CN1047790C - 用低热值固体燃料生产用于产生电能的燃气的气化方法 - Google Patents

用低热值固体燃料生产用于产生电能的燃气的气化方法 Download PDF

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CN1047790C
CN1047790C CN94190559A CN94190559A CN1047790C CN 1047790 C CN1047790 C CN 1047790C CN 94190559 A CN94190559 A CN 94190559A CN 94190559 A CN94190559 A CN 94190559A CN 1047790 C CN1047790 C CN 1047790C
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G·N·瓦克纳斯
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Abstract

一种新颖的利用低热值固体燃料产生电能的方法，它在二个串联的压力反应器中操作，第一个是流化床型，是生成硫化氢的还原方法。第二个压力反应器是固定床反应器，在此直接用氧或氧-蒸汽气化碳的残余物，硫被氧化成二氧化硫。二种气态物流通过克劳斯反应中和，在600℃-800℃和20-30atm下生成燃气，在外部轮机中使用该燃气产生电能和压力蒸汽。

Description

用低热值固体燃料生产用于产生电能的燃气的气化方法
本发明公开了一种低热值固体燃料如褐煤、泥煤分两步进行热解和用氧气或氧气—蒸汽气化的新颖的气化方法。另外还公开了一种在改进的燃气轮机与蒸汽动力联合系统(Co—Gas advancedsystem)中用产生的气体产生大量电能并在操作运转中没有环境污染的新方法。
由于在保证足够量的电能量方面存在危机，并因为在石油的供给和价格方面不正常，所以，生产电能的国家计划宁愿优先发展当地的能源。在该优选的开发计划中，煤是首先被考虑的主要的资源，因为煤是生产电能中要用第一燃料，并且在世界上煤比油的资源丰富，而且分布更均匀。煤资源可分为低热值和高热值的；也可根据它们的含硫量划分。燃烧固体燃料，所含的硫变成二氧化硫，从而毒害环境造成污染，由于这些问题，因此只限于使用含硫量低的固体燃料，并使其对环境的破坏尽可能小。
在使用煤产生电能时观察到，通过煤的燃烧，产生电能的效果很差，同时释放出大量的二氧化硫、飞灰和氧化氮，并对设备产生严重属蚀。
另外，燃烧固体燃料所产生的大量二氧化碳今天被认为是主要的污染因素，是在我们星球上形成“温室效应”的主要原因。使用低热值固体燃料如褐煤和泥煤，所有这些环境的和生产的问题显得更为严重。
对于这些问题，现有的解决办法是降低这些低热值燃料的含硫量并中和燃气。
然而这些解决办法费用很高，并且由于价格问题，使得所提供的解决办法没有吸引力。现在，一种有吸引力的比较好的方法似乎是气化这些低热值燃料，尽管这样可能使能量的损失较大。在完全气化的情况下，可以洗涤煤气，使其与毒气和飞灰分离，但在完全气化的情况下，热值进一步降低到65—70％，并且在操作中需要昂贵的工业装置。
但是，与此同时，随着在电力生产中燃气轮机的发展，可以有利用气体的更经济的解决办法，我们的新颖解决办法是这样一种方法，该方法利用改进的燃气轮机与蒸汽动力联合系统中产生的燃气，用该方法，通过使用燃气轮机和联合系统，增加产生的电能的量。然而为了运行燃气轮机，我们要求燃气无腐蚀性，没有焦油和液体副产物，但具有尽可能高的热能。
考虑到这些进展，在公开的本发明中，已研究了低热值褐煤和泥煤的技术特征，并发现这些固体燃料或它们本身或在除灰之后(在另一发明中)都在这一改进系统中能高效运转来产生电能，这是因为这些燃料高度(40—85％)热解、高度放热，而没有形成焦油和液体副产物。这些低热值燃料热解的最佳条件为400—600℃，热解处理时大量放热。回收的热解残余物的炭纯度很高，热值为4000—6000Kcal/kg，而无灰或在有灰情况下为2200—4000kcal/kg。在公开的本发明中，研究了用氧气，选优用氧气—蒸汽气化炭残余物，并发现产生的燃气具有极高的热值并在900—1000℃回收。该气化实现了炭的完全利用。按照本发明方法，即褐煤和泥煤二步气化达到了很高的高热效率，氧化气化不会生成焦油或液体副产物。
