CN105617830B - 城乡有机废弃物发酵净化提纯生产车用生物氢烷气的方法 - Google Patents
城乡有机废弃物发酵净化提纯生产车用生物氢烷气的方法 Download PDFInfo
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Abstract
本发明涉及生物质废弃物利用技术，旨在提供城乡有机废弃物发酵净化提纯生产车用生物氢烷气的方法。该方法包括步骤：将城乡有机废弃物发酵成的混合气体收集储存，增压后进行脱硫，冷却后再增压，然后进行脱水脱碳，再冷却压缩脱水后，即得到H2和CH4总浓度高于95％的车用生物氢烷气。本发明针对城乡有机废弃物发酵制备的混合气体进行脱硫脱水脱碳提纯，能得到H2和CH4总浓度高于95％的车用生物氢烷气，H2S浓度低于15mg/m3，高位发热量大于31.415MJ/m3，达到车用压缩天然气的国家标准，能够替代石化天然气应用于天然气汽车，具有显著的经济环境和社会效益。
Description
技术领域
本发明是关于生物质废弃物利用技术领域，特别涉及城乡有机废弃物发酵净化提纯生产车用生物氢烷气的方法。
背景技术
氢气具有能量密度高、燃烧产物只有水、对环境无污染、方便储存运输等优点，故是一种理想清洁的无碳新能源。最近几年来，世界范围内以氢气为原料的燃料电池以及氢燃电动汽车的迅猛发展加速了“氢能经济”的进程，故氢能的制备、储存和利用技术开发已成为世界各国实现可持续发展的战略必争领域。我国政府大力支持氢能技术开发，在国家中长期科技发展纲要的前沿技术领域中，开发高效低成本的可再生能源制氢技术是重点支持的先进能源技术之一。利用生物质废弃物发酵制取氢气新能源是国内外的前沿研究热点和高技术竞争焦点。将生物质发酵得到的氢气和甲烷按照一定比例配制成生物氢烷气，具有比纯天然气更优异的节能减排效果。由于氢气的点火能量低(不需要高能点火系统)、燃烧速度高(大约是天然气的8倍)、稀薄燃烧极限低(淬熄距离只有天然气的30％)等突出优势，故汽车发动机燃用生物氢烷气比纯天然气的热效率提高约2-3％，降低CO和HC等污染物排放约400-600ppm。由于发动机热效率提高，故一辆出租车燃用生物氢烷气比燃用天然气的燃料费用降低约10％，通过节能减排取得显著的经济环境和社会效益。
目前对城乡有机废弃物发酵制氢的研究较为活跃，Okamoto利用碳水化合物、蛋白质和脂类作为产氢原料进行研究，结果表明碳水化合物是最佳产氢原料；Lay的研究结果指出，生活有机垃圾的总固体(TS)产氢能力为140～180mL/g；Fang以大米浆为原料的研究结果表明，最佳产氢pH值为4.5，底物浓度5.5g/L，挥发性气体(VS)氢气产率为346mL/g，相当于理论产率的62.6％；Shin以餐厨垃圾为原料比较了中温和高温厌氧发酵制氢，结果表明，由于在高温条件抑制了甲烷和丙酸的生成，它的氢气产率比中温条件下高；Han研究了餐厨垃圾的渗滤床反应器发酵制氢，当稀释率为4.5d-1时具有最佳产氢性能。曹先艳考察了氨氮对餐厨垃圾厌氧发酵产氢的影响，结果指出，在一定浓度范围内，对产氢有促进作用，当氨氮浓度为6.24g/L时，得到最大的氢VS气产率126.8mL/g，当氨氮浓度大于7.89g/L时，对产氢有抑制作用。但是厌氧发酵产氢总是伴随着中间产物的生成，包括醇类和挥发性有机酸(VFA)，这一生化机理决定了厌氧发酵制氢不能完全回收有机质中的能量，限制了该技术的工业应用。因此，可利用厌氧发酵联产氢气和甲烷的方式来提高能源回收率：在产氢阶段，产氢细菌发酵生活有机垃圾生成氢气和中间代谢产物(醇类和VFA)；在产甲烷阶段，产甲烷细菌利用中间产物以及产氢阶段未被降解的残余物进一步生成甲烷。但是对于发酵联产氢气和甲烷后的混合气体净化提纯和脱碳压缩生产车用生物氢烷气的技术方法还很少文献报道。
