CN102796561A - 生物质燃料二氧化碳循环无氧气化方法及设备 - Google Patents

生物质燃料二氧化碳循环无氧气化方法及设备 Download PDF

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CN102796561A
CN102796561A CN2012102821526A CN201210282152A CN102796561A CN 102796561 A CN102796561 A CN 102796561A CN 2012102821526 A CN2012102821526 A CN 2012102821526A CN 201210282152 A CN201210282152 A CN 201210282152A CN 102796561 A CN102796561 A CN 102796561A
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gas
links
tower
synthetic
biomass fuel
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CN102796561B (zh
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张岩丰
张亮
夏明贵
刘文焱
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Wuhan Kaidi Engineering Technology Research Institute Co Ltd
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Wuhan Kaidi Engineering Technology Research Institute Co Ltd
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Priority to CN201210282152.6A priority Critical patent/CN102796561B/zh
Publication of CN102796561A publication Critical patent/CN102796561A/zh
Priority to KR1020157003071A priority patent/KR101609809B1/ko
Priority to EP13827090.5A priority patent/EP2883940B1/en
Priority to CA2881327A priority patent/CA2881327A1/en
Priority to DK13827090.5T priority patent/DK2883940T3/en
Priority to AU2013302099A priority patent/AU2013302099B2/en
Priority to JP2015525713A priority patent/JP5965073B2/ja
Priority to RU2015108053/05A priority patent/RU2604624C2/ru
Priority to PCT/CN2013/079230 priority patent/WO2014023149A1/zh
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Priority to US14/607,020 priority patent/US9469820B2/en
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Abstract

本发明公开了一种生物质燃料二氧化碳循环无氧气化方法及设备，具体来说是一种仅利用二氧化碳作为气化剂将生物质等固体燃料气化成高品质合成气，且回收合成气自身二氧化碳气体及合成气后续利用工艺中生成的二氧化碳气体进行气化循环的整体工艺方法及设备，达到整套系统温室气体二氧化碳排放量为零的目的。该发明具有无氧耗，制取合成气品质高，冷媒气效率高，系统操作简单，且整套系统温室气体二氧化碳排放量为零等显著优点。

