or extended sulphate pulping, in batch or continuously.
  • the pulp is preferably bleached.
  • the bleaching process can be carried out using bleaching chemicals selected from the group of chlorine dioxide, peroxide chemicals and ozone and combinations thereof.
  • the paper strips have a fibrous matrix which comprises pulp of the above kind.
  • the papers which are used as membranes consist of, or consist essentially of, pulp of the above kind.
  • the membranes may contain in addition to the fibrous material of the pulp also various components which modify the properties of the material so that it is better suited for use in LFA.
  • the density of a handsheet made of the unmodified pulp is less than about 600 kg/m 3 .
  • "Unmodified” stands for a pulp which has not been treated with any modifying chemicals as will be described below.
  • the pulp is used in unbeaten state.
  • the pulp has been gently refined.
  • the gently refining comprises steps of improving at least one property selected from flexibility, fibrillation and surface properties, while essentially not changing the fibre length of the pulp.
  • the wet strength of higher grammage paper is higher than that of smaller grammage paper. But on the other, hand lateral flow speed decreaces as the grammage of paper increases. Therefore in one embodiment, the grammage of the paper is about 40 to 120 g/m 2 , preferably about 60 to 100 g/m 2 , for example about 70 to 90 g/m 2 , in particular about 80 g/m 2 , when using bleached, unbeaten, eucalyptus pulp. As mentioned above, the same grammage is applicable to pulp of other deciduous tree species.
  • CMC carboxymethyl cellulose
  • CMC carboxymethyl cellulose
  • Air permeability of an unbacked, optionally chemically modified (as described above) paper strip is, according to one embodiment, in the range of about 5300 ml/min ⁇ 20 %.
  • air permeability of an unbacked, optionally chemically modified (as described above) paper strip is, according to one embodiment, in the range of about 5300 ml/min ⁇ 20 %.
  • surfactant e.g. polyvinyl alcohol or polyoxy alcohol
  • Flow characteristics of paper membrane can be also modified by using additives like starch and starch derivatives, which causes changes to the hydrophilic properties of paper membrane.
  • wet strength chemicals were used.
  • the chemicals can be selected from, e.g. the group of polyamideamineepichlorohydrin (PAE) resin and urea- formaldehyde (UF) resin and mixtures thereof.
  • wet strength chemicals of the PAE type in dosages of 1 up to a mximum of about 20 g/kg fibrous matter, in particular about 2 to 5 g/kg fibrous matter, for example about 2.5 g/kg fibrous matter.
  • UF resin type chemicals can be added in dosages of 1 to 50 g/kg fibrous metier, in particular about 2 to 30 g/kg fibrous matter, in particular about 5 to 20 g/kg fibrous matter, for example about 10 g/kg fibrous matter.
  • a PAE resin (dosage 2.5 g/kg) or UF resin (dosage 10 g/kg) was sufficient when paper is made of eucalyptus pulp.
  • the properties of the cellulose paper have been modified by a combination of the above explained steps such as to obtain a paper strip having a capillary flow time of water which largely corresponds to that of the substrate now commonly in use (nitrocellulose, 315 s/40 mm for a strip having a grammage of about 40 g/m 2 ).
  • the capillary flow time of water for a present paper or handsheet is - as such - about 300 s/40 mm ⁇ 40 %, in particular, 300 s/40 mm ⁇ 30 %, preferably about 300 s/40 mm ⁇ 25 %.
  • Cellulose contains functional side groups that can be exploited in functionalization and immobilization.
  • chemical agents capable of reacting with the functional groups are used to provide surfaces capable of binding proteins and other analytes.
  • carbodiimide (CDI) and periodate are used for activating hydroxyl groups of cellulose.
  • Immobilization of proteins at cellulose surface can be achieved through the conjugation of activated groups to the amino groups of proteins. Immobilization can be carried out during antibody printing process, which enables high-throughput fabrication.
  • a blocking step which in one embodiment comprises the step of soaking the membrane with blocking substances, can be performed to prevent the nonspecific binding of proteins.
  • the blocking step can be carried out by printing or coating methods and therefore it can be included in the LFA roll-to-roll fabrication process.
  • the pore size distribution of paper membrane differs from that of nitrocellulose. Due to the smaller pore size large, conjugated latex beads are generally not capable of flowing into the paper membranes. However, according to one embodiment of the invention, colloidal gold particles or other small-sized labels are used with the paper membranes
  • Figure 2 illustrates an embodiment, wherein a part of the paper membrane can be used as a lateral flow membrane and the distal end of the strip is mechanically (and chemically) modified to function as an absorbent pad.
