若干表面功能化修饰纤维素材料的制备及其应用
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摘要
随着全球经济和工业的高速发展,煤、石油、天然气等不可再生资源被大量消耗,环境污染问题也日益严重,人们开始关注可再生资源的开发和利用。纤维素物质是自然界最丰富的原材料,具有良好的生物相容性、生物降解性、柔韧性、无毒性、多孔性,因而有关纤维素材料的开发和应用成为了当前的研究热点之一。其中,新型纤维素功能材料,如膜材料、发光材料、智能响应材料、疏水材料、抗菌材料、凝胶材料、生物医用材料等被人们竞相开发,成为了纤维素科学领域的研究重点。
本文以天然纤维素物质(普通定量滤纸)为基底,以活性的钛酸四丁酯或锆酸四丁酯为前体物,通过表面溶胶-凝胶法在纤维素纳米纤维表面沉积超薄的金属氧化物凝胶膜(TiO2或Zr02凝胶层),从而活化相对惰性的纤维素表面,用以组装不同功能分子和客体物质,制备出各种具有特定功能和性质的纤维素功能材料,主要结论如下：
(1)寡聚核苷酸功能化的纤维素材料：以锆酸四丁酯为前体物,通过表面溶胶-凝胶法在纤维素纳米纤维表面沉积超薄的ZrO2凝胶层,然后利用磷酸基团与Zr02之间强的配位作用将大量端基磷酸化的探针DNA分子组装于其表面,得到寡聚核苷酸功能化的纤维素材料。SEM和TEM观察表明ZrO2凝胶层能在纳米尺度上复制纤维素的层次结构,即能在纤维素纳米纤维表面很好地覆盖,这为接下来探针DNA链的大量富集和目标DNA链的识别提供了有利条件。所制备的寡聚核苷酸功能化的纸能保持了较好的生物活性,能实现对与探针DNA链完全互补的目标DNA链的反复识别,且具有较好的选择性。相对与平面的石英片基底,纤维素基底具有大的表面积,因而探针DNA分子在纤维素基底上的组装量要远远高出其在石英片基底上的组装量,故基于纤维素基底的DNA识别体系的检测限能达纳摩尔级,要低于基于平面石英片基底的识别体系的检测限两个数量级。此外,对比实验表明,ZrO2凝胶层对于探针DNA的组装和接下来的识别都是必不可少的。
(2)基于纤维素材料的半胱氨酸比色传感器：以锆酸四丁酯为前体物,通过表面溶胶-凝胶法在纤维素纳米纤维表面沉积超薄的ZrO2凝胶层,然后利用羧基与Zr02之间强的配位作用将大量的N719-Hg2+复合物组装于其表面,得到纸质的半胱氨酸比色传感器(类似pH试纸),显示出橙色。半胱氨酸分子中含有游离的巯基,与Hg的结合能力很强,因而当传感器材料与半胱氨酸水溶液接触时,固定在纤维素纤维表面的N719-Hg2+复合物中的Hg能被半胱氨酸夺取,橙色的传感材料立即变为紫色(染料N719的颜色),同时该材料UV-vis谱图中的某一谱带在传感后发生了480nm到520nm的红移,很好地对应了材料颜色的转变。该检测体系方便、快速具有很好的便携性,其检测限低至20μM,且具有很好的选择性,对其它19种天然氨基酸及其混合物均无变色响应。同时该检测体系具有良好的抗干扰能力,能够将其从包含其它19种天然氨基酸的混合溶液中检测出来。我们对该传感材料的重复利用性质也做了研究,通过半胱氨酸和Hg(N03)2水溶液的交替处理可以实现反复使用。此外,对比实验表明,Zr02凝胶层对于N719-Hg2+复合物组装的组装和接下来的比色传感都是必不可少的。
(3)抗菌的纤维素材料：以钛酸四丁酯和壳聚糖乳酸盐为前体物,通过LbL的方法在滤纸基底的纤维素纤维表面交替沉积二氧化钛凝胶层和壳聚糖层得到纤维素/二氧化钛/壳聚糖复合材料。该材料在微观的纳米层次上具有独特的电缆状的核-壳结构,表现为纤维素纳米纤维的核以及核表面所包覆的平整且均匀的二氧化钛/壳聚糖复合物壳,对于10个二氧化钛/壳聚糖双层的膜来说,其平均后都为14nm)。将沉积有二氧化钛/壳聚糖复合物膜的纤维素材料用于Ag+吸附再在紫外光的照射下将其原位还原,产生银纳米颗粒,得到纤维素/二氧化钛/壳聚糖/银纳米颗粒复合材料。该材料在微观的纳米层次上同样具有电缆状的核-壳结构,表现为纤维素纳米纤维的核、核表面所包覆的均匀的二氧化钛/壳聚糖/银纳米颗粒复合物壳,以及均匀分布在纳米纤维表面的粒径在4-10nm的银纳米颗粒。此外,抗菌实验表明,表而功能化修饰的纤维素材料对大肠杆菌和金黄色葡萄球菌均具有一定的抗菌活性。其中二氧化钛/壳聚糖复合物膜修饰的纤维素材料的抗菌效率低于60%,而二氧化钛/壳聚糖/银纳米颗粒复合物膜修饰的纤维素材料由于高的银含量使其能杀死几乎所有接种的细菌,表现出优异的抗菌能力。
(4)具有催化性能的纤维素材料：以钛酸四丁酯为前体物,通过表面溶胶-凝胶法在纤维素纳米纤维表面沉积超薄的Ti02凝胶层。然后采用LbL的方法,通过静电作用将阳离子聚电解质PDDA层以及带负电的KAuCl4和阴离子聚电解质PSS双组分层交替组装到Ti02凝胶层覆盖的纤维素纳米纤维表面,之后用NaBH4水溶液将组装的KAuCl4原位还原成金纳米颗粒,得到金纳米颗粒修饰的纤维素材料。该材料继承了原有纤维素物质层次的纤维状结构：具有典型的金纳米颗粒表面等离子体共振吸收,表现为UV-vis谱图中在520nm处有一明显的吸收峰；其纤维素纳米纤维表面附着着许多粒径在5nm左右的金纳米颗粒。该材料对NaBH4还原4-硝基苯酚(4-NP)的反应具有明显的催化效果,10mL反应液(其中4-NP的浓度为0.1mM, NaBH4的浓度为10mM)经金纳米颗粒修饰的纤维素材料(cellulose/(TiO2)5/Au@(PDDA/PSS)10)过滤一次后,4-NP的转化率高达74.0%,经三次过滤后转化率高达98.7%；相比之下,纯滤纸、沉积有二氧化钛凝胶膜的滤纸以及沉积有二氧化钛凝胶层和聚电解质PDDA/PSS多层的滤纸对该反应均无催化效果,同时对4-NP也无明显吸附作用。
