SGER: Carbon Supported Non-Noble Metal Electrocatalysts Based on Macrocyclic Compounds

贵金属电催化剂是众所周知的，并广泛用于制造各种电化学装置，然而这些材料的高成本显著限制了它们的商业应用。尽管近年来非贵金属催化剂的研究取得了显著进展，但现有的非贵金属催化剂在催化活性、耐久性和化学/电化学稳定性等方面都无法达到铂基催化剂的水平，因此，基于大环化合物的新型非贵金属电催化剂的合成与表征是本文的研究重点。该催化剂将由过渡金属与有机前体螯合并浸渍到改性碳载体中形成富氮纳米结构来合成。本论文的研究成果对于设计新型的大环化合物电催化剂以及理解基于大环化合物的电催化剂的结构-性能关系具有重要的理论意义和应用价值。国家安全和可持续能源。重点研究了碳载体的功能性、金属阳离子大环与载体的配位作用以及催化活性中心的分布。这项工作的更广泛影响将增强新一代非贵金属电催化剂的设计，这些催化剂可用于不同类型的低温燃料电池，如H2，甲醇，乙醇或甲酸燃料电池，电解槽和氢分离装置。从催化剂合成到燃料电池制造的完整实验周期将验证工作的结果。这项研究将与其他科学学科形成联系，例如生物催化剂，其中含有铁阳离子的单一酶位点比Pt原子的活性高两个数量级。这项工作将为新兴的非贵金属催化剂领域的学生提供重要的教育背景。此外，它将有助于加强与其他大学的关系，例如芝加哥的伊利诺伊大学，并为未来的项目提供资金。该项目对于PI作为康涅狄格大学的新教员继续她在燃料电池催化剂领域的工作至关重要，该领域已经开始并已经获得国家和国际认可。

0736111Smirnova, Alevtina Noble metal electrocatalysts are well known and extensively used for manufacturing of various kinds of electrochemical devices, however the high cost of these materials significantly restricts their commercial application. Though remarkable progress has been made recently, none of the existing non-noble metal catalysts can reach the level of a Pt based catalysts in terms of catalytic activity, durability and chemical/electrochemical stability.The proposed research is focused on synthesis and characterization of novel nonnoble metal electro-catalysts based on macrocyclic compounds. The catalysts will be synthesized from transition metals chelated with organic precursors and impregnated into modified carbon supports forming nitrogen enriched nano-structures. As a result, a self-organized network of macro-cycles containing stabilized transition metal cations will be formed inside the modified carbon support possessing high catalytic activity toward oxygen reduction and hydrogen oxidation.The intellectual merit of the proposed work is in designing new catalysts and understanding the structure-properties relationship of the electrocatalysts based on macrocyclic compounds that have direct influence on industrial, environmental, national security and sustainable energy resources. The novel catalysts will be investigated with emphasis on carbon support functionality, coordination effect between metal cation macrocycles and support, and the distribution of active catalytic sites. The broader impacts of this work will enhance design of a new generation of non-noble electrocatalysts that can be used in different kinds of low temperature fuel cells, such as H2, methanol, ethanol, or formic acid fuel cells, electrolyzers, and hydrogen separation devices. The completed experimental cycle from synthesizing catalyst to manufacturing a fuel cell will validate the results of the work. This study will form links to other scientific disciplines, such as those regarding bio-catalysts in which a single enzymatic site containing iron cation is two orders of magnitude more active than Pt atom.This work will give a significant educational background for the students in the emerging area of non-noble metal catalysts. Furthermore, it will allow to enhance relationships with other universities, e.g. University of Illinois in Chicago, and to seed money for future projects. This project is vitally important for the PI as a new faculty member at the University of Connecticut to continue her work in the area of fuel cell catalysts that has been started earlier and has already found national and international recognition.