CN102378809A - 作为源于生物的再生燃料和加热材料的柠檬酸酯 - Google Patents

作为源于生物的再生燃料和加热材料的柠檬酸酯 Download PDF

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CN102378809A
CN102378809A CN2010800157239A CN201080015723A CN102378809A CN 102378809 A CN102378809 A CN 102378809A CN 2010800157239 A CN2010800157239 A CN 2010800157239A CN 201080015723 A CN201080015723 A CN 201080015723A CN 102378809 A CN102378809 A CN 102378809A
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A·英根多
U·梅尔茨
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Abstract

本发明描述了在固定式或移动式内燃机中以及在加热装置中作为加热材料和燃料的柠檬酸酯。这种推进剂和燃料具体地以如下事实为特征:它们完全燃烧而没有烟炱或带有很少的烟炱,因此与已知的化石燃料和可再生燃料如汽油、柴油、煤油、蔬菜油和生物柴油相比,它们导致显著更低的烟炱或精细灰尘的排放。柠檬酸酯可以完全从可再生的蔬菜源获得,因而是CO2中性的。

Description

作为源于生物的再生燃料和加热材料的柠檬酸酯
技术领域
本发明涉及作为燃料和加热材料或作为用于那些材料的添加剂的柠檬酸酯和/或其衍生物。
背景技术
用于发动机和加热装置的燃料和加热材料主要是碳氢化合物,它们是从化石起源的原油中获得的。化石资源的有限性是不利的,另一个缺点是与使用相关的二氧化碳的积累已被确认为全球变暖的原因。由不完全燃烧导致的烟炱和其它产品最终留在环境中,且损害人类健康和影响动植物的生活条件。
因此,为寻找源于生物的可再生资源进行了越来越多的搜索以赢得以下的燃料和加热材料:它们是二氧化碳中性的或它们可以改善燃烧并由此减少所述燃烧的有害副产品和中间产品的排放。
在这个方面已知的例子是植物油、由此生产的生物柴油(脂肪酸甲酯)、生物乙醇和生物丁醇。
发明内容
本发明的目的是发现新材料,迄今它们尚未被用作燃料或加热材料,它们可以从植物、细菌、真菌或藻类获得,或者可以主要以蔬菜原料为基础进行生产。
这个目标已经通过完全地或部分地由柠檬酸酯或柠檬酸酯衍生物组成的加热材料或燃料而得以实现。柠檬酸三乙酯或柠檬酸三丁酯是优选的。此外,各种柠檬酸酯的相互混合物也是合适的。
优选地,相应燃料的已知加热材料可以按照1-99%的比例与柠檬酸酯或柠檬酸酯衍生物混合,上述比例优选地是5-50%,更优选地是5-20%。例如通过这种方式已经发现,10%的柠檬酸酯和90%的作为柴油车的燃料的市售柴油的混合物可以实现显著减少的在一氧化碳和碳氢化合物排放方面的废气值,这是更有利的。特别是柴油、加热油、煤油、固体和液体碳氢化合物、植物和动物油以及脂肪或脂肪酸甲酯适合作为用于这种混合物的传统燃料成分。
根据另一个优选实施例,所述柠檬酸酯衍生物可以包括不含酒精基团的直链或支链的烷基或烷基基团。这种柠檬酸酯衍生物也可以根据已知的方法通过烷基化或酰基化来生产。
通过本发明可以取得以下优点:已经发现,根据本发明的燃料分别的加热材料可以在发动机或在加热装置中燃烧,与来自碳氢化合物、植物油和生物柴油的已知燃料和加热材料相比,具有显著减少的烟炱产生。所述新的燃料分别的加热材料从而可以被归类为比传统燃料显著地更清洁,使得不再需要烟炱过滤。此外,它们可以使用蔬菜原料--例如植物、细菌、真菌或藻类--通过常规技术来生产。
附图说明
具体实施方式
在下面通过例子更详细地描述发明。首先,在原则上阐述柠檬酸的生产及其酯化,这里参考现有技术。目前,柠檬酸是通过霉菌黑曲霉(黑曲霉,Aspergillus niger)的转基因变种而工业化生产的。为此,主要需要三个条件:
1.在培养液中的高葡萄糖和氧含量。
2.低的pH值(pH<3)。一方面,这会导致在柠檬酸循环中柠檬酸合成酶(citricsynthetase)的继任酶-即乌头酸酶-被抑制。如此低的pH值远远偏离酶的最佳pH值,且由于这一点,其活性显著减弱。这导致了正在形成的柠檬酸通过真菌而仅仅轻微地进一步代谢的情况。另一方面,真菌细胞的外膜变得不稳定,柠檬酸被释放到外部的培养液中。此外,在如此低的pH值处,被不希望的外部生物污染的风险是低的。
3.低的Fe2+浓度(<5mg/l,毫克/升)。由于这个原因,乌头酸酶错过了辅助因子。Fe2+离子被加入的六氰铁(III)化钾(potassiumhexacyanidoferrat(III))约束。