Description

生物质燃料二氧化碳循环无氧气化方法及设备
技术领域
本发明涉及生物质为原料的气化利用领域，具体地是指一种生物质燃料二氧化碳循环无氧气化方法及设备。
背景技术
随着公众对全球气候变暖趋势的日益关注，温室气体减排已经越来越受到世界各国的重视，如美国GE能源与环境研究公司、美国零排放联盟以及日本新能源综合开发机构等也提出了零排放能源系统的概念。
当前，解决温室气体零排放的主要工艺方法是将二氧化碳作为反应物，通过化学反应转化为含碳产品，达到零排放的目的。发明专利授权公告号：CN102060662B，一种可回收利用CO2的化工动力多联产能源系统及方法，即通过回收化工尾气中的CO2，其中一部分CO2进行有氧气化循环来制取合成气，另一部分CO2通过添加天然气进行重整反应，最终制取二甲醚或甲醇。该发明专利能回收利用CO2，但是该工艺方法需要氧气气化，因而气化过程中CO2转化量有限，其中大部分CO2需通过天然气重整反应来转化，因而具有需氧耗、需消耗天然气及工艺流程复杂的缺点。
发明内容
本发明的目的是提出一种生物质燃料二氧化碳循环无氧气化方法及设备，该发明具有燃料转化率高、无氧耗，工艺流程简单且整套系统温室气体二氧化碳排放量为零等显著优点。
为实现上述目的，本发明所提供的生物质燃料二氧化碳循环无氧气化方法，它是仅采用CO2作为气化剂将生物质燃料气化成合成气、并利用合成气生产化工油品、以实现整体无氧气化循环的工艺过程，包括如下步骤：
1）气化单元：以回收合成气自身所含的CO2和合成气后续利用生成的CO2作为气化剂，使其在外部辅助能源的作用下与生物质燃料发生剧烈的气化反应，生成主要成分为CO、CO2、CH4、H2、H2O、H2S、COS的高温合成气；
2）冷却单元：对所生成的高温合成气进行两级热交换器降温处理，其中第一级热交换器采用上述气化剂CO2作为冷却介质，用于预热气化剂CO2；第二级热交换器采用水作为冷却介质，得到副产品水蒸汽；
3）洗涤单元：对经过两级热交换降温的合成气进行旋风除尘和洗气塔洗涤处理，得到进一步降温的洁净合成气；
4）变换反应单元：使所得洁净合成气与上述副产品水蒸汽进行水煤气反应，将其中部分CO转化为H2和CO2，以调节洁净合成气的品质达到催化合成反应所需的H2/CO比值范围；
5）脱硫单元：对调质后的洁净合成气进行脱硫处理，将其中的H2S、COS脱除掉；
6）合成气脱碳单元：对脱硫后的洁净合成气进行脱碳处理，将其中的CO2分离出来；
7）催化合成单元：使脱硫脱碳后的洁净合成气通过催化变换反应合成化工油品，同时生成富含CO2的尾气；
8）尾气脱碳单元：对所生成的尾气进行脱碳处理，将其中的CO2分离出来，剩余无温室气体直接或处理后对外排放；
9）气化剂循环单元：将步骤6）和步骤8）所分离出来的CO2重新作为步骤2）中第一级热交换器的冷却介质，经过对高温合成气换热降温，获得预热的气化剂CO2，再利用它进行步骤1）中的气化反应，如此循环最终实现整套工艺零温室气体排放。
作为优选方案，所述步骤1）中，气化反应的温度为600~1300℃，高温合成气出口温度为700~1100℃；所述步骤1）中，气化反应的温度为850~1250℃，高温合成气出口温度为850~1100℃。
进一步地，所述步骤1）中，外部辅助能源为等离子炬能、微波能、太阳能、激光能或电感应能中的一种或几种的组合，所述外部辅助能源占单位时间入炉原料总能量的10~30%。
更进一步地，所述步骤1）中，外部辅助能源占单位时间入炉原料总能量的15~20%。
进一步地，所述步骤1）中，气化剂CO2的用量与单位标态下产气量的比值为0.36~0.51；所述步骤1）中，生物质燃料的粒径为50mm以下，气化剂CO2的喷口流速为30~60m/s；所述步骤2）中，通过第一级热交换器将气化剂CO2预热至350~600℃。
作为又一种优选方案，所述步骤4）中，调节洁净合成气成分至H2/CO为2:1。
为实现上述方法而设计的生物质燃料二氧化碳循环无氧气化设备，包括气化炉、余热换热器、余热锅炉、旋风除尘器、洗气塔、变换反应塔、脱硫塔、合成气脱碳塔、催化合成塔和尾气脱碳塔，其特殊之处在于：
