CN114956802A - 一种低导热红外发射材料及其制备方法与应用 - Google Patents
一种低导热红外发射材料及其制备方法与应用 Download PDFInfo
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Abstract
本发明公开了一种低导热红外发射材料及其制备方法与应用，属于红外节能技术领域。所述的低导热、高红外发射材料通过固相反应合成，合成产物为单一尖晶石物相，且产物元素分布均匀，属于AB2O4尖晶石结构，化学式为(Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)AlxCr2‑xO4。本发明采用MgO、Co3O4、NiO、CuO、ZnO、Al2O3、Cr2O3为原料，按照原子比Mg：Co：Ni：Cu：Zn：(Al+Cr)＝1:1:1:1:1:1:10球磨混合，干燥筛分后，通过压制成型，最后通过高温烧结得到(Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)AlxCr2‑xO4高熵材料。所述红外发射材料热导率低至0.7W m‑1 K‑1，红外发射率为0.86～0.98，具有优异的高温稳定性和耐腐蚀性能，节能效果好，在红外辐射、散热领域具有广泛的应用前景。
Description
技术领域
本发明红外节能技术领域，涉及一种红外节能材料的制备方法，具体涉及一种低导热红外发射材料及其制备方法与应用。
背景技术
工业炉是高温行业中必不可缺的关键设备，同时也是能源消耗最大的主体。在我国，工业炉的能耗约占全国工业总能耗的60％，占全国总能耗的25％。所以，为了实现“双碳”目标，节能降碳是工业炉减排的主要途径，这就需要解决炉内热利用效率和蓄热保温这个核心问题。源于这个大背景和目标，以改善表面辐射特性和强化辐射传热为目的的新型红外辐射节能材料应运而生。
朱杰制得了一种远红外涂料(专利号CN02137694.8)，其主要成分为炭化硅、氧化铁、氧化钴、氧化锰、氧化铝、氧化铬、氧化镍等，解决了当时技术中的红外涂料高温区存在发射率不高、不稳定、涂料粘接力不理想、影响散热效果等不足的问题，但是存在高温稳定性差和远红外辐射率衰减快的缺点；王刚等人发明了一种具有尖晶石结构的高发射率红外节能高熵材料的制备方法(专利号CN202110805503.6)，这个材料是以尖晶石结构(A3O4结构)为主相，A位为Co、Cr、Fe、Mn、Ni、Mg、Cu、Zn、Al的三种到五种金属元素的高发射率红外节能高熵材料。这种高熵材料很好地解决了之前材料出现的高温稳定性差和远红外辐射率衰减快的问题，红外发射率高达0.95，但导热率较高；董淑娟等人发明了一种兼具低热导率和高红外发射率的陶瓷材料(专利号CN202110060049.6)，是为HfO2和Sm2O3为原料通过高温固相反应合成，其热导率为0.60～0.75W/(m·K)，中红外波段的发射率为0.90～0.95，但使用的原料为稀土元素，原材料价格高，不具备良好的经济效益。
因此，如何提供一种高温稳定、低导热、高红外发射率的红外发射材料及其制备方法是本领域技术人员亟需解决的问题。
发明内容
有鉴于此，本发明针对现有技术中存在的问题，提供一种低导热红外发射材料及其制备方法与应用。
需要说明的是，本发明为了同时满足低导热率、高红外发射率和经济效益。本发明利用高熵材料热力学上的高熵效应、动力学上的缓慢扩散效应、结构上的点阵畸变效应以及性能上的鸡尾酒效应，提供一种低导热、高红外发射材料及其制备方法，所得红外发射材料具有良好的节能效果，具有设备要求低、能耗低、成本低廉以及容易实现工业化生产的特点。
为了实现上述目的，本发明的技术方案如下：
一种低导热红外发射材料的制备方法，所述方法是以MgO、Co3O4、NiO、CuO、ZnO、Al2O3、Cr2O3为原料，按照原子比Mg：Co：Ni：Cu：Zn：(Al+Cr)＝1:1:1:1:1:10球磨混合，干燥筛分后，通过压制成型，最后常压高温烧结得到的高熵材料，即为所述低导热红外发射材料。
本发明由于采用等摩尔比的MgO、Co3O4、NiO、CuO、ZnO五种氧化物高温下与Al2O3和Cr2O3反应并固溶形成高熵AB2O4尖晶石结构，结构上具有严重的晶格畸变，声子散射增强，表现出极低的热导率。同时，高熵结构的鸡尾酒效应和能带结构变化导致红外辐射性能大幅提升。
其中，所述MgO可替换为Mg(OH)2或MgCO3；所述Co3O4可替换为CoO或Co(OH)2；所述NiO可替换为Ni(OH)2；所述Al2O3可替换为Al(OH)3。
优选的，所述Al和Cr的原子百分数分别为0～66.7％、0～66.7％，且(Al+Cr)的原子百分数为66.7％。
优选的，所述烧结温度为1000℃～1600℃，保温时间为4h～24h，且烧结气氛为空气、Ar、N2等非还原性气氛。
