软木传热机理与保温性能优化研究
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摘要
软木是自然界中存在的天然隔热材料,本文以国产栓皮栎软木为对象,对比葡萄牙栓皮槠软木,研究了软木细胞的固相骨架的传热机理和热解特性,以及软木热处理后软木细胞固相骨架传热特性变化。最后对软木制品的保温隔热性能进行了优化研究。主要研究结果如下：
(1)将软木单体细胞的结构进行归纳和简化,构建了软木单体细胞传热模型,运用串-并联运算规则,得到固-气结构软木的等效导热系数公式,软木等效导热系数是孔隙率(φ)的函数,与固相导热系数(λs)、气相导热系数(λa)有关。软木等效导热系数的计算公式为：
可以通过等效导热系数方程预测软木制品的导热系数,导热系数的计算值和实测值两者之间平均误差为5.16%,最大误差为9.79%,满足Russell法平均误差和最大误差分别不超过6%和15%的要求。
(2)在软木的热解反应中,将热解过程划分为4个阶段,第一个阶段都出现一个明显的吸热峰,国产栓皮栎软木的吸热峰强度高于葡萄牙产栓皮槠软木。第三个阶段是软木热解的主要阶段,该阶段失重高达77.14～81.59%。整个热解过程是由软木中软木酯、木质素及纤维素等成分的热解过程的叠加组成；软木酯、木质素等成分的热稳定性好,延长了热解反应温度区间,延缓了软木的热解过程。
(3)计算出软木活化能较大,三种产地软木的平均活化能分别达到了172KJ·mol1(甘肃)、169KJ·mol-1(陕西)和164KJ·mol-1(葡萄牙),说明软木的燃烧很难进行,需要在较高的温度下,提供大量的能量时,热解才能发生。根据热分解速率方程导出相应的热解动力学方程,软木的热解反应机理可以用一个一级反应过程米较好地描述。
(4)通过对软木固相骨架的研究,发现栓皮栎和栓皮槠软木的等温吸附线属于Ⅲ型吸附等温线,吸附剂—吸附质之间的相互作用很弱,软木细胞壁没有吸附水的存在。栓皮栎软木细胞壁上有更多的孔隙和更大的比表面积,孔径分布主要位于20nm的范围内。陕西产栓皮栎软木的孔径在50nm以下的介孔高达90.77%,孔隙直径小于气体分子的自由程,消除了细胞壁孔径内气体本身的热传导,其等效导热系数很低。
(5)软木热处理后,软木细胞壁的化学成分出现变化：主要是2852cm-1-2920cm-1的蜡质C-H不对称伸缩和对称伸缩振动减弱,1700cm-1-1800cm-1的区域内出现酯类的羰基((?)C=0)特征峰,在1506cm-1处出现木质素的芳环骨架振动,以及在1456cm-1处出现半纤维素CH2弯曲振动和895cm-1处的β-D-葡萄糖的特征吸收峰,峰强在热处理中都有减弱。
(6)软木热处理后,甘肃产软木细胞壁比表面积呈增加趋势,从2.438m2/g增大到2.907m2／g,增加了16.13%。单点表面积、BJH吸附孔总容积呈减小趋势,细胞壁上孔隙直径分布向20nm以下的介孔集中,20nm以下的介孔分布强度更高,超过50nm的大孔数量明显减少。
(7)软木热处理后视觉特性出现明显变化：主要是明度降低,色差增大,且随处理温度的升高和时间的延长呈明显递增的趋势；热处理后软木的红绿轴色品指数a*和黄蓝轴色品指数b*有不同程度的规律性降低。热处理温度对软木明度和色差的影响远大于热处理时间的影响。
(8)软木制品的保温性能优化研究：同等容重条件下,粗粒颗粒所制备的软木制品的等效导热系数最小,保温性能最好。软木颗粒的粒度较小时,粒度的变化对软木制品保温性能的影响变小；软木粒度相同时,随着容重的增加,软木制品等效导热系数发生显著增加；热处理时间、软木制品容重对导热系数的影响显著。根据正交实验结果,找出优化的方案为：软木粒度为粗粒,软木制品容重为0.5g/cm3,热处理时间2小时。降低软木制品容重,增加热处理时间可以降低等效导热系数,有效提高软木制品保温隔热性能。
Cork is a natural thermal insulation material in the nature.The dissertation took the domestic cork (Quercus variabilis) as the research object, contrasted the Portuguese cork (Quercus suber), and studied the heat-transfer mechanism and the pyrolysis characteristics of the solid skeleton of the cork cells, and the heat-transfer characteristics changes of the solid skeleton of the cork cells after the heat treatment. Finally, the optimization research was implemented for the heat preservation and heat insulation performance of the cork products.The main research results are as follows:
(1) Summarized and simplified the monomer structure of the cork cells, constructed the heat-transfer model of cork monomer cell, and achieved the equivalent coefficient formula of thermal conductivity for the solid-gas structural cork through using the series and parallel operational rule of the thermal resistance. The equivalent coefficient of thermal conductivity of the cork, which is relevant to the solid coefficient of thermal conductivity (λs) and the gas coefficient of the thermal conductivity (λa), is a function about the porosity (φ). The equivalent coefficient formula of thermal conductivity of the cork is:
The the coefficient of thermal conductivity of the cork products can be predicted by the equivalent coefficient equationof thermal conductivity.