所述气化炉的合成气出口与余热换热器的热介质输入端相连，所述余热换热器的热介质输出端与余热锅炉的热源输入端相连，所述余热锅炉的热源输出端与旋风除尘器的进气端相连，所述旋风除尘器的出气端与洗气塔的进口相连，所述洗气塔的出口通过压缩机与变换反应塔的进气口相连，所述余热锅炉的蒸汽输出端与变换反应塔的蒸汽入口相连；
所述变换反应塔的出气口与脱硫塔的输入端相连，所述脱硫塔的输出端与合成气脱碳塔的输入口相连，所述合成气脱碳塔的输出口与催化合成塔的原料进口相连，所述催化合成塔的副产物出口与尾气脱碳塔的尾气进口相连，所述尾气脱碳塔和合成气脱碳塔的CO2出口同时与余热换热器的冷介质输入端相连，所述余热换热器的冷介质输出端与气化炉的气化剂进口相连。
作为优选方案，所述尾气脱碳塔和合成气脱碳塔的CO2出口同时与气柜的进口相连，所述气柜的出口通过鼓风机与余热换热器的冷介质输入端相连。
进一步地，所述气柜的进口还与启动煅烧炉的CO2输出口相连。
更进一步地，所述气化炉的内腔下部设置有布风板，所述布风板下方的炉壁上设置有主气化剂进口，所述布风板上方的炉壁上设置有辅气化剂进口，所述辅气化剂进口上方的炉壁上设置有外部辅助能量入口，所述余热换热器的冷介质输出端分为两路，一路与主气化剂进口相连，另一路与辅气化剂进口相连。
本发明的优点在于：
其一，采用二氧化碳气体作为整套系统循环工质，具有整套工艺系统零温室气体排放、零氧耗的优点。
其二，充分结合生物质燃料自身特性，气化单元仅采用二氧化碳作为气化剂，无氧气化，既补充了碳源又减少燃料燃烧份额，单位燃料转化率高、有效气体含量高。
其三，对原料粒径无特殊要求，只需简单破碎，无需复杂处理，经济性好。
其四，采用外部热源提供辅助热能，能充分结合各种形式能源，能实现能源综合利用。
附图说明
图1是本发明的生物质燃料二氧化碳循环无氧气化设备的连接结构示意图。
图2是图1中气化炉的结构示意图。
图3是图2中的A—A剖视结构示意图。
图中：气化炉1，余热换热器2，余热锅炉3，旋风除尘器4，洗气塔5，压缩机6，变换反应塔7，脱硫塔8，合成气脱碳塔9，催化合成塔10，尾气脱碳塔11，气柜12，鼓风机13，燃料14，外部辅助能量入口15，辅气化剂进口16，给料入口17，合成气出口18，布风板19，主气化剂进口20，排渣口21，给料装置22，冷渣器23，蒸汽24，冷渣25，飞灰26，合成油品27，合成尾气28，CO2气体29，合成气30，排放气31，启动煅烧炉32，石灰石33。
具体实施方式
以下结合附图和具体实施例对本发明作进一步地的详细描述。
图中所示的生物质燃料二氧化碳循环无氧气化设备，主要由气化炉1、余热换热器2、余热锅炉3、旋风除尘器4、洗气塔5、变换反应塔7、脱硫塔8、合成气脱碳塔9、催化合成塔10和尾气脱碳塔11等组成。气化炉1的顶部设有合成气出口18，气化炉1的底部设有排渣口21，气化炉的中部外壁上设有给料入口17，给料入口17与给料装置22相连。气化炉1的内腔下部设置有布风板19，布风板19下方的炉壁上设置有主气化剂进口20，布风板19上方的炉壁上设置有辅气化剂进口16，辅气化剂进口16上方的炉壁上设置有外部辅助能量入口15。
气化炉1的合成气出口18与余热换热器2的热介质输入端相连，余热换热器2的热介质输出端与余热锅炉3的热源输入端相连，余热锅炉3的热源输出端与旋风除尘器4的进气端相连，旋风除尘器4的出气端与洗气塔5的进口相连，洗气塔5的出口通过压缩机6与变换反应塔7的进气口相连，余热锅炉3的蒸汽输出端与变换反应塔7的蒸汽入口相连。
变换反应塔7的出气口与脱硫塔8的输入端相连，脱硫塔8的输出端与合成气脱碳塔9的输入口相连，合成气脱碳塔9的输出口与催化合成塔10的原料进口相连，催化合成塔10的副产物出口与尾气脱碳塔11的尾气进口相连，尾气脱碳塔11和合成气脱碳塔9的CO2出口同时与余热换热器2的冷介质输入端相连，余热换热器2的冷介质输出端分为两路，一路与主气化剂进口20相连，另一路与辅气化剂进口16相连。
尾气脱碳塔11和合成气脱碳塔9的CO2出口同时与气柜12的进口相连，气柜12的出口通过鼓风机13与余热换热器2的冷介质输入端相连；气柜12的进口还与启动煅烧炉32的CO2输出口相连。
