Interplay of nitrogen- and oxygen functionalities of carbon based catalysts in redox reactions

氧化还原反应中碳基催化剂的氮和氧官能团的相互作用

• 批准号: 430661467
• 负责人: Professor Dr. Olaf Klepel
• 金额: --
• 依托单位: Fachgebiet Technische Chemie
• 依托单位国家: 德国
• 项目类别: Research Grants
• 资助国家: 德国
• 项目状态: 未结题
• 来源: https://gepris.dfg.de/gepris/projekt/430661467?language=en
• 关键词: Interplay; nitrogen; oxygen; functionalities; carbon

There is a long-standing interest on the catalytic properties of carbon materials. This interest has even been increased in the recent years due to the developments of novel applications for energy storage and conversion, respectively. Furthermore, carbon based catalysts are also discussed as an energy-saving alternative to long-standing used catalytic systems of the industrial chemistry. Nevertheless, up to date most of the examined carbon catalysts do not exhibit sufficient catalytic activity in a majority of studied reactions. Nitrogen doping of the carbons can enhance the activity for different redox reactions considerably. However, fundamental questions are still open and needed to be clarified, and from that the objectives of the project are derived. This concerns on the one hand the contribution of particular nitrogen functionalities to the catalytic functions and, on the other hand, the interaction of nitrogen and oxygen functionalities with each other as well. In this context, the impact of nitrogen functionalities on the formation of particular oxygen functionalities has to be considered, too. A modular concept of catalyst synthesis is required to investigate the matter. That concept shall be executed applying template assisted routes, which enable the formation of carbon replicas with controlled surface composition, structure and porosity. The catalysts will contain nitrogen functionalities with varied ratios of pyrrole- to pyridine-like species. The impact of the nitrogen species on the formation of oxygen functionalities will be investigated applying defined post treatments with oxidizing agents. The catalysts will be investigated in different test reactions such as the oxidative dehydrogenation of hydrocarbons, and the oxidation of sulphurous acid. The experimental findings shall be completed by quantum chemical calculations on the nature of nitrogen functionalities in model carbons. The prospective results of the submitted research project will provide a better understanding of the interplay of nitrogen and oxygen functionalities with each other in the examined reactions as well as improve a knowledge about new synthesis methods and possible catalytic applications of nitrogen-doped carbon materials.

碳材料的催化特性长期存在。由于新的储能和转换应用程序的发展，近年来，近年来，这种兴趣甚至增加了。此外，还讨论了基于碳的催化剂作为工业化学长期使用的催化系统的节能替代品。然而，最新的大多数检查的碳催化剂在大多数研究的反应中都没有表现出足够的催化活性。碳的氮掺杂可以大大增强不同氧化还原反应的活性。但是，基本问题仍然是开放的，需要澄清，从该项目的目标得出。一方面，这涉及特定的氮功能对催化功能的贡献，另一方面，氮和氧功能之间的相互作用也相互作用。在这种情况下，也必须考虑氮功能对特定氧气功能形成的影响。需要一个模块化的催化剂合成概念来研究此问题。该概念应在应用模板辅助路线上执行，这使得具有控制表面组成，结构和孔隙率的碳复制品的形成。这些催化剂将包含具有吡咯与吡啶样物种比例不同的氮功能。将研究氮物种对氧气功能的形成的影响，并使用氧化剂使用定义的后处理剂。催化剂将在不同的测试反应中进行研究，例如烃的氧化脱氢和硫酸的氧化。实验发现应通过量子化学计算来完成，该计算对碳中的氮功能性质。提交的研究项目的前瞻性结果将更好地理解氮和氧功能在检查的反应中相互的相互作用，并提高了有关新合成方法的知识以及氮掺杂的碳材料的可能催化应用。