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.

基于我们对液体燃料萃取-氧化原位产物分离(ECODS)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从燃料中分离更多的杂原子，并从根本上了解它们对脱硫的影响。在新开发的方法的技术实施方面，两个反应步骤(底物氧氧化，催化剂水溶液中携氧)的空间分离也应该在连续过程中进行。在先前非常成功的项目中，发现了一种高效的氧化-萃取脱硫系统(HPA-5水溶液)，作为迄今工业上多相催化加氢脱硫的替代工艺。我们的系统的优点是所有的脱硫产物(硫酸、磺酸、羧酸)都是从有机相到水相的原位萃取。这一点可以在模型油和真实油中得到证明。继续提议的关键是，我们新开发的液体燃料原位脱硫反应系统(HPA-5水溶液)具有有效地脱硫芳香族和脂肪族体系的潜力。然而，水相中分解产物的积累对催化剂体系有抑制作用。这可以通过添加草酸来避免。在这些有希望的结果的基础上，有必要对燃料中含氮和含氧组分对脱硫的影响进行进一步调查(如继续提案中计划的那样)。因此，例如，含氮燃料组分，如吲哚或喹啉，可能对我们的催化剂系统具有类似的活化作用，这可能对我们的概念的技术实施做出重大贡献。因此，在继续这项提议时，应从根本上研究各种含氮和含氧组分对液体燃料氧化-萃取法脱硫的影响。为此目的，应调查和了解以合适的模型物质为基础的影响，例如脱氮效果对燃料脱硫的影响。这种方法有可能进一步加强我们新开发的脱硫技术，理想的情况是将其与从液体燃料中去除更多的杂原子相结合。