With the rapid development of the global economy and industry, nonrenewable resources such as coal, petroleum and natural gas has been excessively consumed, giving rise to the serious environmental pollution, therefore, more and more attention was paid to the renewable resources. Among them, cellulose substance is the richest raw material in the word, which possesses good biocompatibility, biodegradability, flexibility, nontoxicity and porosity, hence the research regarding the functionalization and application of cellulose materials becomes one of the hottest spots in material research community. Meanwhile, various functional cellulose materials like membrane materials, luminescent materials, smart responsive materials, hydrophobic materials, antibacterial materials, gel materials and medical materials have been largely explored, being the focus in the scope of cellulose science.
Herein, employing natural cellulose substance (ordinary quantitative filter paper) as substrate and metal alkoxide (titanium(IV)n-butoxide or zirconium(IV)n-butoxide) as precursor, an ultrathin metaloxide (TiO2or ZrO2) gel film was first deposited onto cellulose nanofibers of filter paper by means of a surface sol-gel process. The deposited metaloxide gel layer activated the relatively inert surface of cellulose fibers and favord the following immobilization of different functional molecules or guest substances onto its surface, which endowed the cellulose materials with desired functionalities and properties, resulting in lots of advanced functional cellulose materials. The details are described as follows.
(1) Oligonecleotide-functionalized cellulose material:Employing zirconium(IV) n-butoxide as precursor, uniform ultrathin zirconia gel film was first deposited on each cellulose nanofiber in bulk filter paper by a facile surface sol-gel process. Relying on the large surface area and strong affinity of zirconia for phosphate group, terminally phosphated probe DNA was abundantly immobilized on the cellulose fibers so as to convert the composite into a biofunctional material for sensitive, selective and repetitive recognition for the corresponding complementary target DNA at a nanomolar level. By contrast, in spite of the viability of immobilization of probe DNA and recognition of target DNA on quartz plate, the amount of captured probe DNA or recognized target DNA on such flat substrate, was much less than that captured or recognized on filter paper, resulting in relatively insensitive recognition event. Moreover, control experiments on bare filter paper (without zirconia nanocoating) suggested that the zirconia gel film was essential for probe DNA immobilization and the subsequent target DNA recognition.
