木质材料表面装饰用材的光致变色机理的研究
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摘要
对木质材料表面进行装饰,在人居环境中已经成为人们追求高质量、高品位生活的基本要求。目前木质材料表面装饰的方法有很多,主要有贴面装饰和涂饰装饰两大类。但无论是哪一类,都存在光致变色的光劣化问题。因此,本文针对典型的表面装饰材料,即椴木单板、装饰纸(木纹纸与浸渍纸)、PVC贴面(深色与浅色两种)材料进行了其光致变色的研究。利用基于CIE1976标准色度系统LAB均匀颜色空间原理的分光光度计,探究其分别在自然光和紫外光辐照下的变色规律；利用X射线光电子能谱(XPS)、傅里叶变换红外光谱(FT-IR)、电子自旋共振波谱(ESR)、荧光显微镜等多种现代表面分析技术,揭示了装饰材料的表面化学结构变化和颜色产生的理学本质,从而分析和明确了光致变色机理；用紫外可见分光光度计测量了典型漆膜的透射光光谱；本研究旨在为装饰材料表面防止光劣化提供基础理论和科学依据。主要研究结果如下：
(1)光变色规律的共性是：与有机物键能较接近的紫外光引起的变色明显,主要表现是明度指数下降,黄蓝轴色品指数增加,红绿轴色品指数变化较小,色差大,视觉显示黄变；而自然光辐照的效果明显小于紫外光,变色规律基本一致；色差变化主要发生在开始的20小时左右,然后趋于稳定,紫外光的长时间辐照又能引起颜色的较大变化；形貌观测上表现粗糙度增大(PVC除外)。
(2)同样辐照条件各种装饰材料变色程度不同,其变色程度依次是椴木单板>PVC贴面>浸渍纸；色差随辐照时间的变化曲线各不相同(总体上分床型和椅子型)；木纹纸与浸渍纸原纸在本次实验条件下几乎没有发生光劣化现象,其原因是装饰原纸在生产过程中添加了大量钛白粉所致。
(3)变色明显的材料均观察到碳价态和自由基浓度的改变,且变化规律与颜色改变规律基本一致。主要体现部分低价态的碳原子转变成高价态,氧含量增加,自由基浓度增大；具体表现为高聚物的氧化降解,长分子链的断裂,生成类似于羟基和酮基或醛基为主的含氧基团；光辐照初期反应激烈变化大,然后不稳定的结构逐渐让位于稳定结构,表现出光化学反应趋缓和量子产率的下降。
(4)物体颜色感知最后来自于物体总反射光的光谱成分；总反射光中不仅包括物体选择吸收后的反射,还包含散射以及光的衍射现象。因此,应改变传统观念,即颜色变化的原因,不能片面地只强调因材料化学性质的改变,而导致材料对光选择吸收性质的改变。
(5)微观上没有绝对平整的表面,当表面空隙度满足光衍射条件时,总反射光中必定包含衍射的效果,表面空隙度变大时,导致总反射光中长波成分增加,红绿轴和黄蓝轴色品指数增大；若表面层材料(特别是胶体)发生瑞利散射,则也可以使总反射光中增加长波成分。因此,不同的材料,颜色改变(即光谱成分变化)的原因,选择吸收、散射和衍射三者所起的作用不同。即颜色变化的“光散射与衍射”物理解释。
(6)综合所有理论和实验说明,本研究的几种典型表面装饰材料光致变色总体的原因是：
椴木单板光辐照后颜色的改变,更多的是来自于木质素和抽提物氧化降解的缘故,即基本基团相对含量变化使选择吸收性质改变；伴随着木材生物结构(细胞壁和细胞腔)的变化衍射因素也会有影响；但散射因素基本不存在。
浸渍纸(经浸渍胶浸渍后的)光辐照后颜色的改变,一方面来自于高分子材料发色基团的变化(即化学键发生断裂及其重组),从而导致的选择吸收性质改变；另一方面胶层吸收辐射光能量后,分子的热运动促使表层组织不均匀程度发生变化,瑞利散射发生也造成反射光谱成分的改变；伴随形貌的改变光衍射的影响也会存在。
PVC贴面光辐照后颜色发生显著变化的原因,从碳价态相对很稳定的结果看,更多的应该是来自于物理的因素；即分子热运动加剧使颜料分子分布改变、不均匀尺度的变化等,但仍然不能排除衍射的存在。
本研究结果明潦了木质材料的表面装饰用材光致变色的规律和缘由,将为装饰材料的优化选用和科学保护提供理论依据,对提高产品的耐久性,改善人居环境的质量具有重要意义。
Nowadays, the surface decoration of wooden materials have become basic demand for high-quality, high-grade life in human settlement. Most methods can be used for the surface decoration of the wooden materials. And the veneered decoration and the coated decoration are the most important in these methods. However, the problem of damaging induced by light can be neglected neither in veneered decoration nor in coated decoration. In this work, the light-induced discoloration is investigated in basswood single board, decorative paper (wood-veined paper and impregnated paper) and PVC sticker (dark and light color). The spectrophotometer with the CIE chromaticity of 1976 is used to study the law of the change of color. While, we investigate the change of the surface-chemistry structure and the scientific essence of the producing of color, with surface-analysis technology such as x-ray photoelectron spectroscopy (XPS), fourier transform infrared spectroscopy (FT-IR), electron spin resonance spectroscopy (ESR), fluorescence display and so on. Furthermore, the ultraviolet spectrophotometer is also used to measure the transmission spectra of the typical paint films. In this work, we hope to provide basic and scientific theory to avoid damaging induced by light. The main results are shown as follow:
(1) The general characters of the light-induced discoloration are observed in basswood single board, decorative paper and PVC sticker when they are radiated by natural and ultraviolet light. After radiating, we observed basswood single board, decorative paper and PVC sticker by ultraviolet and find that the lightness index decrease, the yellow and blue index increase, the red and green index change little, chromatic difference become big and visual display become yellow. In addition, the color induced by the long-time ultraviolet radiation change more strongly. While the effect induced by natural light is smaller than induced by ultraviolet. The same light-induced discoloration phenomenon is observed in basswood single board, decorative paper and PVC sticker. The change of the chromatic difference is observed mainly in the early 20 hours, and then become steady. Furthermore, the rough index of the morphology increased (excepted PVC).
