CN102985663A - 基于二乙醚的柴油燃料组合物 - Google Patents
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Abstract
压缩点火燃料组合物，该组合物包含二乙醚(DEE)和水，所述二乙醚(DEE)和水的量与具有0至30重量%水含量的无水或含水乙醇(EtOH)的脱水反应产物相符，且特征进一步在于：a)对含有0至20重量%乙醇的混合物而言，按重量%计的二乙醚含量大于或等于50，且按重量%计的水含量低于或等于50减去按重量%计的乙醇浓度；或b)对含有20至30重量%乙醇的混合物而言，按重量%计的二乙醚含量大于或等于54减去0.2乘以按重量%计的乙醇浓度，且按重量%计的水含量低于或等于46减去0.8乘以按重量%计的乙醇浓度；或c)对含有30至70重量%乙醇的混合物而言，按重量%计的二乙醚含量大于或等于61.5减去0.45乘以按重量%计的乙醇浓度，且按重量%计的水含量低于或等于38.5减去0.55乘以按重量%计的乙醇浓度。
Description
本发明涉及压缩点火燃料组合物。本发明特别涉及包含各自为可用作常规标准柴油机中的燃料的量的二乙醚、乙醇和水的a 压缩点火燃料组合物。
含醚共混物已知是优异的压缩点火发动机燃料。在许多公开文献，例如美国专利Nos. 4,892,561、5,906,664和7,449,034中描述了通过醇脱水制成的低碳醚作为压缩点火燃料的用途。
WO8100721公开了基本由下列成分构成的通用液体燃料：
a) 1体积%至71体积%的一种或多种含有1至8个碳原子的伯、仲或叔一元脂族醇、苄醇或其混合物；
b) 0.5体积%至10体积%的水；
c) 1体积%至90体积%的一种或多种植物油或其混合物；和
d) 10%至80%的一种或多种醚。
在美国专利申请008244960 A中提到包含至少大约80重量%醇和大约1-10体积%醚如二甲醚或二乙醚和大约0.008-0.02体积%蒸馏或的有机油的均匀液相的燃料共混物。
美国专利No. 7722688提到由通常液体烃燃料（其包含乙醇和二乙醚）、水、无氮表面活性剂和任选具有最多大约6的pKa的酸构成的具有0.5至50重量%水含量的燃料水共混组合物。
乙醇供能的压缩点火发动机的技术利用点火增强剂（igintion enhancers），如硝酸2-乙基己酯（EHN）、聚亚烷基二醇化合物（EP403516）、具有3-10羟基5基团（3-10 hydroxyl 5 groups）和环氧乙烷和/或环氧丙烷的多元醇（WO9505437）。但是，这些化合物昂贵并还需要对发动机的重大调节。该发动机通常与常规柴油机燃料相比在大约两倍压缩下运行。
我们已经发现，包含以预定混合比共混的二乙醚、乙醇和高含量水的混合物可用作标准压缩点火发动机燃料中的燃料。这种燃料的应用不需要常规柴油供能的压缩点火发动机燃料中的重大调节。这种燃料混合物的一个特定优点在于，它们可通过无水或含水乙醇的脱水产生，从而能使乙醇用作压缩点火发动机的燃料。
根据上述发现，本发明提供压缩点火燃料组合物，该组合物包含二乙醚(DEE)和水，所述二乙醚(DEE)和水的量与具有0至30重量%水含量的无水或含水乙醇(EtOH)的脱水反应产物相符，且特征进一步在于：
a) 对含有0至20重量%乙醇的混合物而言，按重量%计的二乙醚含量大于或等于50，按重量%计的水含量低于或等于50减去按重量%计的乙醇浓度；或
b) 对含有20至30重量%乙醇的混合物而言，按重量%计的二乙醚含量大于或等于54减去0.2乘以按重量%计的乙醇浓度，且按重量%计的水含量低于或等于46减去0.8乘以按重量%计的乙醇浓度；或
c) 对含有30至70重量%乙醇的混合物而言，按重量%计的二乙醚含量大于或等于61.5减去0.45乘以按重量%计的乙醇浓度，且按重量%计的水含量低于或等于38.5减去0.55乘以按重量%计的乙醇浓度。
