CN102628635A - 带凝华脱除co2的气体膨胀天然气带压液化工艺 - Google Patents

带凝华脱除co2的气体膨胀天然气带压液化工艺 Download PDF

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CN102628635A
CN102628635A CN2012101114195A CN201210111419A CN102628635A CN 102628635 A CN102628635 A CN 102628635A CN 2012101114195 A CN2012101114195 A CN 2012101114195A CN 201210111419 A CN201210111419 A CN 201210111419A CN 102628635 A CN102628635 A CN 102628635A
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林文胜
熊晓俊
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Abstract

本发明涉及一种带凝华脱除CO2的气体膨胀天然气带压液化工艺，天然气在预冷器中保持气态被预冷，然后进入结晶器继续降温，凝华分离出固体干冰的同时CO2含量降至0.5％，紧接着进入低温压缩机加压，然后进入液化器，在较高的压力下液化后送入储罐储存。液化流程所需冷量由独立的气体膨胀制冷循环提供。与现有技术相比，本发明省去了常规天然气液化流程中占地面积很大的CO2预处理设备，可大大降低在造价高昂的海上平台进行天然气液化的投资成本。同时，天然气在较高温度下液化也降低了制冷循环的能耗。

Description

带凝华脱除CO2的气体膨胀天然气带压液化工艺
技术领域
本发明属于化工与低温技术领域，涉及天然气的净化和液化工艺，是一种在天然气液化过程中低温脱除二氧化碳的液化工艺，尤其是涉及一种在气体膨胀天然气带压液化过程中凝华脱除二氧化碳的液化工艺。
背景技术
勘探实践证明，在中国海域众多的沉积盆地中蕴藏着丰富的油气资源，目前探明的海上天然气储量约为全国天然气储量的1/3。海上天然气的开发利用不仅能够提供一种高热值的清洁能源，同时可以降低对石油资源的依赖程度，具有重要的环保和能源战略安全意义。为便于天然气的输运贸易，常将其液化。传统的天然气液化之前需进行净化处理，其中脱CO2一般要达到50～100ppm的标准，该预处理过程不仅占地面积大，而且能耗不少。
天然气带压液化技术(PLNG技术)是指在较高的压力约1～2MPa下使天然气液化得到带压的液化天然气(LNG)产品的技术。对应的液化温度约为-100～-120℃，较高的液化温度不仅减少了所需提供的冷量及所需的换热面积，降低了能耗，而且大大增加了LNG中CO2的溶解度(CO2在常压LNG中摩尔溶解度小于0.01％，而在PLNG条件下可增大到1～3％)。溶解度的增大降低了净化过程对脱除CO2的要求，对于PLNG流程来说，考虑安全余量，一般认为达到0.5％的标准即可。最初的PLNG流程主要是针对CO2含量较低的天然气提出的，然而由于CO2在PLNG中的溶解度随温度升高的增量有其限度，PLNG流程对于CO2含量高于0.5％的天然气就无能为力了，其应用因此受到极大限制。如何拓展PLNG流程对CO2含量的适用范围成为亟待解决的问题。
在各种方法中，采用凝华的方法分离脱除天然气中的CO2使其摩尔分数降至0.5％，既保留了普通PLNG流程不专设CO2预处理设备的优点，又避免了某些方法中固液两相同时出现易于引发的堵塞等问题，为CO2摩尔分数高于0.5％的天然气采用PLNG技术提供了可能。