这种方法例如在以下文献中有描述:罗尔夫D.施密德(Rolf D.Schmid):“Taschenatlas der Biotechnologie und Gentechnik(生物技术和基因工程平装图集)”,第2版,Wiley-VCH出版社,魏因海姆(Weinheim),2006年和“Ulimanns
Figure BPA00001445922700031
der technischenChemie(化学技术化学百科全书)”,第4版,第9卷,化学出版社(publisher Chemie),魏因海姆,1975年。
柠檬酸酯可以通过柠檬酸与相应的醇的酸性酯化而获得,例如,按照根据申请人为DHW DEUSCHE HYDRIERWERKE GMBHRODLEBEN(罗达尔本德意志热水股份有限公司)的WO 03008369(公开日期2003-01-30)的方法。下文中将阐明这个方法用于柠檬酸一水合物与丁醇的酯化反应。
在酯化反应器中提供3.6mol(摩尔)丁醇,且将1摩尔柠檬酸一水合物溶解于其中。对于这一点,有利的是使用含有水的丁醇(丁醇含量为约94%至97%),这是在前面的方法中提供的。将混合物迅速升温至约100℃的温度,这时开始丁醇-水-混合物的蒸馏。柠檬酸的结晶水以及反应水连同过量的丁醇以气态的形式释放、通过分离器冷凝和引出。
为了支持所述水分离,反应混合物用少量氮气气化。此外,惰性气体可以防止接触空气中的氧气和由此引起的颜色变化。含水的丁醇(最多20%的水,随着酯化的推进,水的比例越来越小)返回到反应器中。在这个第一酯化步骤a)中,反应温度提高到125℃。经过5个小时的反应时间,反应混合物包括SZ<100mg KOH/g(毫克酸值/克),而反应速度显著减小(通过每单位时间的分离器的水相的减少来识别)。
在第二酯化阶段b)开始时,将0.5%(与无水柠檬酸相关的)甲烷嗍风酸(methane sulfon acid)作为约20%的溶液添加到丁醇中。由于这一点,将会注意到反应速度的一个显著的、但是临时的增大。在反应温度从125℃连续上升到140℃。在2小时后,第二酯化阶段终止,其中SZ<30mg KOH/g。
在第三酯化阶段c)的开始,经由分离器的丁醇循环被阻止了,且无水丁醇被剂量化。在第三酯化阶段c)中在持续三小时的反应周期的过程中的计量化速度,对于一次提供的1mol(摩尔)柠檬酸,达到最大1mol丁醇/小时。由于这种操作方法,余下的反应水从反应混合物中快速地和几乎量化地被移除,并且几乎完全转换了柠檬酸,在质量中带有相应的有利结果,以及实现了最终产品的产量。
下面描述几乎无烟炱燃烧的例子和作为柴油燃料的实际应用。
例1
通过下列的装置来研究按照上述方法或其它方法之一生产的柠檬酸三乙酯的燃烧行为。
将柠檬酸酯倒入一个金属盘中,所述金属盘的直径为12-15厘米且具有3-5厘米高的边沿,直到填充高度达到所述边沿的上边缘以下1厘米处。在金属盘的中间放入由厨房纸卷成的一根灯芯,它可以通过钉子来硬化和下沉。一旦所述灯芯吸收了柠檬酸酯,就点燃该灯芯。柠檬酸酯燃烧,带有黄色的火焰。在这样做时,已经可以光学清楚地看见,没有发生烟炱的形成。
例2
以与例1相同的方式来研究按照上述方法或其它方法之一生产的柠檬酸三丁酯酯。以克为单位的相同数量的柠檬酸三丁酯可以比乙醇酯燃烧长约20%。
在根据例1和例2燃烧柠檬酸酯时,一个白色瓷盘倾斜保持在火焰上方约5厘米处,使得燃烧产物可以碰到所述瓷盘。没有或只有很少的烟炱痕迹显示出来。
在使用生物柴油、植物油、柴油、汽油、煤油和石油的对比实验过程中,火焰已经显示清晰的黑色烟炱的形成。相应地瓷盘被黑色烟炱明显地覆盖。
应用实例
作为应用实例,已经用柠檬酸三丁酯测试运行了发动机。燃料包括市售的矿物柴油和柠檬酸三丁酯的混合物。用这种混合物的发动机测试已经在具有以下规格的发动机中进行:
类型:FLPower 178R中国公司的风冷柴油发动机
Surgetho,发动机排量为296立方厘米(0.296升),制造年份为2006年,功率5PS。采用以下的柠檬酸三丁酯和柴油的混合物以及无柴油添加剂的情况进行了7个测试运行。
所述混合物已经在一个量规上称重,倒入一个塑料容器中,并已经强烈地搅拌了至少10分钟。
为了评估废气中的烟炱形成,所述的废气被引导穿过白色纸巾(Tempo牌)5分钟,它被打开安装在离柴油发动机的排气口约10厘米的距离处。
在每一种情况下,在用新的混合物开始测试运行5分钟后和在该测试运行结束10分钟前执行所述测试。
纸巾上的烟灰残留物根据它们的颜色按照以下尺度被评估为从纯烟炱的黑色到无色。
烟炱形成的评估
0 白色,只有非常低的着色
1 明显轻的着色,但没有黑色的烟炱
2 明显强的着色,但没有黑色的烟炱
3 带有一些黑色烟炱的着色
4 由烟炱引起的弱的黑色着色
5 由烟炱引起的暗黑色着色
Figure BPA00001445922700061
*)2.5是指在2至3之间
这一点也可在图1中看到。
在所有的测试运行中柴油发动机的操作是不引人注意的。已经观察到在纯柴油和带有增大添加量的柠檬酸三丁酯的柴油之间没有差异。也不能确定作为柠檬酸三丁酯的较差燃烧的结果而引起的发动机爆震(knocking)。