本发明发现，热解处理在600℃发生放热，产生350—600Kcal/kg热量，并且放出的热量与热解的程度有关。燃气的热含量和底灰与氧化气化中生产的燃气的热交换增加了能量。
如图1所示，引入固体燃料可采用的额外加热装置。即，也研究了没有使用碳热能也能达到热解处理的热平衡的条件。这导致极大地节省能量以及充分利用低热值固体燃料的热能。
本发明发现气化及热解处理的二步气化和完全气化(用氧或用氧—蒸汽)，有利于生产不同化学性质的产品，其中热解是一种还原处理，其中，硫被气化成硫化氢，而氧化气化处理是化学性质的氧化，且硫被氧化成二氧化硫。然后，研究并拟订出解决办法，通过创造条件将燃气送入克劳斯(Claus)反应器内中和这些含硫气体。在第一次在轮机系统中利用它们的热机能量之后，在600℃、30atm混合这些燃料物流并把它们送入克劳斯催化反应器，含硫气体释放出产物硫。
这种中和含硫气体有利于简单生产有价值硫的可能性是本发明新颖性和重要性的关键，因为它可满足第一个目的，即该R&D所包括的情况，这样可开发一种方法，该方法是用低热值固体燃料生产电能，而不会产生来自二氧化硫和飞灰的毒性污染问题，可以高纯度收集生成的硫，并且还有少量的生成的硫被气流携带，在气流中用水洗涤并收集它们。
本发明的另一创造性是在热解处理期间产生了30atm压力，并在此压力得到燃气，并在气化处理和克劳斯装置两步处理中达到工作压力。在温度为600—900℃，压力为30atm得到该燃气，其没有腐蚀物和含硫气体。
本发明的另一基本的创造性证明是低热值固体燃料(褐煤和泥煤)的放热热解，这是因为这样的有机质中存在一定量的氧，这如同木材一样。众所周知，木材和木质有机质在高于400℃时会放热热解，过去的木材蒸馏处理和近期的废有机质的热解处理都有利地利用了它们。低热值固体燃料(褐煤和泥煤)具有下列木质稠度(woody consistency)。
表1褐煤和泥煤的稠度
组分          褐煤         泥煤
PH           5.8—6.9    4.6—5.4
灰           15—35      6—20.5
蜡质物等     5.2—6.8    8.1—8.3
腐黑酸       20—33.8    18—34.1
腐黑酸物     30—40      37—42.1
全纤维素     31—35      26.1—32.9
d—纤维素    8—15       10.5—12.0
具有以上的性质，就决定了热解趋势的性质和用氧或氧—蒸汽气化的结果，形成的系统有利于在热交换和最后结果中的热平衡。热操作参数的确定如下：
a.  用来自废气、底灰等的废弃热能来加热固体燃料以进行热解处理。
b.  热解气化是放热的，生成250—600Kcal/kg热能，形成高达30atm 的操作压力，其不受水分或灰的影响，所以该热解气化是先进的并且是还原反应。
c.  中和含硫气本的克劳斯反应在600℃燃气温度、30atm燃气压力、H2S/SO2摩尔比2∶1下是自发产生的，反应是定量的。
d.  使用该方法的装置应在30atm压力下，高达900℃燃气温度下操作。
固体燃料如褐煤或泥煤、无论是它们本身或在除灰处理后，将它们以粉料形式干燥，首先机械脱水，然后用在1000℃回收的灰的热能及废气的热能进行热交换，以使最后回收的废气温度降至180—300℃，来加热固体燃料到180—300℃。
用在180—300℃的固体燃料如褐煤开始热解处理，当要热解时，需温度450—600℃。用如下热源达到上述温度：a)与在1000℃回收的氧化气体(冷却到600℃)热交换，可提供200℃给热解物质；b)利用放热热解反应生成的热能，它能将温度升高200—300℃，用这些热能使热解处理达到600℃或更高。如果需要，在褐煤进料处设置加热装置来补偿热解处理的能量，然而这很大程度取决于热解和氧化气化处理的相对程度。
用氧或优选氧气—蒸汽气化时，加入600℃的、高炭纯度且为多孔状的炭质热解残余物，它们非常剧烈地进行反应，使所含的炭进行定量转化并快速提高温度到900—1000℃。在氧化处理中的热能损失比较低，小于12％，这指的是总量的50％。实际热能损耗在6％以下，对于整个气化处理这是很低的，并得到高能量效益。