凝华脱除天然气中CO2的技术，主要是利用CO2三相点温度较高易凝华的相变特性，结合带压液化流程提供给天然气的冷量，使得天然气中的CO2在较低的温度下凝华结霜，从而实现CO2和天然气的气固分离。为避免凝华过程中出现液化现象，必须保证天然气中CO2的结霜温度高于天然气的露点温度，为满足这个要求，在1.4～1.6MPa压力下天然气中CO2的摩尔分数不得高于30％。凝华脱除天然气中CO2的方法，一方面，可以脱除天然气中CO2的含量，使得天然气中CO2的含量达到液化流程的要求；另一方面，还可以得到固体干冰作为副产品。
气体膨胀流程利用高压制冷剂气体通过透平膨胀机绝热膨胀提供冷量实现天然气的液化，制冷剂气体在膨胀机中膨胀降温的同时，还能输出功，可用于驱动流程中的压缩机。该液化流程具有流程简单、调节灵活、工作可靠、易启动、易操作、维护方便等诸多优点。采用气体膨胀制冷循环无需设置可燃制冷剂储罐，可提高装置安全性、减少占地面积；如果采用氮气作为气体膨胀制冷循环的工质，还可进一步提高装置安全性。
已有技术中，申请号为03802427.6、名称为“通过除去可凝固固体生产液化天然气的方法和装置”的发明专利，采用由特殊材料制成的冷却器以及涡流技术连续除去天然气进料物流中的二氧化碳等可凝固组分。但是该专利中的冷却器的材料需为金属氧化物、陶瓷、单晶或者蓝宝石之一，太过特殊而昂贵，难以推广应用；且作为该专利核心的固相在容器中心而不是在壁面上形成的技术，在工程实践中很难实现。专利号为5819555、名称为“进料物流通过气固分离脱除CO2的一种方法”的美国专利，提出了相关的凝华脱除CO2的技术，但是未涉及到天然气液化工艺，且无法保证天然气在后续液化过程中不析出固体CO2。
发明内容
本发明的目的就是为减少天然气液化装置的占地面积，克服海上天然气液化装置应用受限的难题，同时降低天然气液化流程的能耗，提出了一种带凝华脱除CO2的气体膨胀天然气带压液化工艺。该工艺主要是针对CO2含量较高的天然气设计的，对于CO2摩尔分数小于0.5％的天然气，PLNG流程能够容忍全部的CO2而不析出固体，因而可以直接去掉占地很大的CO2预处理设备，为场地极为有限的海上平台实施天然气液化提供可能性。对于CO2摩尔分数大于或等于0.5％的天然气，利用CO2的凝华特性，通过带压液化过程提供的冷量将天然气中的CO2凝华脱除，采用带压液化技术液化天然气，从而实现去掉CO2预处理装置、减少占地面积的目的。
本发明的目的可以通过以下技术方案来实现：
一种带凝华脱除CO2的气体膨胀天然气带压液化工艺，该工艺主要是针对CO2含量较高的天然气设计的，对于CO2摩尔分数小于0.5％的天然气，PLNG流程能够容忍全部的CO2而不析出固体，因而可以直接去掉占地很大的CO2预处理设备，为场地极为有限的海上平台实施天然气液化提供可能性。对于CO2摩尔分数大于或等于0.5％的天然气，利用CO2的凝华特性，通过带压液化过程提供的冷量将天然气中的CO2凝华脱除，采用带压液化技术液化天然气，从而实现去掉CO2预处理装置、减少占地面积的目的。
带凝华脱除CO2的气体膨胀天然气带压液化工艺的主要特点是在天然气液化的过程中凝华脱除CO2，然后生产出带压的LNG产品，该工艺在流程上的创新设计取消了CO2预处理装置，并且保证了后续液化过程中无CO2晶体析出。
本工艺具体包括以下步骤：
1)将CO2摩尔分数在0.5％～30％之间的原料天然气引入压力调节设备，将其调压至1.4～1.6MPa；
2)将通过步骤1)调压后的天然气引入预冷器预冷降温；
3)将通过步骤2)预冷后的天然气引入结晶器降温，凝华分离出其中的固体干冰；
4)将通过步骤3)分离出CO2后的天然气引入低温压缩机加压；
5)将通过步骤4)压缩后的天然气引入液化器，吸收冷量后液化；
6)将通过步骤5)带压液化后的液化天然气产品引入储罐储存即可。
其中，步骤2)、3)、5)中天然气降温液化过程所需冷量由一套独立的气体膨胀制冷系统提供，将制冷剂气体引入压缩机加压，然后引入第一冷却器中冷却，再引入增压膨胀机组增压段增压，然后引入第二冷却器冷却，再引入预冷器预冷，然后引入增压膨胀机机组膨胀段膨胀降温，将膨胀功回收给增压膨胀机组增压段使用，再将膨胀后的气体依次通过液化器、结晶器和预冷器，为这三个设备提供冷量。