本发明的另一目的是提供一种由上述方法制备的红外发射材料，所述材料的结构式为(Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)AlxCr2-xO4。
本发明还有一个目的，就是提供所述低导热红外发射材料在红外节能中的应用。
具体地，公开所述低导热红外发射材料在钢铁冶金高温炉中降低红外辐射能量损耗中的应用。
经由上述的技术方案可知，与现有技术相比，本发明提供了一种低导热红外发射材料及其制备方法与应用，具有如下优异效果：
(1)本发明所制备的(Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)AlxCr2-xO4红外发射材料具有铝尖晶石、铬尖晶石结构，具有良好的高温稳定性、耐腐蚀性和抗热震性能，在较高温度条件下使用，能够保持稳定的服役性能和较好的服役寿命。
(2)本发明所制备的(Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)AlxCr2-xO4红外发射材料，具有的高熵结构具有较多的缺陷和晶格畸变效应，致使原子间的作用力差异增大，声子散射增强，热导率显著降低。此外，缺陷和晶格畸变会导致晶格周期性破坏，晶格振动的对称性降低，偶极矩变化增加，红外辐射能力增强。
(3)本发明所制备的(Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)AlxCr2-xO4红外发射材料，通过Al和Cr固溶，不仅能提高反应过程中的高温体积稳定性，还能调节材料的能带结构，扩展宽波段的红外发射性能。
综上所述，本发明制备的(Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)AlxCr2-xO4红外发射材料热导率低至0.7W·m-1·K-1，红外发射率为0.86～0.98，具有优异的高温稳定性和耐腐蚀性能，服役性能好。因此，本发明具有低导热、高发射、高温稳定、节能效果好的特点。
附图说明
为了更清楚地说明本发明实施例或现有技术中的技术方案，下面将对实施例或现有技术描述中所需要使用的附图作简单地介绍，显而易见地，下面描述中的附图仅仅是本发明的实施例，对于本领域普通技术人员来讲，在不付出创造性劳动的前提下，还可以根据提供的附图获得其他的附图。
图1为实施例1中(Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)Al2O4红外发射材料的XRD图谱
图2为实施例3中(Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)(AlCr)O4红外发射材料的热导率
图3为实施例3中(Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)(AlCr)O4红外发射材料的发射率。
具体实施方式
下面将结合本发明实施例中的附图，对本发明实施例中的技术方案进行清楚、完整地描述，显然，所描述的实施例仅仅是本发明一部分实施例，而不是全部的实施例。基于本发明中的实施例，本领域普通技术人员在没有做出创造性劳动前提下所获得的所有其他实施例，都属于本发明保护的范围。
本发明实施例公开了一种低导热红外发射材料及其制备方法。
为更好地理解本发明，下面通过以下实施例对本发明作进一步具体的阐述，但不可理解为对本发明的限定，对于本领域的技术人员根据上述发明内容所作的一些非本质的改进与调整，也视为落在本发明的保护范围内。
下面，将结合具体实施例，对本发明的技术方案进行进一步的说明。
实施例1：以MgO、Co3O4、NiO、CuO、ZnO、Al2O3粉体为原料，按照原子比Mg:Co:Ni:Cu:Zn:Al＝1:1:1:1:1:1:10球磨混合，80℃干燥后筛分，100MPa下通过压制成型，1500℃下通过固相反应烧结，最终得到(Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)Al2O4红外发射材料。该红外发射材料的热导率为2.6W·m-1·K-1，在3～5μm红外波段平均发射率为0.87。
从图1中可以看出，本实施例中制备的(Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)Al2O4红外发射材料为单一尖晶石相，没有其他杂相，表明形成尖晶石高熵结构。
实施例2：以MgO、Co3O4、NiO、CuO、ZnO、Cr2O3粉体为原料，按照原子比Mg:Co:Ni:Cu:Zn:Cr＝1:1:1:1:1:1:10球磨混合，80℃干燥后筛分，100MPa下通过压制成型，1300℃下通过固相反应烧结，最终得到(Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)Cr2O4红外发射材料。该红外发射材料的热导率为0.6W·m-1·K-1，在3～5μm红外波段平均发射率为0.91。