与具有0至30重量%水含量的无水或含水乙醇的完全转化对应的无乙醇的燃料混合物是本发明的一部分。
图1中的阴影区对应于本发明的二乙醚/乙醇/水燃料混合物的组成范围。
借助本发明，与用常规柴油燃料运行相比，可以用基于乙醇/水混合物的燃料在无点火增强剂、无乳化剂和不对发动机作出重大调节的情况下运行压缩点火发动机。
本发明的燃料混合物在使用前不需要进一步提纯，如除去水。在燃料混合物中可存在附加组分，如润滑剂、乳化剂和抗氧化剂，但不是至关重要的。
可以通过以适当量混合水、二乙醚和乙醇或通过具有0至30重量%水含量的无水或含水乙醇的脱水或通过产生本发明的燃料组合物的任何其它方法制造燃料混合物。
制造燃料的方法可包括旨在获得位于自然平衡外的二乙醚收率的步骤，如萃取、蒸馏、催化蒸馏、水或二乙醚的吸附、再循环。
本发明的一个优选实施方案包含与具有0至30重量%水含量的无水或含水乙醇的脱水反应产物相符的量的乙醇、二乙醚(DEE)和水的三元混合物，特征进一步在于乙醇含量大于或等于8重量%。这对应于图1中的区域A和B所示的燃料组成。
可通过具有0至30重量%水含量的无水或含水乙醇使用本领域中已知的酸催化剂的催化脱水制造这些燃料组合物，没有分离工艺以提高收率。在制成燃料混合物后，该产物在使用前不需要进一步提纯。这意味着在乙醇/二乙醚燃料的车上应用中，既不要求除去在乙醇转化中生成的水，也不要求通过其它方式提高二乙醚浓度。
该产物冷凝成液相可能导致该液相的相分离。因此，在燃料混合物中可存在附加组分，如乳化剂、润滑剂、抗氧化剂，但不是至关重要的。
本发明的另一优选实施方案包含与具有0至30重量%水含量的无水或含水乙醇的脱水反应产物相符的量的乙醇、二乙醚和水的混合物，特征进一步在于按重量%计的二乙醚含量高于或等于145减去4乘以按重量%计的乙醇含量。这对应于附图1中的区域B所示的燃料组成。
上述燃料组合物冷凝成液相不造成相分离。
在再一优选实施方案中，该燃料组合物含有下表1中所示的按重量%计的量的乙醇(EtOH)、水和二乙醚(DEE)。
表1
本发明的燃料在压缩点火发动机中的排放优异。无提纯下的排放已符合EU-IV标准。碳烟微粒的排放比常规柴油燃料低数个量级。氮氧化物的排放也显著降低。因此，可显著减轻或完全移除现今用在柴油供能的压缩点火发动机中的精心设计的废气清洁。
附图1是本发明的燃料混合物的组成图；
图2图示在Audi 1.9升涡轮增压柴油机中的燃料组合物试验的结果。发动机用实心符号所示的燃料组合物运行而不用空心符号所示的燃料组合物运行。标签A、B、C和D指示下列实施例8中所用的燃料组合物；和
图3显用本发明的燃料组合物运行的发动机废气中的测得颗粒排放（particle emission）。
实施例1
此实施例显示70重量%二乙醚、10重量%乙醇和20%水的燃料组合物符合具有0至30重量%水含量的无水或含水乙醇的脱水反应产物。
首先，按重量%计的二乙醚、乙醇和水的量如下换算成摩尔%：
其中指数i是指三种组分二乙醚、乙醇和水；Cmol,i和C重量,i是分别以摩尔%和重量%计的浓度，且Mi是组分的摩尔质量，二乙醚为74，乙醇为46，水为18。因此，该混合物中的70重量%二乙醚相当于
＝41.59摩尔%二乙醚。同样地，乙醇和水的摩尔浓度分别为9.56摩尔%和48.85摩尔%。
使用乙醇至醚的脱水反应的化学计量：2乙醇 =二乙醚 +水，原始无水或含水乙醇的按摩尔%计的乙醇和水含量如下给出：
（2）。
在本实施例中我们发现，乙醇浓度变成9.56+2*41.59 = 92.74摩尔%且水浓度变成48.85 – 41.59 = 7.26摩尔%。这些浓度随后如下换算成重量%：
其中指数i是指水和乙醇。无水或含水乙醇中的乙醇含量随之变成