(2) Cellulose based colorimetric cysteine (Cys) chemosensor:Employing zirconium(Ⅳ) n-butoxide as precursor, uniform ultrathin zirconia gel film was first deposited on each cellulose nanofiber in bulk filter paper by a facile surface sol-gel process. Immobilization of ruthenium dye-Hg2+complex (N719-Hg2+complex) monolayer on such ultrathin zirconia gel film coated cellulose nanofibers of filter paper was conducted to fabricate a solid-phase sensing device with high sensitivity, selectivity and reversibility for colorimetric detection of Cys in aqueous media. This assay relied on the specific mercury displacement by cysteine from the immobilized N719-Hg2+complex. The dissociation of N719and Hg2+caused by such mercury displacement engendered obvious orange-to-purple color change of the zirconia gel layer and N719-Hg2+complex modified filter paper as well as the corresponding band shift from480nm to520nm in UV-vis spectra, hence realizing the colorimetric detection of cysteine. The detection limit of this assay is20μM by the naked eye and the selectivity for Cys against interference of the other19natural amino acids and their mixture is extremely high. Additionally, the deposition of the zirconia gel film onto cellulose fibers was crucial, and without the metal oxide layer, immobilization of the N719-Hg2+complex and subsequent Cys sensing would not be accomplished.
(3) Antibacterial cellulose material:organic/inorganic hybrid materials comprised of titania/chitosan composite were uniformly coated on cellulose nanofibers of filter paper by alternately depositing titania gel layer and chitosan layer for a given number of times. The resultant surface-modified cellulose nanofibers possessed a cable-like core-shell structure, showing cellulose nanofiber core adhered with flat and homogeneous titania/chitosan composite shell, whose average thickness is14nm for10-cycle deposition of titania/chitosan bilayer. By adsorbing silver ions with titania/chitosan composite modified paper followed by reducing the immobilized silver ions with UV irradiation, another kind of organic/inorganic hybrid nanocoating composed of titania/chitosan/silver composite was uniformly deposited on cellulose nanofibers of filter paper. Such resultant surface-decorated cellulose nanofibers also possessed a core-shell structure, exhibiting cellulose nanofiber core coated with14-nanometer-thick titania/chitosan/Ag composite shell for10-cycle titania/chitosan bilayer deposition as well as polydispersed nanosized silver particles (4-20nm in diameter) well distributed on the shell. Moreover, antibacterial tests suggested that the titania gel film coated cellulose papers and the titania/chitosan composite modified cellulose papers exhibited moderate antibacterial activity against E. coli and S. aureus with the antibacterial effects not more than60%, while the titania/chitosan/silver composite decorated cellulose papers nearly disinfected all the inoculated bacteria due to the high loading of Ag NPs, showing splendid antibacterial activity.
(4) Catalytic cellulose material:Employing titanium(IV) n-butoxide as precursor, uniform ultrathin titania gel film was first deposited on each cellulose nanofiber in bulk filter paper by a facile surface sol-gel process. Then, cationic polyelectrolyte layer PDDA as well as the two-component layer containing anionic polyelectrolyte PSS and KAuCl4were alternatively self-assembled onto the titania gel film pre-coated cellulose nanofibers of filter paper through electrostatic interaction. Followed by treatment with aqueous solution of NaBH4, the immobilized KAuCl4molecules were in situ reduced to Au NPs with the diameters about5nm, thus yielding Au NPs modified cellulose material, which inherited the original morphological characteristics of virgin cellulose substance with the hierarchically fibrous structures and exhibited typical SPR band around520nm in UV-vis spectra. Such Au NPs modified cellulose material also showed satisfactory catalytic activity toward the reduction reaction of4-nitrophenol (4-NP) with NaBH4in aqueous environment. By filtering10mL aqueous solution containing4-NP (0.1mM) mixed with NaBH4(10mM) through the Au NPs modified cellulose material (cellulose/(TiO2)5/Au@(PDDA/PSS)10) for one time, the conversion ratio of4-NP reached up to74.0%, which could be further promoted to98.7%after triple filtrations. In sharp contrast, pure filter paper, the titania gel film coated paper and the titania/PDDA/PSS multilayer modified paper displayed neither catalytic effect toward such reduction reaction nor apparent physical adsorption of4-NP.