步骤1)中所述的原料天然气的压力在1.4～1.6MPa时省略步骤1)。
步骤2)中所述的天然气在在预冷器的出口温度不低于天然气中CO2的结霜温度。
步骤3)中所述的结晶器集天然气降温、CO2凝华结晶、干冰回收功能于一体，结晶器气相出口中天然气的CO2摩尔分数为0.5％。
步骤4)中所述的压缩机能承受-110℃，压缩机出口处的天然气的压力为1.8～2.2MPa，压力的升高保证了后续液化过程中无CO2晶体析出。
步骤5)中所述的液化器在1.8～2.2MPa压力下使进入其中的天然气液化。
步骤5)中得到的压力为1.8～2.2MPa的液体不经节流降压，直接作为产品引入储罐储存，液化天然气产品压力高于常规天然气液化流程。
步骤6)中所述的储罐的最低工作压力为1.8～2.2MPa。
所述的制冷剂气体选自氮气或甲烷中的一种或几种。
与现有技术相比，本发明能够省去CO2预处理设备，减少换热面积，节约设备投资，节省占地面积。通过石化行业广泛采用的HYSYS软件的模拟计算，证实本发明能大大提高天然气液化流程对CO2的容忍度，且能明显地降低液化天然气的单位能耗，并获得干冰作为副产品。占地面积的大大减小，能耗的显著降低，为海上天然气的液化提供了可能性。
附图说明
图1为带凝华脱除CO2的气体膨胀天然气带压液化流程图。
图中，1为压力调节设备、2为预冷器、3为结晶器、4为低温压缩机、5为液化器、6为储罐、7为压缩机、8为第一冷却器、9为增压膨胀机组增压段、10为第二冷却器、11为增压膨胀机组膨胀段。
具体实施方式
下面结合附图和具体实施例对本发明进行详细说明。
实施例1
一种带凝华脱除CO2的气体膨胀天然气带压液化工艺，实施方案如图1所示。气体膨胀循环制冷剂为纯甲烷，流量6.693kmol/h，原料天然气摩尔组分0.5％CO2+99.5％CH4、压力1.5MPa、温度35℃、流量1kmol/h，则带凝华脱除CO2的气体膨胀天然气带压液化工艺的具体步骤如下：
(1)由于原料天然气在1.4～1.6MPa压力范围之内，本实施例可以省略掉压力调节设备1。将原料气引入预冷器2，从制冷剂甲烷吸收冷量，流出预冷器2，温度降到-73℃；
(2)将经过步骤(1)预冷后的天然气引入结晶器3，从制冷剂甲烷吸收冷量，温度开始下降，气态天然气中的CO2开始凝华结晶析出，结晶析出的固体CO2从结晶器中分离出来作为副产品干冰。随着温度的进一步降低，更多的CO2结晶析出，残留在气态天然气中的CO2含量逐渐降低，直到达到带压液化流程允许的摩尔含量值0.5％为止，结晶器3气相出口天然气的温度降为-109℃；
(3)将经过步骤(2)凝华脱除CO2后含二氧化碳0.5％的天然气引入低温压缩机4，加压到2MPa，温度升高到-93℃；
(4)将经过步骤(3)加压后的天然气引入液化器5，从制冷剂甲烷吸收冷量进行100％液化，温度降到-107℃；
(5)将经过步骤(4)降温液化后的天然气引入储罐6；
(6)以上天然气降温液化过程所需冷量由一套独立的气体膨胀制冷系统提供。将制冷剂甲烷引入压缩机7加压到3258kPa，冷却至35℃，然后引入增压膨胀机组增压段9加压至5000kPa，冷却至35℃，然后引入预冷器2预冷至-61℃，然后引入增压膨胀机组膨胀段11膨胀至964kPa，产生的2.224kW膨胀功回收给增压膨胀机组增压段9使用，膨胀后的低温制冷剂甲烷温度降为-125℃，依次通过液化器5、结晶器3、预冷器2为天然气提供冷量，最后复温至30℃，回到压缩机7。
经过模拟计算得出，该气体膨胀天然气带压液化流程在凝华脱除CO2后的天然气完全液化时，LNG产品的单位能耗约为0.31kWh/Nm3，相较于常规气体膨胀天然气液化流程约0.50kWh/Nm3的能耗，降低了大约38％。
实施例2
一种带凝华脱除CO2的气体膨胀天然气带压液化工艺，在天然气液化的过程中凝华脱除CO2，然后生产出带压的LNG产品，该工艺在流程上的创新设计取消了CO2预处理装置，并且保证了后续液化过程中无CO2晶体析出。
