Influence of N- and O-containing heteroatoms on the continuous desulfurization of heavy oils and liquid fuels using catalytic oxidation of organic compounds with aqueous polyoxometalate solutions

含氮和含氧杂原子对多金属氧酸盐水溶液催化氧化有机化合物连续脱硫重油和液体燃料的影响

• 批准号: 265880028
• 负责人: Professor Dr.-Ing. Jakob Albert
• 金额: --
• 依托单位: Institut für Technische und Makromolekulare Chemie
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2014
• 资助国家: 德国
• 起止时间: 2013-12-31 至 2022-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/265880028?language=en
• 关键词: Influence; containing; heteroatoms; continuous; desulfurization

Based on our successful preliminary investigations on the extractive-oxidative desulfurization of liquid fuels with in-situ product separation (ECODS), the overall goal of the follow-up project is to extend the previously developed technology to the separation of further heteroatoms from fuels and to fundamentally understand their effect on desulfurization. With regard to a technical implementation of the newly developed method, a spatial separation of the two reaction steps (substrate oxidation by oxygen, loading of the aqueous catalyst solution with oxygen) should also be carried out in a continuous process.In the previous, very successful project, an efficient system for oxidative-extractive desulfurization (aqueous HPA-5 solution) was found as an alternative to the hitherto industrial process of heterogeneously catalyzed hydrodesulfurization. The advantage of our system is that all desulfurization products (sulfuric acid, sulfonic acids, carboxylic acids) are extracted in-situ from the organic to the aqueous phase. This could be shown for model oils as well as for real oils.Essential for the continuation proposal is that our newly developed reaction system (aqueous HPA-5 solution) for the in-situ desulfurization of liquid fuels has the potential to efficiently desulfurize both aromatic and aliphatic systems. However, accumulation of decomposition products in the aqueous phase has been found to inhibit the catalyst system. This could be circumvented by the addition of oxalic acid. Based on these promising results, further investigations (as planned in the continuation proposal) are necessary with regard to the influence of N- and O-containing components in fuels on desulfurization. Thus, for example, N-containing fuel components such as indoles or quinolines could have a similar activating effect on our catalyst system, which could significantly contribute to the technical implementation of our concept. Therefore, in the continuation of the proposal, the influence of various N- and O-containing components on the oxidative-extractive desulfurization of liquid fuels should be fundamentally investigated. For this purpose, the influence on the basis of suitable model substances, e.g. the denitrification effect on the desulfurization of fuels should be investigated and understood. This approach has the potential to further enhance our newly developed desulfurization technology and, ideally, to combine it with the removal of further heteroatoms from liquid fuels.

基于我们对具有原位产品分离（ECOD）的液体燃料的提取性氧化脱硫化的成功初步研究，后续项目的总体目标是将先前开发的技术扩展到将进一步的杂原子从燃料中分离出来，并从根本上了解其对脱硫化的影响。关于新开发方法的技术实施，还应在连续的过程中进行两个反应步骤（通过氧氧化氧化，用氧气氧化，用氧气氧化的底物氧化）的负载。异质催化的氢化硫化。我们系统的优点是，从有机相到水相的原位提取所有脱硫产物（硫酸，磺酸，羧酸）。对于模型油和实际油，可以显示这一点。对于持续提案而言，对于我们新开发的反应系统（HPA-5水溶液）用于液态燃料的原位脱硫具有有效脱硫芳香和脂肪型系统的潜力。但是，已经发现分解产物在水相中的积累抑制催化剂系统。可以通过添加草酸来规避这。基于这些有希望的结果，对于燃料中含N和O的成分对去硫化的影响是必要的进一步研究（按照延续建议中计划）。因此，例如，含N的燃料成分（例如吲哚或喹啉）可能会对我们的催化剂系统产生类似的激活作用，这可能会极大地有助于我们概念的技术实施。因此，在延续提案时，应从根本上研究各种含N和O的成分对液体燃料的氧化提取性去硫化的影响。为此，基于合适的模型物质的影响，例如应研究和理解对燃料脱硫化的反硝化作用。这种方法有可能进一步增强我们新开发的去硫化技术，理想情况下，将其与从液体燃料中取出进一步的杂原子相结合。