CN110564478A - 一种化学链燃烧载氧体 - Google Patents

一种化学链燃烧载氧体 Download PDF

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CN110564478A
CN110564478A CN201910691059.2A CN201910691059A CN110564478A CN 110564478 A CN110564478 A CN 110564478A CN 201910691059 A CN201910691059 A CN 201910691059A CN 110564478 A CN110564478 A CN 110564478A
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陶进峰
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Abstract

本发明提供一种化学链燃烧载氧体，将CaSO4/CaS、BaSO4/BaS、SrSO4/SrS、NiO/Ni、Fe2O3/Fe3O4/FeO/Fe、Co3O4/CoO/Co、Mn2O3/Mn3O4/MnO、CuO/Cu2O/Cu等固体活性成分浸没在熔盐载体中并全部或部分溶解在熔盐载体中，形成液态载氧体或液固两相混合载氧体，载氧体烧结率最低可降至0%，有效解决了现有固体载氧体烧结问题。

Description

一种化学链燃烧载氧体
技术领域
本发明涉及化学链燃烧载氧体，属于节能环保、新能源技术领域。
背景技术
化学链燃烧（Chemical Looping Combustion，简称CLC）基本原理是通过载氧体与燃料、空气的交替循环反应，将空气中的氧传递给燃料，实现燃料与空气的非接触燃烧。化学链燃烧系统通常由燃料反应器、空气反应器和载氧体组成。其中载氧体通常由活性成分与载体组成，活性成分是参与反应传递氧的物质，金属活性成分主要包括NiO/Ni、Fe2O3/Fe3O4/FeO/Fe、Co3O4/CoO/Co、Mn2O3/Mn3O4/MnO、CuO/Cu2O/Cu和CdO/Cd，非金属活性成分主要包括CaSO4/CaS、BaSO4/BaS和SrSO4/SrS，其中，CaSO4、BaSO4和SrSO4是氧化态活性成分，CaS、BaS和SrS是还原态活性成分；载体则是用来承载活性成分的物质，常见载体包括Al2O3、SiO2、TiO2、ZrO2、MgAl2O4、海泡石、高岭土、膨润土。
化学链燃烧包括载氧体还原过程、载氧体氧化过程。以CaSO4/CaS载氧体燃烧CH4为例，见图1，首先，在燃料反应器内，进行载氧体还原反应，氧化态活性成分CaSO4被CH4还原成还原态活性成分CaS，见公式1，这是载氧体还原过程；然后，CaS送往空气反应器内，进行载氧体氧化反应，还原态活性成分CaS被空气氧化成氧化态活性成分CaSO4，见公式2，这是载氧体氧化过程。上述两反应的总反应，见公式3，与传统CH4燃烧相同。
CaSO4+CH4→CaS + CO2+H2O 公式1
CaS+O2→CaSO4 公式2
CH4+O2→CO2+H2O 公式3
化学链燃烧的燃料燃烧产物不会被氮气和过量空气稀释，CO2富集，降低CO2分离系统能耗及成本；燃烧过程中，燃料与氧气不直接接触，避免了燃料型NOx的生成；化学链燃烧还可以用于部分氧化、气化、重整。化学链燃烧是解决当前全球气候变暖问题最有前途的技术之一，是解决能源利用与环境问题的创新性突破口，具有广阔的开发和应用前景，对于能源安全和化学工业等领域也具有重要战略意义。
化学链燃烧至今仍停留在试验研究阶段，其主要原因是尚未研发出适合工业应用的载氧体。金属载氧体拥有较高反应速率，非金属载氧体价格低廉，但金属载氧体和非金属载氧体存在烧结问题，难以满足工业应用要求。因此研发抗烧结载氧体对化学链燃烧工业化非常重要。
发明内容
针对化学链的固体载氧体烧结问题，本发明提供一种化学链燃烧载氧体，该化学链燃烧载氧体将固体活性成分浸没在熔盐载体中并全部或部分溶解在熔盐载体中，形成液态载氧体或液固两相混合载氧体，有效解决了现有固体载氧体烧结问题。
本发明提供了一种化学链燃烧载氧体，化学链燃烧载氧体由活性成分及熔盐载体组成，活性成分浸没在熔盐载体中并全部或部分溶解在熔盐载体中；所述活性成分为非金属活性成分、金属活性成分或其混合物；所述非金属活性成分为CaSO4/CaS、BaSO4/BaS、SrSO4/SrS或其复合物，优选CaSO4/CaS；所述金属活性成分为NiO/Ni、Fe2O3/ Fe3O4/FeO/Fe、Co3O4/CoO/Co、Mn2O3/Mn3O4/MnO、CuO/Cu2O/Cu、CdO/Cd或其复合物，优选Fe2O3/ Fe3O4/FeO、CuO/Cu2O；所述熔盐载体对所述活性成分总溶解度S满足：0.1%<S<100%，优选1%<S<30%。
所述熔盐载体包括CaCl2、CaBr2、NaBr、CaCl2-NaF、CaCl2-CaF2、CaCl2-NaCl、NaCl-KCl-NaF、Na2CO3-Na2SiO3、K2CO3-K2SiO3或Na2CO3-K2CO3-Na2SiO3，优选CaCl2、CaCl2-NaCl或Na2CO3-K2CO3-Na2SiO3。
