Collaborative Research: INFEWS N/P/H2O: Electrochemical Approaches to Sustainable Dinitrogen Fixation

在这个由化学部化学催化项目资助的项目中，来自北卡罗来纳大学教堂山分校（UNC）、耶鲁大学和罗格斯大学的科学家们正在合作开发可持续的电化学固定氮（N2）的方法。可持续固氮是食品、能源和水化学领域挑战的核心。目前的全球粮食生产是通过使用合成肥料来实现的，这种合成肥料是通过固氮过程产生的，从氮和氢（H2）中产生氨（NH3），但对能源和环境造成了巨大的负面影响，消耗了约2%的世界？美国的化石燃料衍生能源供应。在这个项目中，Alexander Miller教授（UNC），詹姆斯·梅耶和帕特里克·霍兰德（耶鲁大学），教授。来自罗格斯大学的Alan Goldman和Gal Hochman正在探索新的、可持续的固氮方法。新的化学将被开发出来，使电化学固氮过程的发展不需要消耗化石燃料来产生氨和硝酸盐。可持续性和政策分析将评估对全球农业和能源部门的变革性影响的潜力（包括考虑将氨作为可能的液体运输燃料）。该项目将培养研究生和博士后研究人员在跨学科的问题为基础的科学方法和积极影响的机构基础设施。该主题和研究结果将被用作一个平台，向非科学家讲授化学催化在工业、农业和现代社会中的重要性。跨学科研究团队在催化剂设计与合成、电催化、机理研究、可持续发展与政策分析等方面具有优势。化学固定N2的方法包括过渡金属电催化N2还原分裂成氮中间体。这些氮化物中间体可以通过质子耦合电子转移（PCET）将氮化物还原为NH3，或者(b)氮化物氧化成硝酸。稳健性和可调钳形配体的中晚期过渡金属配合物将是一个实验重点，并辅以计算研究，以将反应性与分子性质联系起来，并指导催化剂的开发。本文将分析潜在的电化学固氮过程的成本，以估计对一系列因素的依赖，如电力来源的多样性、可持续能源的间歇性和政府政策。

In this project funded by the Chemical Catalysis Program of the Chemistry Division, scientists from the University of North Carolina at Chapel Hill (UNC), Yale University, and Rutgers University are collaborating to develop approaches to sustainable electrochemical fixation of nitrogen (N2). Sustainable nitrogen fixation is central to the nexus of challenges in food, energy, and water chemistry. Current global food production is enabled by the use of synthetic fertilizer that is produced by nitrogen fixation processes that generate ammonia (NH3) from nitrogen and hydrogen (H2), but leave a dramatic negative impact on energy and the environment, consuming about 2% of the world?s fossil fuel-derived energy supply. In this project, Prof. Alexander Miller (UNC), Profs. James Mayer and Patrick Holland (Yale), and Profs. Alan Goldman and Gal Hochman (Rutgers) are exploring new, sustainable methods for nitrogen fixation. New chemistry will be developed that could enable the development of electrochemical nitrogen fixation processes that do not require consumption of fossil fuels to produce ammonia and nitrates. Sustainability and policy analysis will assess the potential for transformative impact on global agriculture and energy sectors (including consideration of ammonia as a possible liquid transportation fuel). The project will train graduate students and postdoctoral researchers in interdisciplinary problem-based scientific methods and positively impact institutional infrastructure. The topic and the results of the research will be used as a platform to teach non-scientists about the importance of chemical catalysis in industry, agriculture, and modern society in general. The interdisciplinary research team has strengths in catalyst design and synthesis, electrocatalysis, mechanistic studies, and sustainability and policy analysis. The chemical approach to N2 fixation involves transition-metal-electrocatalyzed reductive splitting of N2 into nitrido intermediates. These nitrido intermediates can undergo (a) nitride reduction to NH3 by proton-coupled electron transfer (PCET), or (b) nitride oxidation toward nitric acid. Middle-to-late transition metal complexes of robust and tunable pincer ligands will be an experimental focus, with complementary computational studies to correlate reactivity with molecular properties and guide catalyst development. The cost of potential electrochemical N2 fixation processes will be analyzed, to estimate the dependence on a range of factors such as diversity of electricity sources, intermittency of sustainable energy, and governmental policy.