(2) In the pyrolysis reaction process of the cork, the dissertation divided the pyrolysis processinto four phases. The first phase has an obvious endothermic peak, and the endothermic peak intensity of the domestic cork is higher than the Portuguese cork. The third phase is the main pyrolysisphase of the cork, and the weight loss rate of the phase reached up to77.14～81.59%. The entire pyrolysis process is the superposition of the pyrolysis process ofvarious composition such as the cork ester, the lignin and cellulose etc. The cork ester, the lignin, etc. have good thermal stability, so the temperature range of pyrolysis reaction is extended and the pyrolysis process of the cork is delayed.
(3) Through calculating the activation energy, it is found that the corks from three production places have the larger activation energy, and the average activation energy of these corks respectively achieved172KJ·mol-1(Gansu),169KJ·mol-1(Shanxi) and164 KJ·mol-1(Portugal). Further, it indicated that the cork burning is hard to carry out, because it needed the higher temperatures and a lot of energy for the cork pyrolysis. According to the thermal decomposition rate equation, the corresponding pyrolysis kinetic equation of the cork was derived. The pyrolysis reaction mechanism of the cork can be better described by a first order reaction process.
(4) Based on the research for the cork solid skeleton, it is found that theadsorption isotherm of the cork (Quercus variabilis) and the cork (Quercus suber) were the type III adsorption isotherm, the interaction between the adsorbent and the adsorbate is very weak, and there aren't the absorbed water on the cell wall. On the cork cell walls (Quercus variabilis), there are more porosity and larger specific surface area, and the pore size is distributed mainly in the range of20nm. In the pores of Shaanxi cork, the mesoporous, which the pore diameter is under50nm, reached up to90.77%. The pore diameter of the mesoporous is less than the free path of gas molecules, so there is not the heat conduction of the gas inside the aperture of the cell wall, and the equivalent coefficient of thermal conductivity for Shanxi cork is very low.
(5) After heat treatment, the chemical composition of cork cell wall changed:the asymmetric and symmetric stretching vibration of the C-H bond in the waxiness between2852cm-1-2920cm-1is abate. Thecharacteristic peak of carbonyl [)C=0) in the esters appeared between1700cm-1-1800cm-1. The vibration of the aromatic ring skeleton in lignin appeared at1506cm-1. The bending vibration of the CH2bond in hemicellulose appeared at1456cm-1. The characteristic absorption peak of β-D-glucose appeared at895cm-1, and the peak strength has weakened in the heat treatment.
(6) After heat treatment, the specific surface area of Gansu cork cell walls showed an increase trend from2.438m2/g increases to2.907m2/g and decreased16.13%. The single point surface area and the total volume of BJH absorption pore showed a decrease trend. The pore diameter distribution at the cell walls concentrates to the mesoporous under20nm, and the distribution intensity of the mesoporous under20nm is higher, and the number of big pore more than50nm significantly reduced.
(7) After heat treatment, the visual features appeared obvious changes:The brightness reduced, the chromatic aberration increased, and both showed an obvious increasing trend with the rise of temperature and the extension of time. After heat treatment, the chromaticity index a*of cork red-green axis and the chromaticity index b*of cork yellow-blue axis showed the regularity decrease trend at different degree. The influence of heat-treatment temperature on the brightness and chromatic aberration for the cork is greater than the influence of the heat treatment time.
(8) The optimization research on thermal insulation properties of the cork products: Under the condition of the equal density, the cork products produced by the coarse particles have the minimum equivalent coefficient of thermal conductivity, and the best insulation performance. When cork particle size is smaller, the influence of the changes of the particle size on thermal insulation properties of the cork products is smaller. Under the condition of the same cork particle, the equivalent coefficient of thermal conductivity of cork products appeared an obvious increase trend with the increase of volume-weight. The heat treatment time and the volume-weight of cork products can obviously influence the coefficient of the thermal conductivity. According to the result of orthogonal experiment, and the dissertation found out the optimized solutions for:the cork particle size is the coarse particle, the volume-weight of the cork products is0.5g/cm3, and the heat treatment time is2hours. So, reducing the volume-weight of the cork products, and increasing the heat treatment time can decrease the equivalent coefficient of thermal conductivity, and efficiently improve the thermal insulating properties of cork products.