(2) Different decoration materials show different changeable effect of color under the same radiation. From basswood single board, decorative paper to PVC sticker, the change of the color decrease. The curves, which show chromatic difference with the time of radiation, are different (the curve are bed-model and chair-model). The damaging by light of wood-veined paper and impregnated paper are not observed in this experiment. It is because that the most of titanium dioxide is brought to wood-veined paper and impregnated paper.
(3) The change of carbon valence and free radical concentration can be observed in the obvious light-induced discoloration materials. And both of them are changing with color. Part of low valence carbon atoms turn to high valence carbon atoms, the content of oxygen increased. At the same time, free radical concentration increase. This can be shown by oxidative degradation of high polymer and rupture of long molecular chain, which produce oxygenic function comprised by hydroxy group, ketone group and aldehyde group. In addition, the change shown above is drastic at the beginning of the reaction, and then turn to steady.
(4) Object color-perception comes from the spectra of the overall reflected lights. The overall reflected lights are comprised not only by the reflex after selective absorption, but also by dispersion and diffraction. Therefore, the traditional view must be changed. The traditional view is that the change of color is not just because the light selective absorption change induced by the chemical property change of materials.
(5) The absolute flat surface is not observed in microcosm. When porosity can reach the diffraction condition of light, the total reflected light should include the effects of diffraction. The ingredient of the long wave increases, the red-green-axis and yellow-blue-axis color index become higher, as the porosity become bigger. Furthermore, Rayleigh scattering also makes the ingredient of long wavelengths increase in reflected lights. Therefore, selective absorption, scattering and diffraction play different roles to the reason of colors change in different materials. This is physical explanation to the color change of the "scattering and diffraction"
(6) According to analysis above, we conclude the light-induced discoloration of the typical surface decoration materials, which we chose, as follow:
The light-induced discoloration of basswood single board comes from lignin and oxidative degradation. With the biology configuration of wooden materials changed (cell wall and cell cavity), diffraction influent the change of color. However, scattering factor can not be observed in our experiments.
According to the light-induced discoloration of impregnated paper, on the one hand it comes from the chromophoric group change of high polymer materials, which make selective absorption-character changed; on the other hand it comes from the change of asymmetry-effect of surface organize induced by thermal motion of molecule after absorbing light radiation. This means that Rayleigh scattering can change reflected lights.