=97.03重量%乙醇；我们还发现水含量为2.97重量%。这意味着，70重量%二乙醚、10重量%乙醇和20%水的燃料组合物相当于含有2.97重量%水的含水乙醇的脱水反应产物。这种水含量为0至30重量%。
实施例2
此实施例显示70重量%二乙醚、10重量%乙醇和20%水的燃料组合物包括在本发明中。在实施例1中显示，该组合物符合具有0至30重量%水含量的无水或含水乙醇的脱水反应产物。乙醇含量为10重量%且二乙醚含量为70%，这大于50，因此这种燃料组合物包括在本发明中。
实施例3
此实施例显示70重量%二乙醚、10重量%乙醇和20%水的燃料组合物位于图1中的区域A中。
图1中的区域A以包括在本发明中的燃料组合物为特征，其特征进一步在于
（1）乙醇含量大于或等于8重量%，和
（2）二乙醚含量小于或等于145减去4乘以按重量%计的乙醇含量 – 如果其大于或等于这种量，其位于图1中的区域B中。
乙醇含量为10重量%，其高于8重量%并因此满足条件（1）。
条件2的试验：按重量%计的二乙醚含量应低于145 – 4*10 = 105以满足这种条件。二乙醚浓度为70%，因此满足这一条件。在此要指出，所用条件仅是数学试验，其可能产生非物理浓度值（负数值或高于100%的值）。
实施例4
此实施例显示70重量%二乙醚、20重量%乙醇和10%水的燃料组合物不符合具有0至30重量%水含量的无水或含水乙醇的脱水反应产物。
上述燃料的按摩尔%计的组成根据公式（1）为48.85摩尔%二乙醚、22.45摩尔%乙醇和28.70摩尔%水。根据公式（2），发现2*48.85 + 22.45 = 120.16摩尔%乙醇和28.70 – 48.85 = -20.15摩尔%水的当量摩尔含量。根据公式（3）换算成重量%得出107.03重量%乙醇和-7.03重量%水的组成。（非物理）水含量不在0至30重量%之间，因此70重量%二乙醚、20重量%乙醇和10%水的燃料组合物不符合具有0至30重量%水含量的无水或含水乙醇的脱水反应产物。
实施例5
此实施例显示40重量%二乙醚、10重量%乙醇和50重量%水的燃料组合物不符合具有0至30重量%水含量的无水或含水乙醇的脱水反应产物。
上述燃料的按摩尔%计的组成根据公式（1）为15.29摩尔%二乙醚、6.15摩尔%乙醇和78.56摩尔%水。根据公式（2），发现2*15.29 + 6.15 = 36.73摩尔%乙醇和78.56 – 15.29 = 63.27摩尔%水的当量摩尔含量。根据公式（3）换算成重量%得出59.73重量%乙醇和40.27重量%水的组成。水含量不在0至30重量%之间，因此40重量%二乙醚、10重量%乙醇和50%水的燃料组合物不符合具有0至30重量%水含量的无水或含水乙醇的脱水反应产物。
实施例6
此实施例显示45.8重量%二乙醚、38重量%乙醇和16.2重量%水的燃料组合物位于图1中的区域B中。
上述燃料的按摩尔%计的组成根据公式（1）为26.39摩尔%二乙醚、35.23摩尔%乙醇和38.38摩尔%水。根据公式（2），发现2*26.39 + 35.23 = 88.01摩尔%乙醇和38.38 – 26.39 = 11.99摩尔%水的当量摩尔含量。根据公式（3）换算成重量%得出94.94重量%乙醇和5.06重量%水的组成。水含量在0至30重量%之间，因此这种混合物符合具有0至30重量%水含量的无水或含水乙醇的脱水反应产物。
该混合物中的乙醇含量为38重量%。为包括在本发明中，45.8重量%的二乙醚含量必须大于61.5 - 0.45 * 38 (乙醇含量) = 44.4重量%。情况如此，因此这种组合物包括在本发明中。
图1中的区域B，优选实施方案以包括在本发明中的燃料组合物为特征，其特征进一步在于
（1）乙醇含量大于或等于8重量%，
（2）二乙醚含量大于或等于145减去4乘以按重量%计的乙醇含量。
