Collaborative Research: CAS: Electrochemical Approaches to Sustainable Dinitrogen Fixation

合作研究：CAS：可持续二氮固定的电化学方法

• 批准号: 1954942
• 负责人: Alexander Miller
• 金额: $ 31.08万
• 依托单位: University of North Carolina at Chapel Hill
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2020
• 资助国家: 美国
• 起止时间: 2020-08-01 至 2023-10-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1954942&HistoricalAwards=false
• 关键词: Collaborative; Research; CAS; Electrochemical; Approaches

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.

该奖项来自化学系的化学催化（CAT）计划，支持由查佩尔山的北卡罗来纳州大学的亚历山大米勒教授组成的合作团队;罗格斯大学的艾伦·戈德曼，弗兰克·费尔德和加尔·霍曼;耶鲁大学的罗伯特·克拉布特里，帕特里克·霍兰德和詹姆斯·迈耶。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。目前用于制造氨的方法是能量密集型的，并且依赖于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使用水作为氢源的工艺。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和铱基催化剂，将大气中的氮分解为氮原子。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方面的职业做好准备。除了实验室工作外，师生团队还与经济学家合作，测试先进制造业多种方法的可行性。三个州的推广计划正在进行中，以教育公众有关固氮。拟议的合作研究项目的目标是发现和电化学N2还原的新分子催化剂的机理研究。在化学部化学催化计划的资助下，查佩尔山的北卡罗来纳州大学的米勒教授、罗格斯大学的戈德曼、费尔德和霍曼教授以及耶鲁大学的克拉布特里、霍兰德和迈耶教授正在开发能够通过直接N2裂解形成金属氮化物络合物来电催化NH3生产的催化剂。详细的研究提供机制的见解，指导新的钼和钼的配合物和电催化反应条件的设计。通过这种合作方法可获得的系统和方法的多样性正在被利用，以产生对过渡金属络合物的性质的广泛适用的见解，这些络合物有利于N2分裂和氮化物中间体的质子化，以在适合电催化的条件下产生NH3。该奖项反映了NSF的法定使命，并被认为值得通过使用基金会的智力价值和更广泛的评估来支持。影响审查标准。

项目成果

Synthesis and bonding analysis of pentagonal bipyramidal rhenium carboxamide oxo complexes

五角双锥铼甲酰胺氧配合物的合成及成键分析

• DOI: 10.1039/d3dt02617e
• 发表时间: 2023
• 期刊: Dalton Transactions
• 影响因子: 4
• 作者: McMillion, Noah D.;Bruch, Quinton J.;Chen, Chun-Hsing;Hasanayn, Faraj;Miller, Alexander J.
• 通讯作者: Miller, Alexander J.

Catalytic reduction of dinitrogen to ammonia using molybdenum porphyrin complexes

使用钼卟啉配合物催化还原二氮生成氨

• DOI: 10.1039/d2fd00166g
• 发表时间: 2023
• 期刊: Faraday Discussions
• 影响因子: 3.4
• 作者: Hegg, Alexander S.;Mercado, Brandon Q.;Miller, Alexander J. M.;Holland, Patrick L.
• 通讯作者: Holland, Patrick L.