  • nitrocellulose is mechanically very weak and its structure cannot be modified to be suitable for use as an absorbent pad.
  • the use of a separate absorbent pad requires very accurate positioning and gluing of the absorbent pad.
  • paper membranes are mechanically stronger.
  • the absorbency of a paper membrane can be modified mechanically during the converting process; by embossing and by folding the paper strip several times. When folding the paper several times a layered z- directional paper-air-paper structure having high absorbency is created (see Fig 2).
  • the embossing creates "void areas" allowing the strip to hold more liquid.
  • the liquid absorption properties of the distal end of the paper test strip are modified in such a way that the distal end of the paper strip works as an absorption pad. In this case there are no overlaps. Therefore the manufacturing of the immunoassay test is easier and the manufacturing costs are reduced.
  • the absorption pad of the membrane is formed by a portion of the paper strip which is embossed or folded to increase the absorption capacity of the strip.
  • the absorption pad can comprise transversal paper strip folding to provide a plurality of adjacent paper layers.
  • eucalyptus pulp As a raw material of a test strip bleached eucalyptus pulp was selected.
  • the eucalyptus pulp was obtained from a pulp mill and comprised a pulp produced by the sulphate method (Kraft pulps) and bleached using ECF method (elemental chlorine free). This chemical pulp had been delivered as dry pulp sheets.
  • the eucalyptus pulp with short fibres and a narrow fibre length distribution, had good formation as necessary for the paper membrane.
  • a 80 g/m 2 eucalyptus paper was selected, because its properties were close to the properties of a typical nitrocellulose membrane.
  • the paper was produced from an unbeaten, once-dried pulp and contained a wet strength improving chemical (PAE) in a dosage of 2.5 g/kg dry matter (fibres).
  • PAE wet strength improving chemical
  • the composition of the blocking buffer had a profound effect on the speed of the test and on the flow of conjugated colloidal gold on the paper membrane. However, by modifying the buffer compositions it was possible to select a buffer which gave a proper flow and assay sensitivity.
  • the optimal blocker consisted of 3% BSA and 0.1% Tween in a 0.1 M PBS. Obviously, these high concentrations of blocking agents were advantageous for the type of paper developed in this work, because without any blocker, the determined flow rate was high compared to the types of nitrocellulose with the highest flow rates.
  • Figure 3 shows digital images of the visual test for hemoglobin.
  • the LFIA was performed in a one-step sandwich format.
  • the immobilized amounts of anti-hemoglobin (on test line) and anti-mouse (on the control line) were 1.0 ⁇ g/5 mm. Different concentrations of hemoglobin standards are indicated.
  • the wicking time was 2 min and in even higher concentrations, up to 5% BSA in a 0.1 M PBS, the wicking time was as high as 5 min.
  • the sensitivity of the hemoglobin assay and intensity of the test line were somewhat lower.
  • the intensity of the colour development on the test line was proportional to the amount of hemoglobin present in the sample at lower concentrations of hemoglobin, i.e. 0 to 100 ng/ml, and as such the paper-based lateral flow immunoassay can be regarded as a quantitative test for hemoglobin.
  • the cut-off level of 100 ng/ml of hemoglobin is often suggested. The lowest detectable signal was observed at 10 ng/ml and therefore, the developed paper-based test can be presumed to meet the required sensitivity of a diagnostic test.
  • Hydrophilic microchannels on 80 g/m 2 paper membrane made of unbeaten, bleached eucalyptus pulp with PAE (2.5 g/kg), were generated using the method presented in literature (Martinez, A., Phillips, S.T., Wiley, B., Gupta, M. and Whitesides (2008): H.M. FLASH: A rapid method for prototyping paper-based microfluidic devices. Lab Chip (8), 2146). Hydrophobic regions were made on hydrophilic paper using photolithography and conventional photoresist (SU-8). It was noticed that our 80 g/m 2 eucalyptus paper sustains washing with acetone well and more importantly the remaining polymerized photopolymer extends >150 ⁇ through the thickness of the paper. According to the literature cited above, the penetration of polymerized photopolymer has normally been limited to 70 um.
  • Figure 4 shows a photograph of the hydrophilic channel on 80 g/m2 eucalyptus paper.
  • the width of the microfluidic channel is 6 mm.
  • the sample was imaged using a backlight. The transmission of light is higher on the hydrophobic area than on the hydrophilic area.
  • the capillary flow time of the hydrophilic area was increased by about 70% due to the treatment. No change in the wet strength was noticed. The time to break of the paper was 45 minutes both before and after the treatment.