该燃料混合物中的乙醇含量为38重量%，其大于8重量%并因此满足条件1。45.8重量%的二乙醚含量大于145-4*38 = -7，因此也满足条件（2）。这意味着该燃料组合物是本发明的一个优选实施方案。
实施例7
通过混合适当量的无水二乙醚、乙醇和水获得的许多燃料混合物已用作Audi 1.9升涡轮增压柴油机的燃料。将大约2重量%二冲程油（two-stroke oil）添加到燃料中以在发动机中润滑。不添加乳化剂。图2中的实心符号代表可以用于运行发动机的燃料组合物；空心符号代表不可能用于运行发动机的燃料组合物。这表明常规Audi压缩点火发动机可以用位于图1中的线段上方的区域中的燃料组合物运行。
此实施例中不可能用于运行发动机的三种燃料组合物是31.7重量%水和68.3重量%烃燃料、21.4重量%水和78.6重量%烃燃料、和15.2重量%水和84.8重量%烃燃料。这三种组合物都位于美国专利No. 7722688中公开的本发明的燃料组合物的实施方案的界限内。这表明这些实施方案并非总是产生可用于压缩点火发动机的燃料。
实施例8
将使用本发明的燃料混合物的压缩点火发动机的性能与使用标准柴油燃料的性能进行比较。在标准Audi 1.9升涡轮增压柴油机上进行试验。通过将燃料从柴油换成如本文中公开的含有乙醇、二乙醚和水的燃料混合物，进行试验，不进一步调节发动机。该燃料混合物含有大约2重量%用于润滑的二冲程油。该燃料不含乳化剂。
表2显示使用常规柴油燃料和与图2中的点A、B、C和D对应的二乙醚、乙醇和水的四种混合物在发动机的两种不同负荷下在Audi 1.9升柴油机中的热效率以及氮氧化物（NOx）排放和颗粒排放。NOx和颗粒排放是排放规范（例如欧标）的关键参数。
表2中数据表明，使用本发明中公开的燃料混合物的发动机的功率和效率接近用常规柴油燃料获得的那些。但是，可显著降低NOx和颗粒的排放，在无废气的进一步处理下也有可能达到柴油机的排放标准。
大部分颗粒排放归因于二冲程润滑油的存在。这显示在图3中，其显示在将含有二冲程油的含28.5重量%乙醇、53.5重量%二乙醚和18.0重量%水的燃料混合物换成无二冲程油的燃料混合物的运行过程中测得的颗粒排放。在不用二冲程油运行发动机的期间，颗粒数从大约2.8 × 106/立方厘米降至大约4.5 × 105/立方厘米的水平，相当于降低84%。这表明采用如本文中公开的燃料混合物能将颗粒排放降至极低水平。
表2
Claims (5)
1.压缩点火燃料组合物，该组合物包含二乙醚(DEE)和水，所述二乙醚和水的量与具有0至30重量%水含量的无水或含水乙醇(EtOH)的脱水反应产物相符，且特征进一步在于：
a) 对含有0至20重量%乙醇的混合物而言，按重量%计的二乙醚含量大于或等于50，且按重量%计的水含量低于或等于50减去按重量%计的乙醇浓度；或
b) 对含有20至30重量%乙醇的混合物而言，按重量%计的二乙醚含量大于或等于54减去0.2乘以按重量%计的乙醇浓度，且按重量%计的水含量低于或等于46减去0.8乘以按重量%计的乙醇浓度；或
c) 对含有30至70重量%乙醇的混合物而言，按重量%计的二乙醚含量大于或等于61.5减去0.45乘以按重量%计的乙醇浓度，且按重量%计的水含量低于或等于38.5减去0.55乘以按重量%计的乙醇浓度。
2.权利要求1的压缩点火燃料，其中该乙醇含量高于或等于8重量%。
3.权利要求1或2的压缩点火燃料组合物，其中对含乙醇的混合物而言，按重量%计的二乙醚含量高于或等于145减去4乘以按重量%计的乙醇含量。
4.权利要求1的压缩点火燃料组合物，具有如下表中所示的按重量%计的组成
5.根据前述权利要求任一项的压缩点火燃料，进一步包含润滑剂、乳化剂和/或抗氧化剂。
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