CN113631690B - 生产改善的柴油燃料的方法 - Google Patents

生产改善的柴油燃料的方法 Download PDF

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CN113631690B
CN113631690B CN202080024109.2A CN202080024109A CN113631690B CN 113631690 B CN113631690 B CN 113631690B CN 202080024109 A CN202080024109 A CN 202080024109A CN 113631690 B CN113631690 B CN 113631690B
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diesel fuel
pressure
petroleum derived
producing
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CN113631690A (zh
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塞尔希奥·安东尼奥·特雷维尼奥·金塔尼利亚
吉列尔莫·热拉尔多·罗达特·埃雷拉
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Ji LieermoRelaerduoLuodateAileila
Sai ErxiaoAndongniaoTeleiweiniaoJintaniliya
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Ji LieermoRelaerduoLuodateAileila
Sai ErxiaoAndongniaoTeleiweiniaoJintaniliya
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Abstract

一种用于连续生产改善的柴油燃料的方法，该燃料具有改善的点火特性，更具体而言具有更高的导电性、更高的十六烷值和增加的润滑性以及具有更高的完全燃烧百分比，致使在内燃柴油机中同时发生颗粒生成减少和NOx减少，打破这两种污染物从内燃柴油机排放的权衡。

Description

生产改善的柴油燃料的方法
技术领域
本发明涉及用于内燃机的烃燃料升级(upgrading)的系统和方法，并且更具体而言涉及用于连续生产改善的柴油燃料的方法，该改善的柴油燃料具有增强的点火特性，更具体而言具有更大电导率和/或润滑性，允许更大百分比的完全燃烧，从而在功率损失可忽略不计的内燃机柴油发动机中燃烧时，同时致使更少的烟尘产生和氮氧化物(NOx)减少。
背景技术
柴油燃料是世界上使用最广泛的液态烃燃料之一。内燃机使用柴油的主要问题；无论是重型还是轻型，无论是道路发动机还是非道路发动机，都需要在固体碳颗粒(烟尘)和氮氧化物(NOx)排放之间进行权衡。如果需要排放较少的烟尘，可以提高发动机燃烧室的温度，而使其燃烧得更好。烟尘排放量会下降，但燃烧室会产生更多氧化剂，这意味着NOx排放量会显著增加。如果降低燃烧室的温度，则会出现相反的效果，NOx排放量会下降，但烟尘形成会更高。
现有技术示出了解决上述问题的一些努力。
例如，PCT专利公开号WO 2014168889 A1(文献D1)公开了一种通过燃料与添加剂或燃料增强剂的分子断裂和重组进行燃料裂解和优化的方法，包括：预热燃料；将所述预热燃料与水和至少一种添加剂混合直至形成微乳液混合物；使所述混合物通过泵直至达到所需压力；和将所述混合物引导至流体动力学空化反应器，在该反应器中形成空化气泡并发生解聚和新聚合物链的形成，从而提供改性燃料。D1声称所公开的方法：使用不昂贵的添加剂提高燃料体积；改进API指标；产生“更清洁”的燃料；减少燃料中有害要素，如：燃烧时的硫、CO、Ox和碳颗粒以及原油粘度；改进热值；提高D6和D2燃料中的十六烷值；能够增加较轻燃料中的辛烷值；和由于更清洁的燃烧过程，减少相关的系统维护。