所述活性成分为CaSO4/CaS或CuO/Cu2O时，所述熔盐载体包括CaCl2、CaCl2-NaCl、Na2CO3-Na2SiO3、K2CO3-K2SiO3或Na2CO3-K2CO3-Na2SiO3，优选CaCl2或Na2CO3-K2CO3-Na2SiO3。
所述活性成分总质量为所述化学链燃烧载氧体的0.1%~95%，优选0.5%~20%；所述活性成分为非金属活性成分时，所述非金属活性成分总质量为所述化学链燃烧载氧体的1%~50%，优选5%~20%；所述活性成分为金属活性成分时，所述金属活性成分总质量为所述化学链燃烧载氧体的0.1%~50%，优选0.5%~5%。
所述化学链燃烧载氧体的反应温度为300-1200℃，优选700-1000℃；所述活性成分为CaSO4/CaS时，所述化学链燃烧载氧体的反应温度为700-1200℃，优选800-1000℃；所述活性成分为CuO/Cu2O时，所述化学链燃烧载氧体的反应温度为600-1100℃，优选750-950℃。
所述化学链燃烧载氧体适用于化学链燃烧、化学链部分氧化、化学链气化、化学链重整。
所述化学链燃烧载氧体可用于处理热解气、合成气、有机废气、焦油、生物油、废油、塑料、玻璃钢、废线路板、线路板树脂粉、污泥、生物质、煤、硫矿、硫磺。
所述化学链燃烧载氧体与燃料或空气的气液接触形态为气相以气泡形态分散在熔盐中、熔盐以液滴状分散在气相中或熔盐以膜状与气相接触。
本发明的有益效果：本发明打破固体活性成分负载在固体载体上偏见，将固体活性成分浸没在熔盐载体中并全部或部分溶解在熔盐载体中，形成液态载氧体或液固两相混合载氧体，载氧体烧结率最低可降至0%，可有效解决现有固体载氧体烧结问题。
附图说明
图1是化学链燃烧示意图。
具体实施方式
下面结合具体实施方式对本发明的发明内容作进一步的详细描述。应理解，本发明的实施例只用于说明本发明而非限制本发明，在不脱离本发明技术思想的情况下，根据本领域普通技术知识和惯用手段，做出的各种替换和变更，均应包括在本发明的范围内。
实施例1
化学链燃烧载氧体由活性成分及熔盐载体组成，活性成分浸没在熔盐载体中并全部溶解在熔盐载体中，形成液态载氧体；所述活性成分为CaSO4/CaS，初始时所述活性成分为CaSO4；所述熔盐载体为CaCl2；初始时，所述活性成分总质量为所述化学链燃烧载氧体的4~5%；所述熔盐载体对所述活性成分总溶解度S满足：5%<S<15%；所述化学链燃烧载氧体的温度为900-950℃。
上述载氧体化学链燃烧过程包括载氧体还原过程、载氧体氧化过程，具体如下：
载氧体还原过程：将载氧体送入900-950℃燃料反应器中与燃料CH4反应，燃料反应器内压力为1000~5000Pa，燃料CH4以鼓泡方式通入载氧体中，气液接触的相界面积与液相体积之比为100~200m2/m3，该过程中氧化态活性成分CaSO4被CH4还原成还原态活性成分CaS，反应后载氧体送往空气反应器。
载氧体氧化过程：在900-950℃空气反应器内，压力为1000~5000Pa，空气以鼓泡方式通入载氧体中，气液接触的相界面积与液相体积之比为100~200m2/m3，该过程中还原态活性成分CaS被空气氧化成氧化态活性成分CaSO4，反应后载氧体送往燃料反应器。
交替循环载氧体还原过程、载氧体氧化过程，实现化学链燃烧。
上述载氧体蓄热能力强，可有效防止反应器内温度剧烈变化，避免局部高温，有效控制热力型NOx生成；同时化学链载氧体也是热载体，可从空气反应器吸热供燃料反应器使用。
上述载氧体在化学链燃烧CH4过程中以液态形式存在，不存在载氧体烧结现象，载氧体烧结率为0%，彻底避免了载氧体烧结问题。
实施例2
本实施例与实施例1不同之处在于：1）活性成分浸没在熔盐载体中并部分溶解在熔盐载体中，形成液固两相混合载氧体；2）初始时，活性成分总质量为化学链燃烧载氧体的15~20%。
本实施例中，每小时每1m3载氧体可处理60m3的CH4，处理速率高。
本实施例中，活性成分溶解、浸没在液态熔盐载体中，可有效抑制载氧体烧结。
实施例3
本实施例与实施例1不同之处在于：1）活性成分为CuO/Cu2O，初始时活性成分为CuO；2）初始时，活性成分总质量为化学链燃烧载氧体的0.5~0.6%；3)熔盐载体对活性成分总溶解度S满足：0.6%<S<5%。
实施例4
本实施例与实施例1不同之处在于：1）活性成分为CaSO4/CaS和CuO/Cu2O混合物，初始时活性成分为CaSO4和CuO混合物；2）初始时，活性成分CaSO4质量为化学链燃烧载氧体的4~5%，活性成分CuO质量为化学链燃烧载氧体的0.5~0.6%。
实施例5
本实施例与实施例1不同之处在于燃料为硫矿或硫磺，本实施例可制备高纯度二氧化硫。
实施例6
本实施例与实施例1不同之处在于初始时所述活性成分总质量为所述化学链燃烧载氧体的8~10%。
以上所述，仅为本发明较佳的具体实施方式，但本发明的保护范围并不局限于此，任何熟悉本技术领域的技术人员在本发明披露的技术范围内，可轻易想到的变化或替换，都应涵盖在本发明的保护范围之内。因此，本发明的保护范围应该以权利要求书的保护范围为准。