本文以天然纤维素物质(普通定量滤纸)为基底,以活性的钛酸四丁酯或锆酸四丁酯为前体物,通过表面溶胶-凝胶法在纤维素纳米纤维表面沉积超薄的金属氧化物凝胶膜(TiO2或Zr02凝胶层),从而活化相对惰性的纤维素表面,用以组装不同功能分子和客体物质,制备出各种具有特定功能和性质的纤维素功能材料,主要结论如下：
(1)寡聚核苷酸功能化的纤维素材料：以锆酸四丁酯为前体物,通过表面溶胶-凝胶法在纤维素纳米纤维表面沉积超薄的ZrO2凝胶层,然后利用磷酸基团与Zr02之间强的配位作用将大量端基磷酸化的探针DNA分子组装于其表面,得到寡聚核苷酸功能化的纤维素材料。SEM和TEM观察表明ZrO2凝胶层能在纳米尺度上复制纤维素的层次结构,即能在纤维素纳米纤维表面很好地覆盖,这为接下来探针DNA链的大量富集和目标DNA链的识别提供了有利条件。所制备的寡聚核苷酸功能化的纸能保持了较好的生物活性,能实现对与探针DNA链完全互补的目标DNA链的反复识别,且具有较好的选择性。相对与平面的石英片基底,纤维素基底具有大的表面积,因而探针DNA分子在纤维素基底上的组装量要远远高出其在石英片基底上的组装量,故基于纤维素基底的DNA识别体系的检测限能达纳摩尔级,要低于基于平面石英片基底的识别体系的检测限两个数量级。此外,对比实验表明,ZrO2凝胶层对于探针DNA的组装和接下来的识别都是必不可少的。
(2)基于纤维素材料的半胱氨酸比色传感器：以锆酸四丁酯为前体物,通过表面溶胶-凝胶法在纤维素纳米纤维表面沉积超薄的ZrO2凝胶层,然后利用羧基与Zr02之间强的配位作用将大量的N719-Hg2+复合物组装于其表面,得到纸质的半胱氨酸比色传感器(类似pH试纸),显示出橙色。半胱氨酸分子中含有游离的巯基,与Hg的结合能力很强,因而当传感器材料与半胱氨酸水溶液接触时,固定在纤维素纤维表面的N719-Hg2+复合物中的Hg能被半胱氨酸夺取,橙色的传感材料立即变为紫色(染料N719的颜色),同时该材料UV-vis谱图中的某一谱带在传感后发生了480nm到520nm的红移,很好地对应了材料颜色的转变。该检测体系方便、快速具有很好的便携性,其检测限低至20μM,且具有很好的选择性,对其它19种天然氨基酸及其混合物均无变色响应。同时该检测体系具有良好的抗干扰能力,能够将其从包含其它19种天然氨基酸的混合溶液中检测出来。我们对该传感材料的重复利用性质也做了研究,通过半胱氨酸和Hg(N03)2水溶液的交替处理可以实现反复使用。此外,对比实验表明,Zr02凝胶层对于N719-Hg2+复合物组装的组装和接下来的比色传感都是必不可少的。
(3)抗菌的纤维素材料：以钛酸四丁酯和壳聚糖乳酸盐为前体物,通过LbL的方法在滤纸基底的纤维素纤维表面交替沉积二氧化钛凝胶层和壳聚糖层得到纤维素/二氧化钛/壳聚糖复合材料。该材料在微观的纳米层次上具有独特的电缆状的核-壳结构,表现为纤维素纳米纤维的核以及核表面所包覆的平整且均匀的二氧化钛/壳聚糖复合物壳,对于10个二氧化钛/壳聚糖双层的膜来说,其平均后都为14nm)。将沉积有二氧化钛/壳聚糖复合物膜的纤维素材料用于Ag+吸附再在紫外光的照射下将其原位还原,产生银纳米颗粒,得到纤维素/二氧化钛/壳聚糖/银纳米颗粒复合材料。该材料在微观的纳米层次上同样具有电缆状的核-壳结构,表现为纤维素纳米纤维的核、核表面所包覆的均匀的二氧化钛/壳聚糖/银纳米颗粒复合物壳,以及均匀分布在纳米纤维表面的粒径在4-10nm的银纳米颗粒。此外,抗菌实验表明,表而功能化修饰的纤维素材料对大肠杆菌和金黄色葡萄球菌均具有一定的抗菌活性。其中二氧化钛/壳聚糖复合物膜修饰的纤维素材料的抗菌效率低于60%,而二氧化钛/壳聚糖/银纳米颗粒复合物膜修饰的纤维素材料由于高的银含量使其能杀死几乎所有接种的细菌,表现出优异的抗菌能力。
(4)具有催化性能的纤维素材料：以钛酸四丁酯为前体物,通过表面溶胶-凝胶法在纤维素纳米纤维表面沉积超薄的Ti02凝胶层。然后采用LbL的方法,通过静电作用将阳离子聚电解质PDDA层以及带负电的KAuCl4和阴离子聚电解质PSS双组分层交替组装到Ti02凝胶层覆盖的纤维素纳米纤维表面,之后用NaBH4水溶液将组装的KAuCl4原位还原成金纳米颗粒,得到金纳米颗粒修饰的纤维素材料。该材料继承了原有纤维素物质层次的纤维状结构：具有典型的金纳米颗粒表面等离子体共振吸收,表现为UV-vis谱图中在520nm处有一明显的吸收峰；其纤维素纳米纤维表面附着着许多粒径在5nm左右的金纳米颗粒。该材料对NaBH4还原4-硝基苯酚(4-NP)的反应具有明显的催化效果,10mL反应液(其中4-NP的浓度为0.1mM, NaBH4的浓度为10mM)经金纳米颗粒修饰的纤维素材料(cellulose/(TiO2)5/Au@(PDDA/PSS)10)过滤一次后,4-NP的转化率高达74.0%,经三次过滤后转化率高达98.7%；相比之下,纯滤纸、沉积有二氧化钛凝胶膜的滤纸以及沉积有二氧化钛凝胶层和聚电解质PDDA/PSS多层的滤纸对该反应均无催化效果,同时对4-NP也无明显吸附作用。