一种来自于热解、一种来自于氧气或氧气—蒸汽气化的二种气流，在回收它们时或在轮机中能量交换利用之后混合。然后进入在压力下操作的克劳斯装置。在克劳斯装置内，中和含硫气体，并回收没有腐蚀气体的燃料气流。
分析用儿种希腊产褐煤和泥煤在进行热解和氧气气化的二个反应器中产生的气体，在下表2中给出其最大和最小组成。
表2
热解和氧气气化的气体燃料组成
热解，％         氧气气化，％甲烷    20—35一氧化碳30—35     一氧化碳    35—40二氧化碳2—6       二氧化碳    16—22氢      16—22     氢          40—60硫化氢  1—3       二氧化硫    1—2
几种低热值固体燃料热解反应过程得到的结果列于表3。
表3低热值褐煤和泥煤的热解反应，以％计(无灰，干燥)
温   度 泥煤    Ptolemais(北希腊)     Megalopolis(Peloponessus)希腊     Aliveri(Euboea)希腊
    400℃450℃500℃550℃600℃650℃灰含量固体燃料的Kcal/kg煤残余物的-Kca1/kg     15.2％22.434.2434.4844.0044.6311.55％4,4004,465      17.3％23.535.2839.4344.2446.610.8％5,1005,200       35.4％44.352.467.4275.4279.3820.6％4,4004,020     16.8％23.437.244.6451.0056.0011.5％5,4005,730
本发明工艺流程图示出利用产生的气体产生电能的流程，显而易见，具有创造性并可获得能量收益。
生产工序由二个压力反应器组成，一个是热解反应器，一个是用氧气气化的反应器。热解反应器设计操作压力为50atm，操作温度为700℃，是流化床型，采用自动加煤和排出得到的产品(炭质残余物和燃气)的系统。
气化反应器设计操作温度高达1200℃，压力高达50atm，是固定床型，设有自动进料和引入氧气并释放出灰和生成气的系统。
应用本发明的另一可能性是热解处理和在现有的生产压力蒸汽的锅炉内燃烧炭质残余物相结合。
按照这种方案，把固体燃料如褐煤和泥煤引入热解反应器内，含至多60％的水或是干状的，或是半干状的，生成的燃气送入轮机以利用它们的热机能量，然后洗涤，并用公知的方法如与Stretford方法相结合来中和存在的硫化氢。之后，燃烧该燃气，在改进的联合系统中生成大量电能。在这种情况下，在现有锅炉中燃烧炭质残余物以生产压力蒸汽，用来运转现有的蒸汽轮机或新的装置。按照该方法，电能产量大约是现有技术得到电能的三倍以上，而脱硫达到固体燃料中存在的硫总量的70％。
在本发明描述的系统中，具有创造性并被实践证明，热解处理不受存在的灰的水分的影响，而且，这种处理将能量转换形式、能量利用生成的产物、气体和炭质残余物表现出来，并且生成的蒸汽实际上明显增加了气体的体积和它们的能量。除了通过生物精制(biorefining)而使固体燃料达到最佳利用外，放热反应明显地增加了能量并作为热源。
将从反应器出来的燃气混合，并进入轮机，释放出部分热机能量作为电能，然后引入克劳斯反应装置内。在克劳斯装置内，气体应有400—450℃的温度和工作压力。热机能量也可通过热交换用于产生蒸汽。
在最后，燃气含有的热能达到生物精制使用的最初固体燃料热能的95％，并且还有放热反应的能量。
将燃气送入改进的联合循环系统中，用于产生电能。按照本发明，与轮机一起，对热机能量利用可超过65％。
目前，电能的产率是1.1Kg 300Kcal褐煤每KWh，或用热含量800—1200Kcal/Kg的褐煤和泥煤，其生产率是1.8—4.1Kg/KW电能。按照本发明，电的生产能力给人的印象是很深刻的，达到0.41—0.62Kg褐煤或泥煤/KWh，因为根据褐煤和泥煤在干燥状态时的能量含量利用低热值的褐煤和泥煤，并另外通过适度放热反应的影响又可增加能量20—30％。从上述结论看出，本发明在使用具有30—80％的热解趋势的低热值固体燃料方面，提高了电能生产产率，它与高热值固体燃料及油相当，并且在操作中完全没有污染。
因此，本发明介绍一种用地球上分布很广的低热值固体燃料低成本产生电能的方法，并且在操作时产生大量的电能，但没有引入飞灰、SO2污染，并且也可以使其没有氧化氮，这就完全消除了污染。也使得每生产单元CO2的释放降低75％。