发明内容
本发明的主要目的在于克服现有技术中的不足，提供一种利用城乡有机废弃物发酵净化提纯生产车用生物氢烷气的方法。为解决上述技术问题，本发明的解决方案是：
提供城乡有机废弃物发酵净化提纯生产车用生物氢烷气的方法，具体包括下述步骤：
(1)将城乡有机废弃物发酵成的混合气体收集储存(混合气压力为1～3kPa、温度为18～20℃)后，将混合气体经鼓风机增压至20～40kPa；
(2)利用膜式湿法脱硫反应器对增压后的混合气体进行脱硫，膜式湿法脱硫反应器中装填有中空纤维膜，将混合气体以流量320～400m3/h通入中空纤维膜内侧由上而下流动，并将质量浓度为25～35％的混合醇胺溶液通入中空纤维膜外侧，通过逆向流动脱除混合气体中的H2S；
(3)将脱硫后的混合气体冷却后，增压到0.8～1.0Mpa，再经固体分子筛(沸石型硅酸铝盐)吸附脱除混合气体中的H2O；
(4)将脱除水分后的混合气体以流量32～50m3/h自下而上通入脱碳吸收塔，与质量浓度为30％的复合胺基吸收剂逆向流动反应，然后将脱除CO2提纯后的混合气体由脱碳吸收塔的塔顶引出，再冷却至20～40℃；
(5)将经过步骤(4)处理后的混合气体压缩到20MPa，经固体分子筛(沸石型硅酸铝盐)吸附脱除水分后，即得到H2和CH4总浓度高于95％的车用生物氢烷气。
在本发明中，所述城乡有机废弃物发酵制备的混合气体，含有的成分为：5～21％的H2、35～63％的CH4、30～50％的CO2、0.2～1％的H2S、0.2～1％的H2O；各成分的浓度为体积浓度。
在本发明中，所述步骤(2)中使用的膜式湿法脱硫反应器，装填的中空纤维膜为聚丙烯中空纤维膜，膜内径为0.4mm，孔隙率为60％，平均孔径为0.01～0.1μm。
在本发明中，所述步骤(2)中，混合醇胺溶液是溶质为乙醇胺和甲基二乙醇胺，溶剂为水的混合溶液，其中，乙醇胺的质量浓度为10～15％，甲基二乙醇胺的质量浓度15～20％(水的质量浓度为65～75％)。
在本发明中，所述步骤(2)中，使用后的混合醇胺溶液经过在温度110～120℃条件下加热使CO2气体完全脱附进行再生处理后，能重新进入膜式湿法脱硫反应器进行利用。
在本发明中，所述步骤(4)中，复合胺基吸收剂是溶质为乙醇胺、N甲基二乙醇胺和哌嗪，溶剂为水的混合溶液，其中，乙醇胺、N甲基二乙醇胺和哌嗪的摩尔比为1:1:0.6。
在本发明中，所述步骤(4)中，使用后的复合胺基吸收剂经过在温度110～120℃条件下加热使CO2气体完全脱附进行再生处理后，能重新进入脱碳吸收塔进行利用。
与现有技术相比，本发明的有益效果是：
本发明的方法针对城乡有机废弃物发酵制备的混合气体(含有的成分为：5～21％的H2、35～63％的CH4、30～50％的CO2、0.2～1％的H2S、0.2～1％的H2O；各成分的浓度为体积浓度)进行脱硫脱水脱碳提纯，使发酵混合气体中CO2脱除效率高达95～99％，净化提纯后气体产物中的CO2体积浓度低于3％，复合胺基吸收剂的再生能耗比传统乙醇胺降低10％。净化提纯后能得到H2和CH4总浓度高于95％的车用生物氢烷气，H2S浓度低于15mg/m3，高位发热量大于31.415MJ/m3，达到车用压缩天然气的国家标准(GB18047-2000)，能够替代石化天然气应用于天然气汽车，具有显著的经济环境和社会效益。