然而，文献D1中公开的方法有几个不足，例如：
·D1没有充分和清楚地描述“空化”是什么意思，因为它仅将其描述为气泡发生装置，然而，D1没有提及实现他们所寻找的效果的理想工艺条件。对于空化反应器的作用，也没有在技术上进行合理解释。
·D1没有描述所添加的添加剂或燃料改善剂，它们只提到了一系列纯物质，如水、甲醇等。这些物质不是添加剂，因为它们不会给燃料添加任何特性。
·D1提及了柴油的分子断裂和解聚以及随后的再聚合。首先，柴油不含聚合物分子，无论如何，柴油不是聚合物。也不希望破坏分子，因为这会失去其热值。所有这些技术论点都基于错误的假设，即柴油是聚合物或包含聚合物分子。任何了解碳氢化合物的人都不会认为这种语义是充分的，论点也不是有效的。
·D1中描述的所有好处都没有明确的目的，它们似乎是在改性所述燃料而“改进”燃烧，但它们并没有解释“改进”的含义。
·D1提到所述改性燃料“允许”产生更少的CO、NOx和SO2排放。减少CO没有多大意义，因为现代发动机目前不产生这种气体。NOx的减少是相关的，但D1没有证明这种效果，也没有解释实现这种效果的意义。SO2排放的减少也是不准确的，因为这种排放取决于燃料中硫的浓度。没有能够对柴油进行改性或分子分解，从而产生停止硫氧化物产生的效果。只有分离所述燃料并产生另一硫的料流，才能降低硫浓度。另一个不精确之处是发动机很少产生SO2，SO3的排放是更为常见的。此外，D1揭示的降低百分比也缺乏证明其合理性的逻辑解释。
PCT专利公开号WO 2015053649(文献D2)描述了旨在制备用于内燃机和锅炉中燃烧的各种含水燃料混合物以及用于从水中去除石油和石油产品的微米粒子和纳米粒子的空化反应器。D2公开了如果在空化场(cavitation field)中进行灌注水-油混合物的高强度水力机械处理(空化过程)，则它们会变成油水乳液形式的替代燃料类型，其中水会进入精细分散的相，这在微观层面上会对液体燃料的燃烧(无论是在一滴量级上还是在火炬中的液滴群燃烧过程中均会)产生积极影响。
D2公开了广为人知的燃料乳液的生产。D2公开的乳液中的水浓度非常高(超过8％)，这在燃烧像D2中描述的燃料油的燃料时会产生众所周知的效果。
美国专利申请No.20160046878(文献D3)公开了用于升级或改进重油原料质量的系统和方法。D3中描述的系统和方法利用空化能，如超声空化能，将超声或其他空化能(例如，空化力、剪切力、微射流、冲击波、微对流、局部热点等)传递至重油中而在通常认为不适合处理重油的低压氢条件(例如，小于500psig)下驱动加氢转化。
D3公开了对重质原油的改性，但没有带来任何明确的改善。它只是提到他们通过利用空化而改善了重质原油。它不关注燃烧。另一方面，D2将流体动力空化与超声混淆。它们却是不同的现象。
世界上也有很多科学努力去解决这个问题，但都没有成功，因为许多能够不增加NOx而减少烟尘的技术基本上将燃料的热功率降低了20％左右，并且它们还使燃料在许多参数上超出规格。它们在技术上是绝对不可行的。
鉴于上述问题和需要，申请人开发了一种用于连续生产改善的柴油燃料的方法，该改善的柴油燃料具有增强的点火特性，更具体而言具有更大的导电性和增强的润滑性，允许更大百分比的完全燃烧。
本发明的方法包括将柴油燃料与两种特定添加剂混合并均质化，并将所述混合均质化的混合物在具有转子的振荡动力反应器(shock power reactor)内进行受控空化(cavitation)，以获得改善的双极性柴油燃料。在内燃机中使用该改善的柴油燃料，允许减少总氮氧化物(NOx)排放以及减少超过30％的总烟尘和总P.M.排放量。该改善的柴油燃料打破了柴油内燃机中NOx和烟尘产生的权衡，燃料耗损(fuel penalty)仅为0％-3％。
发明内容
因此，本发明的主要目的是提供一种用于连续生产改善的柴油燃料的方法，该改善的柴油燃料具有增强的点火特性，更具体而言具有更大的导电性和增强的润滑性，这允许更大百分比的完全燃烧，致使烟尘生成减少且同时NOx降低。