(1)将软木单体细胞的结构进行归纳和简化,构建了软木单体细胞传热模型,运用串-并联运算规则,得到固-气结构软木的等效导热系数公式,软木等效导热系数是孔隙率(φ)的函数,与固相导热系数(λs)、气相导热系数(λa)有关。软木等效导热系数的计算公式为：
可以通过等效导热系数方程预测软木制品的导热系数,导热系数的计算值和实测值两者之间平均误差为5.16%,最大误差为9.79%,满足Russell法平均误差和最大误差分别不超过6%和15%的要求。
(2)在软木的热解反应中,将热解过程划分为4个阶段,第一个阶段都出现一个明显的吸热峰,国产栓皮栎软木的吸热峰强度高于葡萄牙产栓皮槠软木。第三个阶段是软木热解的主要阶段,该阶段失重高达77.14～81.59%。整个热解过程是由软木中软木酯、木质素及纤维素等成分的热解过程的叠加组成；软木酯、木质素等成分的热稳定性好,延长了热解反应温度区间,延缓了软木的热解过程。
(3)计算出软木活化能较大,三种产地软木的平均活化能分别达到了172KJ·mol1(甘肃)、169KJ·mol-1(陕西)和164KJ·mol-1(葡萄牙),说明软木的燃烧很难进行,需要在较高的温度下,提供大量的能量时,热解才能发生。根据热分解速率方程导出相应的热解动力学方程,软木的热解反应机理可以用一个一级反应过程米较好地描述。
(4)通过对软木固相骨架的研究,发现栓皮栎和栓皮槠软木的等温吸附线属于Ⅲ型吸附等温线,吸附剂—吸附质之间的相互作用很弱,软木细胞壁没有吸附水的存在。栓皮栎软木细胞壁上有更多的孔隙和更大的比表面积,孔径分布主要位于20nm的范围内。陕西产栓皮栎软木的孔径在50nm以下的介孔高达90.77%,孔隙直径小于气体分子的自由程,消除了细胞壁孔径内气体本身的热传导,其等效导热系数很低。
(5)软木热处理后,软木细胞壁的化学成分出现变化：主要是2852cm-1-2920cm-1的蜡质C-H不对称伸缩和对称伸缩振动减弱,1700cm-1-1800cm-1的区域内出现酯类的羰基((?)C=0)特征峰,在1506cm-1处出现木质素的芳环骨架振动,以及在1456cm-1处出现半纤维素CH2弯曲振动和895cm-1处的β-D-葡萄糖的特征吸收峰,峰强在热处理中都有减弱。
(6)软木热处理后,甘肃产软木细胞壁比表面积呈增加趋势,从2.438m2/g增大到2.907m2／g,增加了16.13%。单点表面积、BJH吸附孔总容积呈减小趋势,细胞壁上孔隙直径分布向20nm以下的介孔集中,20nm以下的介孔分布强度更高,超过50nm的大孔数量明显减少。
(7)软木热处理后视觉特性出现明显变化：主要是明度降低,色差增大,且随处理温度的升高和时间的延长呈明显递增的趋势；热处理后软木的红绿轴色品指数a*和黄蓝轴色品指数b*有不同程度的规律性降低。热处理温度对软木明度和色差的影响远大于热处理时间的影响。
(8)软木制品的保温性能优化研究：同等容重条件下,粗粒颗粒所制备的软木制品的等效导热系数最小,保温性能最好。软木颗粒的粒度较小时,粒度的变化对软木制品保温性能的影响变小；软木粒度相同时,随着容重的增加,软木制品等效导热系数发生显著增加；热处理时间、软木制品容重对导热系数的影响显著。根据正交实验结果,找出优化的方案为：软木粒度为粗粒,软木制品容重为0.5g/cm3,热处理时间2小时。降低软木制品容重,增加热处理时间可以降低等效导热系数,有效提高软木制品保温隔热性能。
Cork is a natural thermal insulation material in the nature.The dissertation took the domestic cork (Quercus variabilis) as the research object, contrasted the Portuguese cork (Quercus suber), and studied the heat-transfer mechanism and the pyrolysis characteristics of the solid skeleton of the cork cells, and the heat-transfer characteristics changes of the solid skeleton of the cork cells after the heat treatment. Finally, the optimization research was implemented for the heat preservation and heat insulation performance of the cork products.The main research results are as follows:
(1) Summarized and simplified the monomer structure of the cork cells, constructed the heat-transfer model of cork monomer cell, and achieved the equivalent coefficient formula of thermal conductivity for the solid-gas structural cork through using the series and parallel operational rule of the thermal resistance. The equivalent coefficient of thermal conductivity of the cork, which is relevant to the solid coefficient of thermal conductivity (λs) and the gas coefficient of the thermal conductivity (λa), is a function about the porosity (φ). The equivalent coefficient formula of thermal conductivity of the cork is:
The the coefficient of thermal conductivity of the cork products can be predicted by the equivalent coefficient equationof thermal conductivity.