本发明中，生物质等固体燃料14首先通过给料装置22由给料口17送入气化炉1内，循环的气化剂CO2通过鼓风机13鼓入，气化剂CO2分为两路，一路通过主气化剂进口20引入，经过布风板19进入气化炉1中；另一路通过辅气化剂进口16进入气化炉1中，同时，通过外部辅助能量入口15引入热能，在炉内进行高温反应，最初进行热解气化，主要裂解生成CO、CO2、CH4、H2及半焦，由于炉内反应温度控制在600~1600℃，高温下主要由半焦物质与CO2气体进行气化反应，且气化反应速率快，主要反应为C+CO2=2CO+Q。
以生物质稻壳测试，以1Nm3合成气为基准，辅助能源量为入口燃料总能的15~25%，反应温度800℃，需循环CO2量为0.51Nm3需生物质量0.48kg，出口合成气体积成份为：CO：50~55%、CO2：22~28%、H2：6~12%。
高温合成气30由气化炉1的合成气出口18引出，而燃料冷渣25由排渣口21排出，经冷渣器23后排至渣场。
其中，气化炉反应区温度控制在600~1300℃，而850~1250℃为其最佳温度。合成气出口温度控制在800~1100℃范围内。气化单元中给料载气、工艺吹扫用气均利用循环的CO2气体。外部输入能源占处理原料能量的15~30%。外部能源型式除采用等离子火炬外，也包含微波能、太阳能、激光能、电感应能等其他可转换为热能的能源型式。气化剂CO2循环量可依据炉温、燃料情况适当调节。气化炉内气化剂布风板喷口流速可依据燃料粒径合理控制，较佳实例为粒径在50mm以下范围，风速为30~60m/s。气化炉启动运行时，采用启动煅烧炉32，利用外热煅烧石灰石33，来制取高纯CO2气体作为启动用气。为了使本工艺达到最佳工作效果，满足工艺整体性能要求，设计中关键是控制床层温度，实时调节等离子功率及二氧化碳供给量。通过对合成气出口监测单元来达到对上述关键因素的控制，也能实现连锁控制，进行全自动化操作，提高运行稳定性。
高温合成气30随后进入余热换热器2中，与作为气化剂的CO2气体29进行换热，起到预热气化剂的作用，提高了气化炉转化效率。一级降温后的高温合成气然后进入余热锅炉3中继续降温，并副产水蒸汽24，两级降温后合成气再经过旋风除尘器4、洗气塔5进一步对合成气降温除尘，分离下来的飞灰26经收集后排至渣场，其中预热CO2温度为350~600℃。
冷却洗涤后的合成气随后通过压缩机6升压，升压后进入变换塔7，在变换塔7内对合成气进行调质处理，主要反应为水煤气反应，其中水蒸汽24来源于余热锅炉3，这样达到整体工艺物质合理利用的目的。
调质后的合成气随后进入脱硫塔8、合成气脱碳塔9进行脱硫脱碳净化处理。从合成气脱碳塔9引出的洁净合成气随后进入催化合成塔10，从合成气脱碳塔9分离的CO2气体29依靠余压输送至气柜12。
合成气进入催化合成塔10中，通过合成反应将合成气合成化工油品27，同时也伴随生成合成尾气28。
合成尾气28随后送入尾气脱碳塔11中，在塔内分离出CO2气体29，剩余无温室气体的排放气31处理后对外排放，如此实现整体工艺零温室气体的排放。
合成气脱碳塔9与尾气脱碳塔11分离出的CO2气体29一起进入气柜12，通过鼓风机13后输送至气化炉1的主气化剂进口20及辅气化剂进口16处，如此进行气化循环。

Claims (13)

1.一种生物质燃料二氧化碳循环无氧气化方法，它是仅采用CO2作为气化剂将生物质燃料气化成合成气、并利用合成气生产化工油品、以实现整体无氧气化循环的工艺过程，包括如下步骤：
1）气化单元：以回收合成气自身所含的CO2和合成气后续利用生成的CO2作为气化剂，使其在外部辅助能源的作用下与生物质燃料发生剧烈的气化反应，生成主要成分为CO、CO2、CH4、H2、H2O、H2S、COS的高温合成气；
2）冷却单元：对所生成的高温合成气进行两级热交换器降温处理，其中第一级热交换器采用上述气化剂CO2作为冷却介质，用于预热气化剂CO2；第二级热交换器采用水作为冷却介质，得到副产品水蒸汽；
3）洗涤单元：对经过两级热交换降温的合成气进行旋风除尘和洗气塔洗涤处理，得到进一步降温的洁净合成气；
4）变换反应单元：使所得洁净合成气与上述副产品水蒸汽进行水煤气反应，将其中部分CO转化为H2和CO2，以调节洁净合成气的品质达到催化合成反应所需的H2/CO比值范围；
5）脱硫单元：对调质后的洁净合成气进行脱硫处理，将其中的H2S、COS脱除掉；
6）合成气脱碳单元：对脱硫后的洁净合成气进行脱碳处理，将其中的CO2分离出来；
7）催化合成单元：使脱硫脱碳后的洁净合成气通过催化变换反应合成化工油品，同时生成富含CO2的尾气；