本发明还有的一个主要目的是提供一种连续生产上述性质的改善的柴油燃料的方法，该方法包括将柴油燃料与两种特定添加剂混合并均质化，并将所述混合均质化的混合物在具有转子的振荡动力反应器内进行受控空化，以获得改善的双极性柴油燃料。
本发明还有的一个附加目的是提供一种连续生产上述性质的改善的柴油燃料的方法，其中所述改善的柴油燃料在用于内燃机中时允许减少总氮氧化物(NOx)排放以及减少超过30％的总烟尘和总P.M.排放。
本发明的另一个主要目的是提供一种连续生产上述性质的改善的柴油燃料的方法，其中所述改善的柴油燃料打破柴油燃烧发动机中NOx和烟尘生成的权衡，燃料耗损仅为0-3％。
本发明的连续生产改善的柴油燃料的方法的这些和其他目的和优点根据以下对本发明实施方式参照附图进行的详细描述对本领域普通技术人员而言将变得显而易见。
附图说明
图1是本发明连续生产改善的柴油燃料的方法的流程图。
图2是显示测试1的稳态试验结果的图。
图3是显示测试1的瞬态试验结果的图。
图4是显示测试2的第一稳态试验的图。
图5是显示测试2的第二稳态试验的图。
图6是显示测试2的瞬态试验的图。
具体实施方式
本发明的改善的柴油燃料基于添加两种组分混合物的“常规”商用柴油。这些组分将被称为“S1”(对应于添加剂编号1)和“S2”(对应于添加剂编号2)。
“S1”包含能够用6-80摩尔范围内的环氧乙烷进行乙氧基化的乙氧基化脂肪酸酯。该分子由1,4-脱水山梨糖醇和脂肪酸形成(参见式1)。通常而言，这种物质由山梨糖醇的硬脂酸酯和棕榈酸酯及其单酐和二酐的混合物组成。这种乙氧基化衍生物也能够通过几摩尔环氧乙烷加成为单甘油酯的形式而制备，并且根据所加成的环氧乙烷的摩尔数，具有宽范围的HLB值。
式1：S1的示意结构，其中“R”代表脂肪酸(月桂酸、棕榈酸、油酸或硬脂酸)。
S2是一种复杂的水基(water based)混合物，由具有一个或两个甲基基团的芳族溶剂如对“p-”或邻“o-”二甲苯与余量的四种可以是烷基型链或者也可以是壬基型链的乙氧基苯酚衍生的表面活性剂(见式2)混合而形成。表面活性剂的化学余量应配制为匹配S1的HLB值。
式2：这种表面活性剂之一的实例(4-(2,4-二甲基庚烷-3-基)苯酚)
关于S2的水浓度应处于50％-90％范围内，并且水以胺皂的形式加入。胺皂应在化学反应器中制备，其中叔胺和具有三个醇基团的三醇都是粘性有机化合物(见下图)，将会被具有一个双键和6-18个碳的烷基链的脂族脂肪酸中和。
S1是非极性物质，而S2是双极性混合物。这两种物质都会与柴油或超低柴油燃料形成复杂的分子分散体。
两种添加剂都注入主工艺流程，并通过振荡波动力反应器(SPR)充分混合。
现在将根据设计用于处理连续柴油料流的具体实施方式描述本发明的方法，其中本发明的方法包括以下步骤：
a)通过具有40HP电机以及35-350加仑/min的最大流量和60-100psig的工作压力的螺旋齿轮泵(BPS 002)，在60-100psig的压力下提供(非极性)商用柴油燃料(也可以使用超低硫柴油(ULSD))的连续主料流(SD)。在环境温度和罐的流体静压(最小为1psi)下，泵以4-1400L/min的范围从恒定体积流体源(罐ULSD)接收柴油。主料流(SD)流经4″管道，但根据整个工艺过程的规模，也可以使用其他具有不同直径的管道；
b)通过4英寸“V形”Coriolis质量流量计测量主料流(SD)的流量，并通过主料流控制阀NPS 4英寸150级标准RF法兰连接件调节主料流。主流量在20-90psig的压力下进行调节，即与所述螺旋齿轮泵提供的压力相同；
c)通过渐进式腔注射泵(螺杆泵，progressive cavity injection pump)(BPS002)提供S1组分料流，该泵具有5HP电机，具有0-5加仑/min(优选4.55加仑/min)的最大比例流量和25-120psig(优选100psig)的工作压力，该工作压力必须大于主料流(SD)的压力。渐进式腔注射泵在环境温度下以罐的流体静压从罐接收S1组分；