气体膨胀循环制冷剂为纯甲烷，流量7.837kmol/h，原料天然气摩尔组分10％CO2+90％CH4、压力1.5MPa、温度35℃、流量1kmol/h，则带凝华脱除CO2的气体膨胀天然气带压液化工艺的具体步骤如下：
(1)由于原料天然气在1.4～1.6MPa压力范围之内，本实施例可以省略掉压力调节设备1。将原料气引入预冷器2，从制冷剂甲烷吸收冷量，流出预冷器2，温度降到-73℃；
(2)将经过步骤(1)预冷后的天然气引入结晶器3，从制冷剂甲烷吸收冷量，温度开始下降，气态天然气中的CO2开始凝华结晶析出，结晶析出的固体CO2从结晶器中分离出来作为副产品干冰。随着温度的进一步降低，更多的CO2结晶析出，残留在气态天然气中的CO2含量逐渐降低，直到达到带压液化流程允许的摩尔含量值0.5％为止，结晶器3气相出口天然气的温度降为-109℃；
(3)将经过步骤(2)凝华脱除CO2后含二氧化碳0.5％的天然气引入低温压缩机4，加压到2MPa，温度升高到-93℃；
(4)将经过步骤(3)加压后的天然气引入液化器5，从制冷剂甲烷吸收冷量进行100％液化，温度降到-107℃；
(5)将经过步骤(4)降温液化后的天然气引入储罐6；
(6)以上天然气降温液化过程所需冷量由一套独立的气体膨胀制冷系统提供。将制冷剂甲烷引入压缩机7加压到3384kPa，冷却至35℃，然后引入增压膨胀机组增压段9加压至5000kPa，冷却至35℃，然后引入预冷器2预冷至-61℃，然后引入增压膨胀机组膨胀段11膨胀至1142kPa，产生的2.361kW膨胀功回收给增压膨胀机组增压段9使用，膨胀后的低温制冷剂甲烷温度降为-121℃，依次通过液化器5、结晶器3、预冷器2为天然气提供冷量，最后复温至30C，回到压缩机7。
经过模拟计算得出，该气体膨胀天然气带压液化流程在凝华脱除CO2后的天然气完全液化时，LNG产品的单位能耗约为0.35kWh/Nm3，相较于常规气体膨胀天然气液化流程约0.50kWh/Nm3的能耗，降低了大约30％，且可得到近0.1kmol/h的固体CO2产品。
实施例3
一种带凝华脱除CO2的气体膨胀天然气带压液化工艺，该工艺主要是针对CO2含量较高的天然气设计的，对于CO2摩尔分数小于或等于0.5％的天然气，PLNG流程能够容忍全部的CO2而不析出固体，因而可以直接去掉占地很大的CO2预处理设备，为场地极为有限的海上平台实施天然气液化提供可能性。对于CO2摩尔分数大于0.5％的天然气，利用CO2的凝华特性，通过带压液化过程提供的冷量将天然气中的CO2凝华脱除，采用带压液化技术液化天然气，从而实现去掉CO2预处理装置、减少占地面积的目的。
带凝华脱除CO2的气体膨胀天然气带压液化工艺的主要特点是在天然气液化的过程中凝华脱除CO2，然后生产出带压的LNG产品，该工艺在流程上的创新设计取消了CO2预处理装置，并且保证了后续液化过程中无CO2晶体析出。
气体膨胀循环制冷剂为纯甲烷，流量7.837kmol/h，原料天然气摩尔组分30％CO2+70％CH4、压力1.5MPa、温度35℃、流量1kmol/h，则带凝华脱除CO2的气体膨胀天然气带压液化工艺的具体步骤如下：
(1)由于原料天然气在1.4～1.6MPa压力范围之内，本实施例可以省略掉压力调节设备1。将原料气引入预冷器2，从制冷剂甲烷吸收冷量，流出预冷器2，温度降到-73℃；
(2)将经过步骤(1)预冷后的天然气引入结晶器3，从制冷剂甲烷吸收冷量，温度开始下降，气态天然气中的CO2开始凝华结晶析出，结晶析出的固体CO2从结晶器中分离出来作为副产品干冰。随着温度的进一步降低，更多的CO2结晶析出，残留在气态天然气中的CO2含量逐渐降低，直到达到带压液化流程允许的摩尔含量值0.5％为止，结晶器3气相出口天然气的温度降为-109℃；
(3)将经过步骤(2)凝华脱除CO2后含二氧化碳0.5％的天然气引入低温压缩机4，加压到2MPa，温度升高到-93℃；
