Computationally Accelerated Discovery of Catalysts for Electrification of the Nitrogen Cycle

在化学系化学催化项目的支持下，科罗拉多大学博尔德分校的Charles Musgrave教授和他的团队将使用计算量子化学方法和机器学习来发现无碳肥料合成的新电催化剂。向无碳肥料生产的重大转变可能即将到来，这将使人们能够使用可持续的过程来养活未来的世界人口。马斯格雷夫和他的研究小组旨在通过可再生能源驱动的碳中性电化学过程，专注于氨和硝酸铵（肥料的关键成分）的合成，从而加速这一转变。通过利用尖端的量子化学计算方法，马斯格雷夫旨在加速新型电催化剂的发现和设计，这对彻底改变肥料生产至关重要。值得注意的是，这种方法不仅旨在提高肥料合成，而且还旨在降低硝酸盐水平，解决全球水生系统中水污染的紧迫问题。通过对成千上万种候选催化剂材料的细致探索，马斯格雷夫研究小组旨在发现控制电催化剂性能的关键原理。这项研究有可能影响广泛的电催化过程，并将有助于在日益重要的电催化领域教育未来的劳动力。该项目的中心目标是利用可再生能源加速电催化碳中性合成氨和硝酸铵，特别侧重于打破长期限制电催化氮还原、硝酸盐还原和氮氧化反应的结垢关系。为了做到这一点，该项目将利用大正则密度泛函理论方法，提供电气化界面的量子力学描述。之所以选择这种方法，是因为它能够基本而准确地描述电催化剂界面上发生的电化学过程，以及这些过程如何随着施加的偏压而变化。这些研究有可能使人们对电催化的复杂过程有更深入的了解。通过深入研究电催化剂的电子结构及其对应用电位的响应，本研究旨在揭示反应能量学，相对动力学以及独特材料打破结垢关系的潜力的关键见解。项目范围涵盖了二进制和Chevrel化学空间内的各种材料，目的是促进预测各种成分和潜力的活动趋势。这种综合的方法不仅旨在阐明不同反应和材料空间的标度原理的可转移性，而且还为其他电催化化学的发展提供信息。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。

With support from the Chemical Catalysis Program in the Division of Chemistry, Professor Charles Musgrave and his team at the University of Colorado-Boulder will use computational quantum chemical methods and machine learning to discover new electrocatalysts for carbon-free fertilizer synthesis. A significant shift to carbon-free fertilizer production could be on the horizon that would enable feeding the future population of the world using sustainable processes. Musgrave and his research group aims to accelerate this transformation by focusing on the synthesis of ammonia and ammonium nitrate, crucial components of fertilizers, through carbon-neutral electrochemical processes driven by renewable energy. By leveraging cutting-edge quantum chemical computational methods, Musgrave aims to accelerate the discovery and design of novel electrocatalysts that are essential for revolutionizing fertilizer production. Notably, this approach not only aims to enhance fertilizer synthesis but also to reduce nitrate levels, addressing the pressing issue of water contamination in global aquatic systems. Through the meticulous exploration of tens of thousands of candidate catalyst materials, the Musgrave research group aims to discover the key principles that govern the performance of electrocatalysts. This research has the potential to impact a wide array of electrocatalytic processes and will help in educating the future workforce in the increasingly important area of electrocatalysis. The central goal of this project is to accelerate the electrocatalytic carbon-neutral synthesis of ammonia and ammonium nitrate using renewable energy, with a particular focus on breaking the scaling relations that have long constrained electrocatalytic nitrogen reduction, nitrate reduction, and nitrogen oxidation reactions. To do this, the project will utilize grand canonical density functional theory methods that provide a quantum mechanical description of the electrified interface. This approach was chosen because it enables a fundamental and accurate description of electrochemical processes that occur at the electrocatalyst interface and how these processes change with the applied bias. These studies have the potential to enable a deeper understanding of the intricate processes underlying electrocatalysis. By delving into the electronic structure of electrocatalysts and their response to the applied potential, this research aims to uncover key insights into reaction energetics, relative kinetics, and the potential of unique materials to break scaling relations. The project scope encompasses a diverse range of materials within the binary and Chevrel chemical spaces, with the aim of facilitating the prediction of activity trends across various compositions and potentials. This comprehensive approach is intended to not only shed light on the transferability of scaling principles across different reactions and materials spaces, but also to inform the development of other electrocatalytic chemistries.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.