d)通过1英寸直管式Coriolis质量流量计测量S1组分的料流，用控制阀NPS 3/4英寸进行调节，该控制阀以25-125psig的最大压力(优选100psig)调节S1组分的料流。
e)通过位于主料流控制阀之后的位置处的标准“T”型连接器以25-125psig(优选100psig)的压力(必须大于主料流压力)将S1化合物料流注入主料流(SD)4”管道，以产生最大质量流量为35-400加仑/min(优选359.55加仑/min)的SD+S1料流，其中输入质量流量对应于0.9％-1.5％的SD流量。
f)通过长约120cm、直径约4英寸并带有5个PMS叶片单元和150级标准RF法兰连接件的第一静态混合器(MEZC 001)混合并均质化SD+S1料流，并产生约8psig的压降以产生约20-110psig(优选67psig)的SD+S1混合料流；
g)通过渐进式腔注射泵(BPS 003)提供S2组分料流，该泵具有3HP电机，具有最大流量0-10加仑/min(优选8.75加仑/min)和工作压力25-125psig(优选100psig)。渐进式腔注射泵在环境温度下以罐的流体静压从该罐接收S2组分；
h)通过3/4英寸直管式Coriolis质量流量计测量S2组分料流，通过控制阀NPS 3/4英寸150级标准RF法兰连接件进行调节，其以25-125psig(优选100psig)的压力调节S2料流。
i)通过标准“T”连接器在第一静态混合器之后的位置处以25-125psig(优选100psig)的压力(必须高于主料流压力)将S2组分料流注入到4”管道的SD+S1料流中，以400加仑/min的最大质量流量产生SD+S1+S2料流，其中S2组分的输入质量流对应于大约1.5％-3.0％的SD+S1+S2流量。
j)通过第二静态混合器(MEZC 002)混合并均质化SD+S1+S2料流，该静态混合器长约87cm，直径约4英寸，带有3个PMS叶片单元和150级标准RF法兰连接件，并产生约4psig的压降，由此产生在环境温度下具有25-125psig(优选约63psig)压力的SD+S1+S2混合料流；
k)在环境温度下将具有压力为25-125psig(优选约63psig)的SD+S1+S2料流进料于振荡波动力反应器(SPR)中以将所述料流进行“受控空化”，这将非极性柴油燃料转化为双极性柴油燃料，使润滑性参数提高超过40％。该SPR反应器包括以600RPM-3000RPM的速度旋转的转子。该旋转动作在远离金属表面的转子腔中产生流体动力空化。该空化作用是受控的，因此没有损坏。随着微观空化气泡的产生和塌缩，振荡波释放到能够加热和/或混合的液体中(Hydrodynamics,2018)。该设备保证SD+S1+S2料流的均匀混合，并且结果得到具有约30℃-80℃的温度的改善的柴油燃料，这对应于约30℃的温度升高。
在本发明的方法的其他实施方式中，在步骤e)和i)中，组分S1总是以高于或略高于主料流(SD)压力的压力注入，而组分S2总是以大于或略大于SD+S1料流压力的压力注入。
尽管描述了该方法设计用于处理连续柴油料流，但它也可以以间歇方式处理柴油。
通过本发明的方法生产的改善的柴油燃料具有增强的点火特性，更具体而言与常规柴油燃料相比具有超过1000倍的更大电导率，并且与常规柴油燃料相比具有超过100％的润滑度值(value of lubricity)，具有更高的完全燃烧百分比，致使在内燃柴油机中烟尘产生减少同时NOx降低。
通过本发明的方法获得的所述改善的柴油燃料是具有约0.300mm润滑度参数的双极性柴油燃料。
该改善的柴油燃料已在基于EPA和CARB标准循环的发动机上进行了验证试验，该燃料基于常规ULSD的效果是减少超过30％的总烟尘和总P.M.排放，以及总氮氧化物(NOx)排放。该改善的柴油(ND)打破了柴油内燃机中NOx和烟尘产生的权衡，且燃料耗损仅为0-3％。
该改善的柴油燃料有别于基础燃料的特性在于，在显微镜下观察，可以观察到极性颗粒的分散体，这就是它具有双极性特性的原因。
如前所述，还能够看到相对于基础燃料的电导率增加了超过1000倍，而无需加入添加剂。这根据ASTM D2624进行测量。