附图说明
图1为本发明的方法流程图。
具体实施方式
下面结合附图与具体实施方式对本发明作进一步详细描述：
下面的实施例可以使本专业的专业技术人员更全面地理解本发明，但不以任何方式限制本发明。
实施例1
将城乡有机废弃物发酵制备的混合气体(各成分体积浓度为：5％的H2、63％的CH4、30％的CO2、1％的H2S以及1％的H2O)收集储存，混合气压力为1kPa、温度为18℃。将混合气体经鼓风机增压至20kPa，送往膜式湿法脱硫反应器。脱硫反应器装填有聚丙烯中空纤维膜(膜内径0.4mm，孔隙率60％，平均孔径0.01～0.1μm)。混合气体以流量400m3/h通入中空纤维膜内侧由上而下流动，将质量浓度为35％的混合醇胺溶液(质量浓度为15％的乙醇胺、20％的甲基二乙醇胺与65％水的混合物)通入中空纤维膜外侧，通过逆向流动脱除混合气体中的H2S。使用后的混合醇胺溶液可经过再生处理后，重新进入膜式湿法脱硫反应器进行利用。将脱硫后的混合气体冷却后，增压到0.8Mpa，经固体分子筛(沸石型硅酸铝盐)吸附脱除混合气体中的H2O。将脱除水分后的混合气体以流量50m3/h自下而上通入脱碳吸收塔，与质量浓度为30％的复合胺基吸收剂(溶质组成为乙醇胺、N甲基二乙醇胺和哌嗪(摩尔比为1:1:0.6)，溶剂为水)逆向流动反应，将脱除CO2提纯后的气体由塔顶引出，冷却至20℃。使用后的复合胺基吸收剂可经过再生处理后，重新进入脱碳吸收塔进行利用。将脱除CO2后的混合气体压缩到20MPa，经固体分子筛(沸石型硅酸铝盐)吸附脱除水分后，得到H2和CH4总浓度为96％的车用生物氢烷气。
实施例2
将城乡有机废弃物发酵制备的混合气体(各成分体积浓度为：9.6％的H2、40％的CH4、50％的CO2、0.2％的H2S以及0.2％的H2O)收集储存，混合气压力为2kPa、温度为19℃。将混合气体经鼓风机增压至30kPa，送往膜式湿法脱硫反应器。脱硫反应器装填有聚丙烯中空纤维膜(膜内径0.4mm，孔隙率60％，平均孔径0.05μm)。混合气体以流量360m3/h通入中空纤维膜内侧由上而下流动，将质量浓度为25％的混合醇胺溶液(质量浓度为10％的乙醇胺、15％的甲基二乙醇胺与75％水的混合物)通入中空纤维膜外侧，通过逆向流动脱除混合气体中的H2S。使用后的混合醇胺溶液可经过再生处理后，重新进入膜式湿法脱硫反应器进行利用。将脱硫后的混合气体冷却后，增压到0.9Mpa，经固体分子筛(沸石型硅酸铝盐)吸附脱除混合气体中的H2O。将脱除水分后的混合气体以流量40m3/h自下而上通入脱碳吸收塔，与质量浓度为30％的复合胺基吸收剂(溶质组成为乙醇胺、N甲基二乙醇胺和哌嗪(摩尔比为1:1:0.6)，溶剂为水)逆向流动反应，将脱除CO2提纯后的气体由塔顶引出，冷却至30℃。使用后的复合胺基吸收剂可经过再生处理后，重新进入脱碳吸收塔进行利用。将脱除CO2后的混合气体压缩到20MPa，经固体分子筛(沸石型硅酸铝盐)吸附脱除水分后，得到H2和CH4总浓度为97％的车用生物氢烷气。
实施例3