(2) In the pyrolysis reaction process of the cork, the dissertation divided the pyrolysis processinto four phases. The first phase has an obvious endothermic peak, and the endothermic peak intensity of the domestic cork is higher than the Portuguese cork. The third phase is the main pyrolysisphase of the cork, and the weight loss rate of the phase reached up to77.14～81.59%. The entire pyrolysis process is the superposition of the pyrolysis process ofvarious composition such as the cork ester, the lignin and cellulose etc. The cork ester, the lignin, etc. have good thermal stability, so the temperature range of pyrolysis reaction is extended and the pyrolysis process of the cork is delayed.
(3) Through calculating the activation energy, it is found that the corks from three production places have the larger activation energy, and the average activation energy of these corks respectively achieved172KJ·mol-1(Gansu),169KJ·mol-1(Shanxi) and164 KJ·mol-1(Portugal). Further, it indicated that the cork burning is hard to carry out, because it needed the higher temperatures and a lot of energy for the cork pyrolysis. According to the thermal decomposition rate equation, the corresponding pyrolysis kinetic equation of the cork was derived. The pyrolysis reaction mechanism of the cork can be better described by a first order reaction process.
(4) Based on the research for the cork solid skeleton, it is found that theadsorption isotherm of the cork (Quercus variabilis) and the cork (Quercus suber) were the type III adsorption isotherm, the interaction between the adsorbent and the adsorbate is very weak, and there aren't the absorbed water on the cell wall. On the cork cell walls (Quercus variabilis), there are more porosity and larger specific surface area, and the pore size is distributed mainly in the range of20nm. In the pores of Shaanxi cork, the mesoporous, which the pore diameter is under50nm, reached up to90.77%. The pore diameter of the mesoporous is less than the free path of gas molecules, so there is not the heat conduction of the gas inside the aperture of the cell wall, and the equivalent coefficient of thermal conductivity for Shanxi cork is very low.
(5) After heat treatment, the chemical composition of cork cell wall changed:the asymmetric and symmetric stretching vibration of the C-H bond in the waxiness between2852cm-1-2920cm-1is abate. Thecharacteristic peak of carbonyl [)C=0) in the esters appeared between1700cm-1-1800cm-1. The vibration of the aromatic ring skeleton in lignin appeared at1506cm-1. The bending vibration of the CH2bond in hemicellulose appeared at1456cm-1. The characteristic absorption peak of β-D-glucose appeared at895cm-1, and the peak strength has weakened in the heat treatment.
(6) After heat treatment, the specific surface area of Gansu cork cell walls showed an increase trend from2.438m2/g increases to2.907m2/g and decreased16.13%. The single point surface area and the total volume of BJH absorption pore showed a decrease trend. The pore diameter distribution at the cell walls concentrates to the mesoporous under20nm, and the distribution intensity of the mesoporous under20nm is higher, and the number of big pore more than50nm significantly reduced.
(7) After heat treatment, the visual features appeared obvious changes:The brightness reduced, the chromatic aberration increased, and both showed an obvious increasing trend with the rise of temperature and the extension of time. After heat treatment, the chromaticity index a*of cork red-green axis and the chromaticity index b*of cork yellow-blue axis showed the regularity decrease trend at different degree. The influence of heat-treatment temperature on the brightness and chromatic aberration for the cork is greater than the influence of the heat treatment time.
(8) The optimization research on thermal insulation properties of the cork products: Under the condition of the equal density, the cork products produced by the coarse particles have the minimum equivalent coefficient of thermal conductivity, and the best insulation performance. When cork particle size is smaller, the influence of the changes of the particle size on thermal insulation properties of the cork products is smaller. Under the condition of the same cork particle, the equivalent coefficient of thermal conductivity of cork products appeared an obvious increase trend with the increase of volume-weight. The heat treatment time and the volume-weight of cork products can obviously influence the coefficient of the thermal conductivity. According to the result of orthogonal experiment, and the dissertation found out the optimized solutions for:the cork particle size is the coarse particle, the volume-weight of the cork products is0.5g/cm3, and the heat treatment time is2hours. So, reducing the volume-weight of the cork products, and increasing the heat treatment time can decrease the equivalent coefficient of thermal conductivity, and efficiently improve the thermal insulating properties of cork products.
引文
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