Claims (10)

1.本发明提供一种化学链燃烧载氧体，其特征在于，化学链燃烧载氧体由活性成分及熔盐载体组成，活性成分浸没在熔盐载体中并全部或部分溶解在熔盐载体中；所述活性成分为非金属活性成分、金属活性成分或其混合物；所述非金属活性成分为CaSO4/CaS、BaSO4/BaS、SrSO4/SrS或其复合物，优选CaSO4/CaS；所述金属活性成分为NiO/Ni、Fe2O3/ Fe3O4/FeO/Fe、Co3O4/CoO/Co、Mn2O3/Mn3O4/MnO、CuO/Cu2O/Cu、CdO/Cd或其复合物，优选Fe2O3/Fe3O4/FeO、CuO/Cu2O；所述熔盐载体对所述活性成分总溶解度S满足：0.1%<S<100%，优选1%<S<30%。
2.根据权利要求1所述的化学链燃烧载氧体，其特征在于，所述熔盐载体包括CaCl2、CaBr2、NaBr、CaCl2-NaF、CaCl2-CaF2、CaCl2-NaCl、NaCl-KCl-NaF、Na2CO3-Na2SiO3、K2CO3-K2SiO3或Na2CO3-K2CO3-Na2SiO3，优选CaCl2、CaCl2-NaCl或Na2CO3-K2CO3-Na2SiO3。
3.根据权利要求1所述的化学链燃烧载氧体，其特征在于，所述活性成分为CaSO4/CaS或CuO/Cu2O时，所述熔盐载体包括CaCl2、CaCl2-NaCl、Na2CO3-Na2SiO3、K2CO3-K2SiO3或Na2CO3-K2CO3-Na2SiO3，优选CaCl2或Na2CO3-K2CO3-Na2SiO3。
4.根据权利要求1所述的化学链燃烧载氧体，其特征在于，所述活性成分总质量为所述化学链燃烧载氧体的0.1%~95%，优选0.5%~20%。
5.根据权利要求1所述的化学链燃烧载氧体，其特征在于，所述活性成分为非金属活性成分时，所述非金属活性成分总质量为所述化学链燃烧载氧体的1%~50%，优选5%~20%。
6.根据权利要求1所述的化学链燃烧载氧体，其特征在于，所述活性成分为金属活性成分时，所述金属活性成分总质量为所述化学链燃烧载氧体的0.1%~50%，优选0.5%~5%。
7.根据权利要求1所述的化学链燃烧载氧体，其特征在于，所述化学链燃烧载氧体的反应温度为300-1200℃，优选700-1000℃。
8.根据权利要求1所述的化学链燃烧载氧体，其特征在于，所述活性成分为CaSO4/CaS时，所述化学链燃烧载氧体的反应温度为700-1200℃，优选800-1000℃；所述活性成分为CuO/Cu2O时，所述化学链燃烧载氧体的反应温度为600-1100℃，优选750-950℃。
9.根据权利要求1所述的化学链燃烧载氧体，其特征在于，所述化学链燃烧载氧体适用于化学链燃烧、化学链部分氧化、化学链气化、化学链重整。
10.根据权利要求1所述的化学链燃烧载氧体，其特征在于，所述化学链燃烧载氧体可用于处理热解气、合成气、有机废气、焦油、生物油、废油、塑料、玻璃钢、废线路板、线路板树脂粉、污泥、生物质、煤、硫矿、硫磺。
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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN114314509A (zh) * 2021-11-30 2022-04-12 西安交通大学 一种液态化学链气化/重整制备富氢合成气系统与工艺
CN114353063A (zh) * 2021-11-30 2022-04-15 西安交通大学 一种液态化学链燃烧热电联产及碳捕集系统与工艺

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN114314509A (zh) * 2021-11-30 2022-04-12 西安交通大学 一种液态化学链气化/重整制备富氢合成气系统与工艺
CN114353063A (zh) * 2021-11-30 2022-04-15 西安交通大学 一种液态化学链燃烧热电联产及碳捕集系统与工艺

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