实施例3：以MgO、Co3O4、NiO、CuO、ZnO、Al2O3、Cr2O3粉体为原料，按照原子比Mg:Ni:Co:Cu:Zn:Al:Cr＝1:1:1:1:1:5:5球磨混合，80℃干燥后筛分，100MPa下通过压制成型，1600℃下通过固相反应烧结，最终得到(Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)(AlCr)O4红外发射材料。该红外发射材料的热导率为2.7W·m-1·K-1，在3～5μm红外波段平均发射率为0.92。
从图2、图3中可以看出，本实施例中制备的(Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)(AlCr)O4红外发射材料室温～800℃热导率为0.6～0.7W·m-1·K-1，在3～5μm红外波段发射率为0.86～0.98。
实施例4：以Mg(OH)2、Co(OH)2、Ni(OH)2、CuO、ZnO、Al(OH)3、Cr2O3粉体为原料，按照原子比Mg:Ni:Co:Cu:Zn:Al:Cr＝1:1:1:1:1:5:5球磨混合，80℃干燥后筛分，100MPa下通过压制成型，1500℃下通过固相反应烧结，最终得到(Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)(AlCr)O4红外发射材料。该红外发射材料的热导率为2.1W·m-1·K-1，在3～5μm红外波段平均发射率为0.90。
实施例5：以MgO、Co3O4、NiO、CuO、ZnO、Al2O3、Cr2O3粉体为原料，按照原子比Mg:Ni:Co:Cu:Zn:Al:Cr＝1:1:1:1:1:8:2球磨混合，80℃干燥后筛分，100MPa下通过压制成型，1500℃下通过固相反应烧结，最终得到(Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)(Al1.6Cr0.4)O4红外发射材料。该红外发射材料的热导率为2.3W·m-1·K-1，在3～5μm红外波段平均发射率为0.90。
实施例6：以MgO、Co3O4、NiO、CuO、ZnO、Al2O3粉体为原料，按照原子比Mg:Co:Ni:Cu:Zn:Al＝1:1:1:1:1:1:10球磨混合，80℃干燥后筛分，100MPa下通过压制成型，1600℃下通过固相反应烧结，最终得到(Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)Al2O4红外发射材料。该红外发射材料的热导率为2.8W·m-1·K-1，在3～5μm红外波段平均发射率为0.88。
对所公开的实施例的上述说明，使本领域专业技术人员能够实现或使用本发明。对这些实施例的多种修改对本领域的专业技术人员来说将是显而易见的，本文中所定义的一般原理可以在不脱离本发明的精神或范围的情况下，在其它实施例中实现。因此，本发明将不会被限制于本文所示的这些实施例，而是要符合与本文所公开的原理和新颖特点相一致的最宽的范围。
Claims (6)
1.一种低导热红外发射材料的制备方法，其特征在于，所述方法是以MgO、Co3O4、NiO、CuO、ZnO、Al2O3、Cr2O3为原料，按照原子比Mg：Co：Ni：Cu：Zn：(Al+Cr)＝1:1:1:1:1:10球磨混合，干燥筛分后，通过压制成型，最后常压高温烧结得到的高熵材料，即为所述低导热红外发射材料。
2.根据权利要求1所述的一种低导热红外发射材料的制备方法，其特征在于，所述MgO可替换为Mg(OH)2或MgCO3；所述Co3O4可替换为CoO或Co(OH)2；所述NiO可替换为Ni(OH)2；所述Al2O3可替换为Al(OH)3。
3.根据权利要求1所述的一种低导热红外发射材料的制备方法，其特征在于，所述Al和Cr的原子百分数分别为0～66.7％、0～66.7％，且(Al+Cr)的原子百分数为66.7％。
4.根据权利要求1所述的一种低导热红外发射材料的制备方法，其特征在于，所述烧结温度为1000℃～1600℃，保温时间为4h～24h，且烧结气氛为空气、Ar、N2等非还原性气氛。
5.一种如权利要求1～4任一所述方法制备的低导热红外发射材料，其特征在于，所述红外发射材料的结构式为(Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)AlxCr2-xO4(0≤x≤2)，及所述红外发射材料的热导率为0.7～3W·m-1·K-1。
6.一种如权利要求1～4任一所述方法制备的低导热红外发射材料或如权利要求5所述低导热红外发射材料在红外节能中的应用。
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