Claims (14)

1.  一种利用低热值固体燃料生产用于产生电能的燃气的气化方法，其特征在于该方法包括：
a)在450℃-600℃的温度下将所述固体燃料热解，将这些燃料炭质部分的40-80％热解，从而形成第一种气体和炭质残余物，
b)在氧或氧-蒸汽的存在下加热该炭质残余物将炭质残余物气化，其中该气化反应是用干燥的、高纯度和高表面活性的600℃的物料进行的；或者燃烧该炭质残余物。
2.  根据权利要求1的方法，其中，所述固体燃料是褐煤或泥煤。
3.  根据权利要求1的方法，其中，所述固体燃料经还原反应热解，在第一种气体中形成硫化氢，并且炭质残余物经氧化反应气化，形成含有二氧化硫的第二种气体，并且在该方法还包括在下述克劳斯反应有效操作条件下混合该第一种气体和第二种气体，使硫化氢和二氧化硫中和，定量地形成分子硫：
4.  根据权利要求3的方法，其中，第一种气体和第二种气体的混合物被送入轮机或蒸汽机中，以产生电能或压力蒸汽。
5.  根据权利要求1的方法，其中，在步骤(b)中的炭质残余物被燃烧用于生产蒸汽。
6.  根据权利要求1的方法，其中，所述固体燃料含有至多60％的湿分，并且步骤(a)中的热解处理有效地将该固体燃料脱水。
7.  根据权利要求1的方法，其中，达到所述热解处理温度所需的热能，由放热反应给出200-300℃的能量，通过与气化气体热交换可给出200℃的温升，还有引入180-320℃的固体燃料所含的热能。
8.  根据权利要求3的方法，其中，所述固体燃料呈粉末形式，并且在步骤(a)之前通过与废气或底灰进行热交换被加热至180-320℃的温度，同时脱水60％-90％。
9.  根据权利要求3的方法，其中，步骤(b)中的气化只消耗6％的炭质，并且操作气体保持的总热量为所述固体燃料的热量的90％。
10.  根据权利要求3的方法，其中，在600℃-900℃的温度和20-30atm的压力下产生第一种气体和第二种气体的混合物，并且该方法还包括将该混合物加入到轮机中，用以产生电能。
11.  根据权利要求3的方法，其中，将第一种气体和第二种气体的混合物用水进行洗涤，然后加入到联合循环装置中，产生超过该气体混合物的热含量的电能。
12.  根据权利要求3的方法，其中，所述第一种气体包含：
甲烷        20％-32％
一氧化碳    30％-50％
二氧化碳    2％-6％
硫化氢      2％-3％。
13.  根据权利要求3的方法，其中，所述第二种气体包含：
一氧化碳    35％-40％
二氧化碳    16％-22％
氢气        40％-60％
二氧化硫    1％-2％。
14.  根据权利要求12或13的方法，其中，所述混合物在联合循环装置中用作燃料，产生相当于得到的所述固体燃料的热值的55％-65％的电能。
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SK13295A3 (en) 1995-07-11
HU9500331D0 (en) 1995-03-28
HUT71882A (en) 1996-02-28
CN1113086A (zh) 1995-12-06
EP0654072B1 (en) 2001-09-12
YU48699B (sh) 1999-07-28
AU6805094A (en) 1995-01-03
DE69428250D1 (de) 2001-10-18
PL307331A1 (en) 1995-05-15
GR1001615B (el) 1994-07-29
BG62889B1 (bg) 2000-10-31
US5626638A (en) 1997-05-06
RU95106490A (ru) 1996-11-20
CA2141682A1 (en) 1994-12-22
YU48694A (sh) 1997-05-28
EP0654072A1 (en) 1995-05-24
PL178845B1 (pl) 2000-06-30
DE69428250T2 (de) 2002-06-27
RU2128683C1 (ru) 1999-04-10
BG99390A (bg) 1996-01-31
WO1994029410A1 (en) 1994-12-22

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