ASTM D6079测得的润滑度高得多，而无需添加润滑添加剂。
本发明的改善的柴油的规格
工艺数据
流入流量
流入流量(GPM) 350
S1相对于流入流量(％) 0.012
S2相对于流入流量(％) 0.02
分子量
密度
物质平衡
粘度
Conv L/G 0.264172
使用本发明的改善的柴油的发动机试验
发动机的试验方法是由环保局(Environmental protection agency)(英文缩写EPA)管理和认可的联邦试验协议(Federal Test Protocol)(英文缩写FTP)。试验在稳态(Steady State)和瞬态(Transient)循环下运行。
试验1
Navistar
·车型年份：2016N13
·排放合规：2010
·排量，升：12.4
·额定功率：1700转/分时475hp
·尾气再循环(英文缩写EGR)
·高压共轨燃料系统(英文缩写HPCR)
代表美国和欧洲当前生产的基础发动机
稳态试验
·1700rpm和50％负载
·使用下一代燃料减少33％的烟尘
参考图2的图
瞬态试验
·FTP试验证明：
√减少烟尘14％
√减少NOx 8.6％
参考图3的图
试验2
DD系列60
·车型年份：1998系列60
·排放合规：1998
·排量，升：14.0
·额定功率：1800rpm时450hp
·无废气再循环(EGR)
·无后处理
·单位喷油器
传统车队库存的代表
稳态试验1
·1800rpm和25％负载
·使用下一代燃料减少烟尘34％
·NOx和燃料消耗量不变
参考图4的图
稳态试验2
·1200rpm和100％负载
·使用下一代燃料减少烟尘26％
·NOx和燃料消耗不变
参考图5的图
瞬态试验
·FTP试验证明：
·NOx和燃料消耗不变
·烟尘减少29％
参考图6的图
CHEVRON PHILLIPS生产的未经处理的常规柴油的分析
/>
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批号：19FPDST01
SOUTHWEST RESEARCH INSTITUTE开展的本发明改善的柴油(下一代柴油)分析
(*不能发动。样品已经浑浊)
下一代柴油-#1
通过荧光指示剂吸附法的ASTM D1319烃类型
饱和烃含量，体积％ 67.1
芳烃含量，体积％ 30.5
烯烃含量，体积％ 2.4
D6079高频往复机
石油产品在大气压下的ASTM D86蒸馏
下一代柴油-#2
通过荧光指示剂吸附法的ASTM D1319烃类型
饱和烃含量，体积％ 69.8
芳烃含量，体积％ 28.6
烯烃含量，体积％ 1.6
D6079高频往复机
石油产品环境压力下的蒸馏
/>

Claims (11)

1.一种生产石油衍生柴油燃料的方法，包括以下步骤：
a）混合和均质化以下料流：由石油衍生柴油燃料组成的第一料流（SD）；第一添加剂的第二料流（S1），所述第一添加剂包含用环氧乙烷进行乙氧基化的乙氧基化脂肪酸酯，其中所述脂肪酸酯由1,4-脱水山梨糖醇和脂肪酸形成，所加成的环氧乙烷的摩尔数为6-80；包含第二添加剂的第三料流（S2），所述第二添加剂包含含有以下各项的混合物的水性乳液：具有一个或两个甲基基团的芳族溶剂、4-(2,4-二甲基庚烷-3-基)苯酚以及胺皂，所述胺皂通过以下化合物与具有一个双键和6-18个碳的烷基链的脂族脂肪酸反应得到：
，
从而产生包含SD+S1+S2的混合均质化的料流；和
b）通过在具有转子的振荡动力反应器内使混合均质化的混合物进行受控空化，将步骤a）中获得的所述混合均质化的料流中所含的柴油燃料转化为双极性石油衍生柴油燃料，以获得所述石油衍生柴油燃料，
其中S2组分的输入质量流量对应于SD+S1+S2流体的1.5-3.0%，以及
其中在步骤b）中，SD+S1+S2的所述混合均质化的料流以25-125 psig的压力且在环境温度下进料至振荡波动力反应器，所述振荡波动力反应器包括以600 RPM-3000 RPM的速度旋转的转子。
