Collaborative Research: CAS: Electrochemical Approaches to Sustainable Dinitrogen Fixation

该奖项来自化学系化学催化（CAT）项目，支持由北卡罗来纳大学教堂山分校的亚历山大·米勒教授组成的合作团队；罗格斯大学的Alan Goldman、Frank Felder和Gal Hochman；以及耶鲁大学的罗伯特·克拉布特里、帕特里克·霍兰德和詹姆斯·梅尔。该团队正在设计将氮转化为氨的新方法。氨是许多有用材料的前体，包括大多数肥料、乳胶、尼龙、炸药和一些电池电解质。目前制造氨的方法是能源密集型的，并且依赖化石燃料作为氢的来源。根据初步结果，该团队正在开发一种以水为氢源的工艺。大气中的氮（占我们呼吸的空气的78%）是另一种原料。这项工作的关键是新的钼基和铼基催化剂，它们将大气中的氮分解成氮原子。研究生接受计算和实验室技术的实践培训，为他们未来在能源和可持续发展领域的职业生涯做好准备。除了实验室工作外，师生团队还与经济学家合作，测试各种先进制造方法的可行性。三个州正在开展推广项目，向公众宣传固氮作用。该合作研究项目的目标是发现和研究电化学还原N2的新型分子催化剂。在化学部化学催化项目的资助下，北卡罗来纳大学教堂山分校的米勒教授、罗格斯大学的戈德曼、费尔德和霍克曼教授，以及耶鲁大学的克拉伯里、霍兰德和梅尔教授，正在开发能够通过直接氮气分裂产生NH3的电催化催化剂，形成金属氮化物配合物。详细的研究提供了指导设计新的钼和铼配合物和电催化反应条件的机理。通过这种合作方法，系统和方法的多样性正在被利用来产生广泛适用的见解，以了解过渡金属配合物的性质，这些配合物有利于N2分裂和氮化中间体的质子化，在适合电催化的条件下产生NH3。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

This award from the Chemical Catalysis (CAT) Program in the Division of Chemistry, supports a collaborative team consisting of Professors Alexander Miller at the University of North Carolina at Chapel Hill; Alan Goldman, Frank Felder and Gal Hochman at Rutgers University; and Robert Crabtree, Patrick Holland, and James Mayer at Yale University. The team is designing new ways to convert nitrogen into ammonia. Ammonia is the precursor to many useful materials, including most fertilizers, latex, nylon, explosives and some electrolytes for batteries. Present day methods for making ammonia are energy intensive and rely on fossil fuels as a source of hydrogen. Acting on preliminary results, the team is developing a processes that uses water as the hydrogen source. Atmospheric nitrogen, which comprises ~78% of the air we breathe, is the other feedstock. Key to this work are new molybdenum- and rhenium-based catalysts that cleave atmospheric nitrogen into nitrogen atoms. Graduate students receive hands-on training on calculations and laboratory techniques to prepare them for future careers in energy and sustainability. In addition to the laboratory work, the faculty-student teams are working with economists to test the feasibility of diverse approaches to advanced manufacturing. Outreach programs in three states are underway to educate the public about nitrogen fixation. The proposed collaborative research project targets the discovery and mechanistic study of new molecular catalysts for electrochemical N2 reduction. With funding from the Chemical Catalysis Program in the Chemistry Division, Professor Miller of the University of North Carolina at Chapel Hill, Professor Goldman, Felder and Hochman of Rutgers University, and Professors Crabtree, Holland, and Mayer of Yale University are developing catalysts capable of electrocatalytic NH3 production via direct N2 splitting to form metal nitride complexes. Detailed studies afford mechanistic insight that is guiding the design of new molybdenum and rhenium complexes and reaction conditions for electrocatalysis. The diversity of systems and methods available through this collaborative approach are being leveraged to generate broadly applicable insights into the properties of transition metal complexes that favor N2 splitting and protonation of nitride intermediates to yield NH3 under conditions amenable to electrocatalysis.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.