The reason of the light-induced discoloration of PVC sticker is from physical factor, which can be observed by the relative steady of carbon valence. Although the dramatic thermal motion of molecule change the asymmetry-effect of surface organize and the distribute of fuel molecule; the influence of diffraction can not be neglected.
In conclusion, the reason and law of the light-induced discoloration are synthesized. This will provide theoretical basis for the scientific protection and optimized selection of the decoration materials. In addition, it provide a very important significance to improve production durability and the quality of human settlement.
(1)光变色规律的共性是：与有机物键能较接近的紫外光引起的变色明显,主要表现是明度指数下降,黄蓝轴色品指数增加,红绿轴色品指数变化较小,色差大,视觉显示黄变；而自然光辐照的效果明显小于紫外光,变色规律基本一致；色差变化主要发生在开始的20小时左右,然后趋于稳定,紫外光的长时间辐照又能引起颜色的较大变化；形貌观测上表现粗糙度增大(PVC除外)。
(2)同样辐照条件各种装饰材料变色程度不同,其变色程度依次是椴木单板>PVC贴面>浸渍纸；色差随辐照时间的变化曲线各不相同(总体上分床型和椅子型)；木纹纸与浸渍纸原纸在本次实验条件下几乎没有发生光劣化现象,其原因是装饰原纸在生产过程中添加了大量钛白粉所致。
(3)变色明显的材料均观察到碳价态和自由基浓度的改变,且变化规律与颜色改变规律基本一致。主要体现部分低价态的碳原子转变成高价态,氧含量增加,自由基浓度增大；具体表现为高聚物的氧化降解,长分子链的断裂,生成类似于羟基和酮基或醛基为主的含氧基团；光辐照初期反应激烈变化大,然后不稳定的结构逐渐让位于稳定结构,表现出光化学反应趋缓和量子产率的下降。
(4)物体颜色感知最后来自于物体总反射光的光谱成分；总反射光中不仅包括物体选择吸收后的反射,还包含散射以及光的衍射现象。因此,应改变传统观念,即颜色变化的原因,不能片面地只强调因材料化学性质的改变,而导致材料对光选择吸收性质的改变。
(5)微观上没有绝对平整的表面,当表面空隙度满足光衍射条件时,总反射光中必定包含衍射的效果,表面空隙度变大时,导致总反射光中长波成分增加,红绿轴和黄蓝轴色品指数增大；若表面层材料(特别是胶体)发生瑞利散射,则也可以使总反射光中增加长波成分。因此,不同的材料,颜色改变(即光谱成分变化)的原因,选择吸收、散射和衍射三者所起的作用不同。即颜色变化的“光散射与衍射”物理解释。
(6)综合所有理论和实验说明,本研究的几种典型表面装饰材料光致变色总体的原因是：
椴木单板光辐照后颜色的改变,更多的是来自于木质素和抽提物氧化降解的缘故,即基本基团相对含量变化使选择吸收性质改变；伴随着木材生物结构(细胞壁和细胞腔)的变化衍射因素也会有影响；但散射因素基本不存在。
浸渍纸(经浸渍胶浸渍后的)光辐照后颜色的改变,一方面来自于高分子材料发色基团的变化(即化学键发生断裂及其重组),从而导致的选择吸收性质改变；另一方面胶层吸收辐射光能量后,分子的热运动促使表层组织不均匀程度发生变化,瑞利散射发生也造成反射光谱成分的改变；伴随形貌的改变光衍射的影响也会存在。
PVC贴面光辐照后颜色发生显著变化的原因,从碳价态相对很稳定的结果看,更多的应该是来自于物理的因素；即分子热运动加剧使颜料分子分布改变、不均匀尺度的变化等,但仍然不能排除衍射的存在。
本研究结果明潦了木质材料的表面装饰用材光致变色的规律和缘由,将为装饰材料的优化选用和科学保护提供理论依据,对提高产品的耐久性,改善人居环境的质量具有重要意义。
Nowadays, the surface decoration of wooden materials have become basic demand for high-quality, high-grade life in human settlement. Most methods can be used for the surface decoration of the wooden materials. And the veneered decoration and the coated decoration are the most important in these methods. However, the problem of damaging induced by light can be neglected neither in veneered decoration nor in coated decoration. In this work, the light-induced discoloration is investigated in basswood single board, decorative paper (wood-veined paper and impregnated paper) and PVC sticker (dark and light color). The spectrophotometer with the CIE chromaticity of 1976 is used to study the law of the change of color. While, we investigate the change of the surface-chemistry structure and the scientific essence of the producing of color, with surface-analysis technology such as x-ray photoelectron spectroscopy (XPS), fourier transform infrared spectroscopy (FT-IR), electron spin resonance spectroscopy (ESR), fluorescence display and so on. Furthermore, the ultraviolet spectrophotometer is also used to measure the transmission spectra of the typical paint films. In this work, we hope to provide basic and scientific theory to avoid damaging induced by light. The main results are shown as follow:
(1) The general characters of the light-induced discoloration are observed in basswood single board, decorative paper and PVC sticker when they are radiated by natural and ultraviolet light. After radiating, we observed basswood single board, decorative paper and PVC sticker by ultraviolet and find that the lightness index decrease, the yellow and blue index increase, the red and green index change little, chromatic difference become big and visual display become yellow. In addition, the color induced by the long-time ultraviolet radiation change more strongly. While the effect induced by natural light is smaller than induced by ultraviolet. The same light-induced discoloration phenomenon is observed in basswood single board, decorative paper and PVC sticker. The change of the chromatic difference is observed mainly in the early 20 hours, and then become steady. Furthermore, the rough index of the morphology increased (excepted PVC).