2.根据权利要求1所述的生产石油衍生柴油燃料的方法，其中在步骤a）中，所述第一料流（SD）包含通过螺旋齿轮泵在60-100 psig的压力下泵送的非极性石油衍生柴油（CD），所述螺旋齿轮泵具有40 HP的电机且流量为35-350加仑/min，并且工作压力为60-100 psig，其中所述泵在环境温度和罐的流体静压下以4-1400 L/min的范围从恒定体积流体源接收所述石油衍生柴油，以及其中所述第一料流通过Coriolis质量流量计测量，并且通过主流量控制阀NPS 150级标准RF法兰连接件在20-90 psig的压力下进行调节。
3.根据权利要求1所述的生产石油衍生柴油燃料的方法，其中在步骤a）中，所述第二料流（S1）通过渐进式腔注射泵提供，所述渐进式腔注射泵的比例流量为0-5加仑/min，且工作压力为25-120 psig，其中所述渐进式腔注射泵在环境温度下在罐的流体静压下从罐接收所述第一添加剂，以及其中由所述渐进式腔注射泵提供的所述第二料流通过直管式Coriolis质量流量计进行测量，用控制阀进行调节，所述控制阀以25-125 psig的压力调节所述第二料流。
4.根据权利要求1所述的生产石油衍生柴油燃料的方法，其中在步骤a）中，所述第三料流（S2）通过渐进式腔注射泵提供，所述渐进式腔注射泵的流量为0-10加仑/min，并且工作压力为25-125 psig，其中所述渐进式腔注射泵在环境温度下在罐的流体静压下从罐接收所述第二添加剂，以及其中由所述渐进式腔注射泵提供的所述第三料流通过直管式Coriolis质量流量计进行测量，通过控制阀NPS 150级标准RF法兰连接件进行调节，所述控制阀以25-125 psig的压力调节S2添加剂的所述第三料流。
5.根据权利要求1所述的生产石油衍生柴油燃料的方法，其中在步骤a）中：
I. 将所述第二料流（S1）注入所述第一料流（SD）；
II. 所得料流（SD+S1）通过静态混合器均质化，从而产生均质化料流；
III. 将所述第三料流S2注入步骤II中获得的所述均质化料流；
IV. 将步骤III中所获得的料流（SD+S1+S2）通过静态混合器均质化。
6.根据权利要求5所述的生产石油衍生柴油燃料的方法，其中在步骤I中，所述第二料流（S1）通过标准“T”型连接器在25-125 psig的压力下注入，所述压力必须大于主料流的压力，从而产生具有35-400加仑/min的质量流量的SD+S1料流，其中输入质量流量对应于第一料流SD的0.9-1.5%。
7.根据权利要求5所述的生产石油衍生柴油燃料的方法，其中在步骤II中，所得料流（SD+S1）通过具有5个PMS叶片单元和150级标准RF法兰连接件且产生8 psig的压降的第一静态混合器均质化，以产生20-110 psig的SD+S1混合料流。
8.根据权利要求5所述的生产石油衍生柴油燃料的方法，其中在步骤III中，所述第三料流S2通过位于第一静态混合器之后的位置处的标准“T”型连接器以25-125 psig的压力注入，所述压力必须大于所述第一料流（SD）的压力，从而产生最大质量流量为400加仑/min的SD+S1+S2料流。
9.根据权利要求5所述的生产石油衍生柴油燃料的方法，其中在步骤III中，包含SD+S1+S2的料流通过具有3个PMS叶片单元和150级标准RF法兰连接件且产生4 psig压降的第二静态混合器进行均质化和混合，由此产生在环境温度下具有25-125 psig的压力的SD+S1+S2混合料流。
10.一种通过权利要求1-9中任一项所述的方法生产的石油衍生柴油燃料，其中所述石油衍生柴油燃料是双极性石油衍生柴油燃料，具有相比于常规柴油燃料的电导率超过1000倍的电导率，0.300 mm的润滑度参数，大于0的芳烃含量，以及其中所述石油衍生柴油燃料在被柴油内燃机燃烧时使烟尘产生降低超过30%且降低NOx产生，并且燃料耗损仅为0-3%。
11.根据权利要求10所述的石油衍生柴油燃料，其中所述芳烃含量处于28.6体积%至30.5体积%的范围内。
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