8）尾气脱碳单元：对所生成的尾气进行脱碳处理，将其中的CO2分离出来，剩余无温室气体直接或处理后对外排放；
9）气化剂循环单元：将步骤6）和步骤8）所分离出来的CO2重新作为步骤2）中第一级热交换器的冷却介质，经过对高温合成气换热降温，获得预热的气化剂CO2，再利用它进行步骤1）中的气化反应，如此循环最终实现整套工艺零温室气体排放。
2.根据权利要求1所述的生物质燃料二氧化碳循环无氧气化方法，其特征在于：所述步骤1）中，气化反应的温度为600~1300℃，高温合成气出口温度为700~1100℃。
3.根据权利要求1所述的生物质燃料二氧化碳循环无氧气化方法，其特征在于：所述步骤1）中，气化反应的温度为850~1250℃，高温合成气出口温度为850~1100℃。
4.根据权利要求1或2或3所述的生物质燃料二氧化碳循环无氧气化方法，其特征在于：所述步骤1）中，外部辅助能源为等离子炬能、微波能、太阳能、激光能或电感应能中的一种或几种的组合，所述外部辅助能源占单位时间入炉原料总能量的10~30%。
5.根据权利要求4所述的生物质燃料二氧化碳循环无氧气化方法，其特征在于：所述步骤1）中，外部辅助能源占单位时间入炉原料总能量的15~20%。
6.根据权利要求1或2或3所述的生物质燃料二氧化碳循环无氧气化方法，其特征在于：所述步骤1）中，气化剂CO2的用量与单位标态下产气量的比值为0.36~0.51。
7.根据权利要求1或2或3所述的生物质燃料二氧化碳循环无氧气化方法，其特征在于：所述步骤1）中，生物质燃料的粒径为50mm以下，气化剂CO2的喷口流速为30~60m/s。
8.根据权利要求1或2或3所述的生物质燃料二氧化碳循环无氧气化方法，其特征在于：所述步骤2）中，通过第一级热交换器将气化剂CO2预热至350~600℃。
9.根据权利要求1所述的生物质燃料二氧化碳循环无氧气化方法，其特征在于：所述步骤4）中，用以调节洁净合成气成分至H2/CO为2:1。
10.一种为实现权利要求1所述方法而设计的生物质燃料二氧化碳循环无氧气化设备，包括气化炉（1）、余热换热器（2）、余热锅炉（3）、旋风除尘器（4）、洗气塔（5）、变换反应塔（7）、脱硫塔（8）、合成气脱碳塔（9）、催化合成塔（10）和尾气脱碳塔（11），其特征在于：
所述气化炉（1）的合成气出口（18）与余热换热器（2）的热介质输入端相连，所述余热换热器（2）的热介质输出端与余热锅炉（3）的热源输入端相连，所述余热锅炉（3）的热源输出端与旋风除尘器（4）的进气端相连，所述旋风除尘器（4）的出气端与洗气塔（5）的进口相连，所述洗气塔（5）的出口通过压缩机（6）与变换反应塔（7）的进气口相连，所述余热锅炉（3）的蒸汽输出端与变换反应塔（7）的蒸汽入口相连；
所述变换反应塔（7）的出气口与脱硫塔（8）的输入端相连，所述脱硫塔（8）的输出端与合成气脱碳塔（9）的输入口相连，所述合成气脱碳塔（9）的输出口与催化合成塔（10）的原料进口相连，所述催化合成塔（10）的副产物出口与尾气脱碳塔（11）的尾气进口相连，所述尾气脱碳塔（11）和合成气脱碳塔（9）的CO2出口同时与余热换热器（2）的冷介质输入端相连，所述余热换热器（2）的冷介质输出端与气化炉（1）的气化剂进口相连。
11.根据权利要求10所述的生物质燃料二氧化碳循环无氧气化系统，其特征在于：所述尾气脱碳塔（11）和合成气脱碳塔（9）的CO2出口同时与气柜（12）的进口相连，所述气柜（12）的出口通过鼓风机（13）与余热换热器（2）的冷介质输入端相连。
12.根据权利要求11所述的生物质燃料二氧化碳循环无氧气化系统，其特征在于：所述气柜（12）的进口还与启动煅烧炉（32）的CO2输出口相连。
13.根据权利要求10或11或12所述的生物质燃料二氧化碳循环无氧气化系统，其特征在于：所述气化炉（1）的内腔下部设置有布风板（19），所述布风板（19）下方的炉壁上设置有主气化剂进口（20），所述布风板（19）上方的炉壁上设置有辅气化剂进口（16），所述辅气化剂进口（16）上方的炉壁上设置有外部辅助能量入口（15），所述余热换热器（2）的冷介质输出端分为两路，一路与主气化剂进口（20）相连，另一路与辅气化剂进口（16）相连。
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