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Abstract

La présente invention concerne les étapes de traitement nécessaires à la fabrication à faible coût de systèmes de dosages à écoulement latéral (LFA) à base de papier par rapport à des produits actuels. De plus, le faible coût et l'utilisation de l'impression comme procédé de fabrication des LFA permettent d'utiliser les systèmes de LFA dans des applications complètement nouvelles, par exemple des produits de grande diffusion liés au mode de vie. Le but de l'invention est de développer des systèmes jetables, de grande diffusion, à faible coût, lesquels exploitent les avantages du papier ou d'une structure fibreuse, par exemple, la biodégradabilité, le faible coût et la capacité de transférer des liquides.
PCT/FI2010/050852 2009-10-27 2010-10-27 Membranes destinées à des dosages à écoulement latéral WO2011051562A1 (fr)

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FI20096105A FI20096105A0 (fi) 2009-10-27 2009-10-27 Menetelmä lateraalivirtausmembraanin valmistamiseksi ja membraani

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Cited By (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP2427770A1 (fr) * 2009-05-04 2012-03-14 Teknologian Tutkimuskeskus VTT Bande d'épreuve de dosage à écoulement latéral et son procédé de fabrication
US20120202211A1 (en) * 2011-02-08 2012-08-09 The Board Of Regents For Oklahoma State University Apparatus and method for biologic sample rapid collection and recovery device, and convenient storage
WO2017066645A1 (fr) 2015-10-15 2017-04-20 Inbios International, Inc. Systèmes de dosage à écoulement latéral multiplexé et leurs procédés d'utilisation
CN110031617A (zh) * 2019-04-17 2019-07-19 厦门大学 一种用于免疫诊断的一维纸芯片及其制备方法与应用
US10458067B2 (en) 2017-01-31 2019-10-29 Kimberly-Clark Worldwide, Inc. High bulk tissue comprising cross-linked fibers
WO2021083983A1 (fr) 2019-10-29 2021-05-06 Lifesure Limited Immunodosage à écoulement latéral, et ses utilisations
WO2022069470A1 (fr) * 2020-09-30 2022-04-07 Merck Patent Gmbh Papiers en nitrocellulose, procédés de production et d'utilisation
CN115506179A (zh) * 2022-09-26 2022-12-23 陕西科技大学 一种硝酸纤维素/植物纤维复合膜及其制备方法
US11970819B2 (en) 2020-01-30 2024-04-30 Kimberly-Clark Worldwide, Inc. Tissue products comprising crosslinked fibers

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US20030045001A1 (en) * 2001-08-29 2003-03-06 Deborah Burgess Immunochromatographic test strip with arcuate sample application zone for ease-of-use in the field
WO2003023371A1 (fr) * 2001-09-10 2003-03-20 Quidel Corporation Procede d'addition d'une ligne transparente d'absence de signal a un test rapide de diagnostic
WO2008030546A2 (fr) * 2006-09-06 2008-03-13 Ouantrx Biomedical Corporation Bandelette réactive pour chromatographie avec marqueur mobile
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WO1996035123A1 (fr) * 1995-05-02 1996-11-07 Carter Wallace, Inc. Dispositif et procede de diagnostic par detection
US20030045001A1 (en) * 2001-08-29 2003-03-06 Deborah Burgess Immunochromatographic test strip with arcuate sample application zone for ease-of-use in the field
WO2003023371A1 (fr) * 2001-09-10 2003-03-20 Quidel Corporation Procede d'addition d'une ligne transparente d'absence de signal a un test rapide de diagnostic
WO2008030546A2 (fr) * 2006-09-06 2008-03-13 Ouantrx Biomedical Corporation Bandelette réactive pour chromatographie avec marqueur mobile
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Cited By (13)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP2427770A1 (fr) * 2009-05-04 2012-03-14 Teknologian Tutkimuskeskus VTT Bande d'épreuve de dosage à écoulement latéral et son procédé de fabrication
EP2427770A4 (fr) * 2009-05-04 2012-11-28 Teknologian Tutkimuskeskus Vtt Oy Bande d'épreuve de dosage à écoulement latéral et son procédé de fabrication
US20120202211A1 (en) * 2011-02-08 2012-08-09 The Board Of Regents For Oklahoma State University Apparatus and method for biologic sample rapid collection and recovery device, and convenient storage
US9423398B2 (en) * 2011-02-08 2016-08-23 The Board Of Regents For Oklahoma State University Apparatus and method for biologic sample rapid collection and recovery device, and convenient storage
WO2017066645A1 (fr) 2015-10-15 2017-04-20 Inbios International, Inc. Systèmes de dosage à écoulement latéral multiplexé et leurs procédés d'utilisation
US10996221B2 (en) 2015-10-15 2021-05-04 Inbios International, Inc. Multiplexed lateral flow assay systems and methods for their use
US10458067B2 (en) 2017-01-31 2019-10-29 Kimberly-Clark Worldwide, Inc. High bulk tissue comprising cross-linked fibers
CN110031617A (zh) * 2019-04-17 2019-07-19 厦门大学 一种用于免疫诊断的一维纸芯片及其制备方法与应用
WO2021083983A1 (fr) 2019-10-29 2021-05-06 Lifesure Limited Immunodosage à écoulement latéral, et ses utilisations
US11970819B2 (en) 2020-01-30 2024-04-30 Kimberly-Clark Worldwide, Inc. Tissue products comprising crosslinked fibers
WO2022069470A1 (fr) * 2020-09-30 2022-04-07 Merck Patent Gmbh Papiers en nitrocellulose, procédés de production et d'utilisation
CN115506179A (zh) * 2022-09-26 2022-12-23 陕西科技大学 一种硝酸纤维素/植物纤维复合膜及其制备方法
CN115506179B (zh) * 2022-09-26 2023-11-21 陕西科技大学 一种硝酸纤维素/植物纤维复合膜及其制备方法

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