(4)将经过步骤(3)加压后的天然气引入液化器5，从制冷剂甲烷吸收冷量进行100％液化，温度降到-107℃；
(5)将经过步骤(4)降温液化后的天然气引入储罐6；
(6)以上天然气降温液化过程所需冷量由一套独立的气体膨胀制冷系统提供。将制冷剂甲烷引入压缩机7加压到3552kPa，冷却至35℃，然后引入增压膨胀机组增压段9加压至5000kPa，冷却至35℃，然后引入预冷器2预冷至-61℃，然后引入增压膨胀机组膨胀段11膨胀至1406kPa，产生的2.766kW膨胀功回收给增压膨胀机组增压段9使用，膨胀后的低温制冷剂甲烷温度降为-116℃，依次通过液化器5、结晶器3、预冷器2为天然气提供冷量，最后复温至30℃，回到压缩机7。
经过模拟计算得出，该气体膨胀天然气带压液化流程在凝华脱除CO2后的天然气完全液化时，LNG产品的单位能耗约为0.50kWh/Nm3，相较于常规气体膨胀天然气液化流程约0.50kWh/Nm3的能耗，能耗无增加，且可得到近0.3kmol/h的固体CO2产品。

Claims (9)

1.一种带凝华脱除CO2的气体膨胀天然气带压液化工艺，其特征在于，该工艺包括以下步骤：
1)将CO2摩尔分数在0.5％～30％之间的原料天然气引入压力调节设备(1)，将其调压至1.4～1.6MPa；
2)将通过步骤1)调压后的天然气引入预冷器(2)预冷降温；
3)将通过步骤2)预冷后的天然气引入结晶器(3)降温，凝华分离出其中的固体干冰；
4)将通过步骤3)分离出CO2后的天然气引入低温压缩机(4)加压；
5)将通过步骤4)压缩后的天然气引入液化器(5)，吸收冷量后液化；
6)将通过步骤5)带压液化后的液化天然气产品引入储罐(6)储存即可；
其中，步骤2)、3)、5)中天然气降温液化过程所需冷量由一套独立的气体膨胀制冷系统提供，将制冷剂气体引入压缩机(7)加压，然后引入第一冷却器(8)中冷却，再引入增压膨胀机组增压段(9)增压，然后引入第二冷却器(10)冷却，再引入预冷器(2)预冷，然后引入增压膨胀机机组膨胀段(11)膨胀降温，将膨胀功回收给增压膨胀机组增压段(9)使用，再将膨胀后的气体依次通过液化器(5)、结晶器(3)和预冷器(2)，为这三个设备提供冷量。
2.根据权利要求1所述的一种带凝华脱除CO2的气体膨胀天然气带压液化工艺，其特征在于，步骤1)中所述的原料天然气的压力在1.4～1.6MPa时省略步骤1)。
3.根据权利要求1所述的一种带凝华脱除CO2的气体膨胀天然气带压液化工艺，其特征在于，步骤2)中所述的天然气在在预冷器(2)的出口温度不低于天然气中CO2的结霜温度。
4.根据权利要求1所述的一种带凝华脱除CO2的气体膨胀天然气带压液化工艺，其特征在于，步骤3)中所述的结晶器(3)具有天然气降温、CO2凝华结晶、干冰回收功能，结晶器(3)气相出口中天然气的CO2摩尔分数为0.5％。
5.根据权利要求1所述的一种带凝华脱除CO2的气体膨胀天然气带压液化工艺，其特征在于，步骤4)中所述的压缩机(4)能承受-110℃低温，压缩机(4)出口处的天然气的压力为1.8～2.2MPa。
6.根据权利要求1所述的一种带凝华脱除CO2的气体膨胀天然气带压液化工艺，其特征在于，步骤5)中所述的液化器(5)在1.8～2.2MPa压力下使进入其中的天然气液化。
7.根据权利要求1所述的一种带凝华脱除CO2的气体膨胀天然气带压液化工艺，其特征在于，步骤5)中得到的压力为1.8～2.2MPa的液体不经节流降压，直接作为产品引入储罐(6)储存，液化天然气产品压力高于常规天然气液化流程。
8.根据权利要求1所述的一种带凝华脱除CO2的气体膨胀天然气带压液化工艺，其特征在于，步骤6)中所述的储罐(6)的最低工作压力为1.8～2.2MPa。
9.根据权利要求1所述的一种带凝华脱除CO2的气体膨胀天然气带压液化工艺，其特征在于，所述的制冷剂气体选自氮气或甲烷中的一种或几种。
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