(2) Different decoration materials show different changeable effect of color under the same radiation. From basswood single board, decorative paper to PVC sticker, the change of the color decrease. The curves, which show chromatic difference with the time of radiation, are different (the curve are bed-model and chair-model). The damaging by light of wood-veined paper and impregnated paper are not observed in this experiment. It is because that the most of titanium dioxide is brought to wood-veined paper and impregnated paper.
(3) The change of carbon valence and free radical concentration can be observed in the obvious light-induced discoloration materials. And both of them are changing with color. Part of low valence carbon atoms turn to high valence carbon atoms, the content of oxygen increased. At the same time, free radical concentration increase. This can be shown by oxidative degradation of high polymer and rupture of long molecular chain, which produce oxygenic function comprised by hydroxy group, ketone group and aldehyde group. In addition, the change shown above is drastic at the beginning of the reaction, and then turn to steady.
(4) Object color-perception comes from the spectra of the overall reflected lights. The overall reflected lights are comprised not only by the reflex after selective absorption, but also by dispersion and diffraction. Therefore, the traditional view must be changed. The traditional view is that the change of color is not just because the light selective absorption change induced by the chemical property change of materials.
(5) The absolute flat surface is not observed in microcosm. When porosity can reach the diffraction condition of light, the total reflected light should include the effects of diffraction. The ingredient of the long wave increases, the red-green-axis and yellow-blue-axis color index become higher, as the porosity become bigger. Furthermore, Rayleigh scattering also makes the ingredient of long wavelengths increase in reflected lights. Therefore, selective absorption, scattering and diffraction play different roles to the reason of colors change in different materials. This is physical explanation to the color change of the "scattering and diffraction"
(6) According to analysis above, we conclude the light-induced discoloration of the typical surface decoration materials, which we chose, as follow:
The light-induced discoloration of basswood single board comes from lignin and oxidative degradation. With the biology configuration of wooden materials changed (cell wall and cell cavity), diffraction influent the change of color. However, scattering factor can not be observed in our experiments.
According to the light-induced discoloration of impregnated paper, on the one hand it comes from the chromophoric group change of high polymer materials, which make selective absorption-character changed; on the other hand it comes from the change of asymmetry-effect of surface organize induced by thermal motion of molecule after absorbing light radiation. This means that Rayleigh scattering can change reflected lights.
The reason of the light-induced discoloration of PVC sticker is from physical factor, which can be observed by the relative steady of carbon valence. Although the dramatic thermal motion of molecule change the asymmetry-effect of surface organize and the distribute of fuel molecule; the influence of diffraction can not be neglected.
In conclusion, the reason and law of the light-induced discoloration are synthesized. This will provide theoretical basis for the scientific protection and optimized selection of the decoration materials. In addition, it provide a very important significance to improve production durability and the quality of human settlement.
引文
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