With the rapid development of the global economy and industry, nonrenewable resources such as coal, petroleum and natural gas has been excessively consumed, giving rise to the serious environmental pollution, therefore, more and more attention was paid to the renewable resources. Among them, cellulose substance is the richest raw material in the word, which possesses good biocompatibility, biodegradability, flexibility, nontoxicity and porosity, hence the research regarding the functionalization and application of cellulose materials becomes one of the hottest spots in material research community. Meanwhile, various functional cellulose materials like membrane materials, luminescent materials, smart responsive materials, hydrophobic materials, antibacterial materials, gel materials and medical materials have been largely explored, being the focus in the scope of cellulose science.
Herein, employing natural cellulose substance (ordinary quantitative filter paper) as substrate and metal alkoxide (titanium(IV)n-butoxide or zirconium(IV)n-butoxide) as precursor, an ultrathin metaloxide (TiO2or ZrO2) gel film was first deposited onto cellulose nanofibers of filter paper by means of a surface sol-gel process. The deposited metaloxide gel layer activated the relatively inert surface of cellulose fibers and favord the following immobilization of different functional molecules or guest substances onto its surface, which endowed the cellulose materials with desired functionalities and properties, resulting in lots of advanced functional cellulose materials. The details are described as follows.
(1) Oligonecleotide-functionalized cellulose material:Employing zirconium(IV) n-butoxide as precursor, uniform ultrathin zirconia gel film was first deposited on each cellulose nanofiber in bulk filter paper by a facile surface sol-gel process. Relying on the large surface area and strong affinity of zirconia for phosphate group, terminally phosphated probe DNA was abundantly immobilized on the cellulose fibers so as to convert the composite into a biofunctional material for sensitive, selective and repetitive recognition for the corresponding complementary target DNA at a nanomolar level. By contrast, in spite of the viability of immobilization of probe DNA and recognition of target DNA on quartz plate, the amount of captured probe DNA or recognized target DNA on such flat substrate, was much less than that captured or recognized on filter paper, resulting in relatively insensitive recognition event. Moreover, control experiments on bare filter paper (without zirconia nanocoating) suggested that the zirconia gel film was essential for probe DNA immobilization and the subsequent target DNA recognition.