Claims (8)

1.一种用于移动式或固定式内燃机或带有燃烧器的加热装置的加热材料或燃料,特征在于所述加热材料或燃料完全地或部分地由柠檬酸酯或柠檬酸酯衍生物组成。
2.根据权利要求1的加热材料或燃料,特征在于包括柠檬酸三乙酯。
3.根据权利要求1的加热材料或燃料,特征在于包括柠檬酸三丁酯。
4.根据权利要求1至3之一的加热材料或燃料,特征在于包括柠檬酸酯相互的混合物。
5.根据一个或多个前述权利要求的加热材料或燃料,特征在于已知的加热材料相应的燃料按照1-99%的混合比例被添加到柠檬酸酯或柠檬酸酯衍生物中。
6.根据权利要求5的加热材料或燃料,特征在于所述柠檬酸酯或柠檬酸酯衍生物和传统的加热材料相应的燃料的混合比例是5-50%,优选为5-20%。
7.根据权利要求5至6之一的加热材料或燃料,特征在于所述已知的加热材料/燃料包括柴油、加热油、煤油、固体和液体碳氢化合物、植物和动物油以及脂肪或脂肪酸甲酯。
8.根据权利要求1的加热材料或燃料,特征在于所述柠檬酸酯衍生物包括不含乙醇基团的直链或支链的烷基或烷基基团。
CN2010800157239A 2009-03-28 2010-03-23 作为源于生物的再生燃料和加热材料的柠檬酸酯 Pending CN102378809A (zh)

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Cited By (2)

* Cited by examiner, † Cited by third party
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CN106967464A (zh) * 2017-04-24 2017-07-21 青岛百事德工艺礼品有限公司 一种茶炉油及其制备方法
CN109777530A (zh) * 2019-01-31 2019-05-21 中实投石化科技有限公司 一种柴油发动机尾气净化液

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