将城乡有机废弃物发酵制备的混合气体(各成分体积浓度为：21％的H2、35％的CH4、42.8％的CO2、0.6％的H2S以及0.6％的H2O)收集储存，混合气压力为3kPa、温度为20℃。将混合气体经鼓风机增压至40kPa，送往膜式湿法脱硫反应器。脱硫反应器装填有聚丙烯中空纤维膜(膜内径0.4mm，孔隙率60％，平均孔径0.1μm)。混合气体以流量320m3/h通入中空纤维膜内侧由上而下流动，将质量浓度为30％的混合醇胺溶液(质量浓度为15％的乙醇胺、15％的甲基二乙醇胺与70％水的混合物)通入中空纤维膜外侧，通过逆向流动脱除混合气体中的H2S。使用后的混合醇胺溶液可经过再生处理后，重新进入膜式湿法脱硫反应器进行利用。将脱硫后的混合气体冷却后，增压到1MPa，经固体分子筛(沸石型硅酸铝盐)吸附脱除混合气体中的H2O。将脱除水分后的混合气体以流量32m3/h自下而上通入脱碳吸收塔，与质量浓度为30％的复合胺基吸收剂(溶质组成为乙醇胺、N甲基二乙醇胺和哌嗪(摩尔比为1:1:0.6)，溶剂为水)逆向流动反应，将脱除CO2提纯后的气体由塔顶引出，冷却至40℃。使用后的复合胺基吸收剂可经过再生处理后，重新进入脱碳吸收塔进行利用。将脱除CO2后的混合气体压缩到20MPa，经固体分子筛(沸石型硅酸铝盐)吸附脱除水分后，得到H2和CH4总浓度为98％的车用生物氢烷气。
最后，需要注意的是，以上列举的仅是本发明的具体实施例。显然，本发明不限于以上实施例，还可以有很多变形。本领域的普通技术人员能从本发明公开的内容中直接导出或联想到的所有变形，均应认为是本发明的保护范围。
Claims (1)
1.城乡有机废弃物发酵净化提纯生产车用生物氢烷气的方法，其特征在于，具体包括下述步骤：
(1)将城乡有机废弃物发酵成的混合气体收集储存后，将混合气体经鼓风机增压至20～40kPa；
所述城乡有机废弃物发酵制备的混合气体，含有的成分为：5～21％的H2、35～63％的CH4、30～50％的CO2、0.2～1％的H2S、0.2～1％的H2O；各成分的浓度为体积浓度；
(2)利用膜式湿法脱硫反应器对增压后的混合气体进行脱硫，膜式湿法脱硫反应器中装填有中空纤维膜，将混合气体以流量320～400m3/h通入中空纤维膜内侧由上而下流动，并将质量浓度为25～35％的混合醇胺溶液通入中空纤维膜外侧，通过逆向流动脱除混合气体中的H2S；
所述膜式湿法脱硫反应器装填的中空纤维膜为聚丙烯中空纤维膜，膜内径为0.4mm，孔隙率为60％，平均孔径为0.01～0.1μm；
所述混合醇胺溶液是溶质为乙醇胺和甲基二乙醇胺，溶剂为水的混合溶液，其中，乙醇胺的质量浓度为10～15％，甲基二乙醇胺的质量浓度15～20％；使用后的混合醇胺溶液经过在温度110～120℃条件下加热使CO2气体完全脱附进行再生处理后，能重新进入膜式湿法脱硫反应器进行利用；
(3)将脱硫后的混合气体冷却后，增压到0.8～1.0Mpa，再经固体分子筛吸附脱除混合气体中的H2O；
(4)将脱除水分后的混合气体以流量32～50m3/h自下而上通入脱碳吸收塔，与质量浓度为30％的复合胺基吸收剂逆向流动反应，然后将脱除CO2提纯后的混合气体由脱碳吸收塔的塔顶引出，再冷却至20～40℃；发酵混合气体中CO2脱除效率高达95～99％；
所述复合胺基吸收剂是溶质为乙醇胺、N甲基二乙醇胺和哌嗪，溶剂为水的混合溶液，其中，乙醇胺、N甲基二乙醇胺和哌嗪的摩尔比为1:1:0.6；使用后的复合胺基吸收剂经过在温度110～120℃条件下加热使CO2气体完全脱附进行再生处理后，能重新进入脱碳吸收塔进行利用；
(5)将经过步骤(4)处理后的混合气体压缩到20MPa，经固体分子筛吸附脱除水分后，即得到H2和CH4总浓度高于95％的车用生物氢烷气；净化提纯后气体产物中的CO2体积浓度低于3％，H2S浓度低于15mg/m3，高位发热量大于31.415MJ/m3。
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