(2) Cellulose based colorimetric cysteine (Cys) chemosensor:Employing zirconium(Ⅳ) n-butoxide as precursor, uniform ultrathin zirconia gel film was first deposited on each cellulose nanofiber in bulk filter paper by a facile surface sol-gel process. Immobilization of ruthenium dye-Hg2+complex (N719-Hg2+complex) monolayer on such ultrathin zirconia gel film coated cellulose nanofibers of filter paper was conducted to fabricate a solid-phase sensing device with high sensitivity, selectivity and reversibility for colorimetric detection of Cys in aqueous media. This assay relied on the specific mercury displacement by cysteine from the immobilized N719-Hg2+complex. The dissociation of N719and Hg2+caused by such mercury displacement engendered obvious orange-to-purple color change of the zirconia gel layer and N719-Hg2+complex modified filter paper as well as the corresponding band shift from480nm to520nm in UV-vis spectra, hence realizing the colorimetric detection of cysteine. The detection limit of this assay is20μM by the naked eye and the selectivity for Cys against interference of the other19natural amino acids and their mixture is extremely high. Additionally, the deposition of the zirconia gel film onto cellulose fibers was crucial, and without the metal oxide layer, immobilization of the N719-Hg2+complex and subsequent Cys sensing would not be accomplished.
(3) Antibacterial cellulose material:organic/inorganic hybrid materials comprised of titania/chitosan composite were uniformly coated on cellulose nanofibers of filter paper by alternately depositing titania gel layer and chitosan layer for a given number of times. The resultant surface-modified cellulose nanofibers possessed a cable-like core-shell structure, showing cellulose nanofiber core adhered with flat and homogeneous titania/chitosan composite shell, whose average thickness is14nm for10-cycle deposition of titania/chitosan bilayer. By adsorbing silver ions with titania/chitosan composite modified paper followed by reducing the immobilized silver ions with UV irradiation, another kind of organic/inorganic hybrid nanocoating composed of titania/chitosan/silver composite was uniformly deposited on cellulose nanofibers of filter paper. Such resultant surface-decorated cellulose nanofibers also possessed a core-shell structure, exhibiting cellulose nanofiber core coated with14-nanometer-thick titania/chitosan/Ag composite shell for10-cycle titania/chitosan bilayer deposition as well as polydispersed nanosized silver particles (4-20nm in diameter) well distributed on the shell. Moreover, antibacterial tests suggested that the titania gel film coated cellulose papers and the titania/chitosan composite modified cellulose papers exhibited moderate antibacterial activity against E. coli and S. aureus with the antibacterial effects not more than60%, while the titania/chitosan/silver composite decorated cellulose papers nearly disinfected all the inoculated bacteria due to the high loading of Ag NPs, showing splendid antibacterial activity.
(4) Catalytic cellulose material:Employing titanium(IV) n-butoxide as precursor, uniform ultrathin titania gel film was first deposited on each cellulose nanofiber in bulk filter paper by a facile surface sol-gel process. Then, cationic polyelectrolyte layer PDDA as well as the two-component layer containing anionic polyelectrolyte PSS and KAuCl4were alternatively self-assembled onto the titania gel film pre-coated cellulose nanofibers of filter paper through electrostatic interaction. Followed by treatment with aqueous solution of NaBH4, the immobilized KAuCl4molecules were in situ reduced to Au NPs with the diameters about5nm, thus yielding Au NPs modified cellulose material, which inherited the original morphological characteristics of virgin cellulose substance with the hierarchically fibrous structures and exhibited typical SPR band around520nm in UV-vis spectra. Such Au NPs modified cellulose material also showed satisfactory catalytic activity toward the reduction reaction of4-nitrophenol (4-NP) with NaBH4in aqueous environment. By filtering10mL aqueous solution containing4-NP (0.1mM) mixed with NaBH4(10mM) through the Au NPs modified cellulose material (cellulose/(TiO2)5/Au@(PDDA/PSS)10) for one time, the conversion ratio of4-NP reached up to74.0%, which could be further promoted to98.7%after triple filtrations. In sharp contrast, pure filter paper, the titania gel film coated paper and the titania/PDDA/PSS multilayer modified paper displayed neither catalytic effect toward such reduction reaction nor apparent physical adsorption of4-NP.
引文
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