CAS: Collaborative Research: Physics-Informed Machine Learning for Electrochemical C-N Coupling by Metal-Organic Materials

With the support of the Chemical Catalysis program in the Division of Chemistry, Professor V. Sara Thoi of Johns Hopkins University and Professor Fanglin Che of University of Massachusetts, Lowell are studying the design of catalytic materials for electrochemical synthesis of organonitrogen compounds. Organonitrogen species are a ubiquitous class of compounds used in a variety of industries, from agriculture to pharmaceuticals. Urea, for instance, is an important fertilizer, but it is industrially derived from a highly energy-intensive process called the Haber-Bosch process. Electrochemical transformation of abundant carbon and nitrogen molecules, such as carbon dioxide and nitrogen gas, to organonitrogen products thus emerges as an attractive approach. Electrochemical synthesis can be conducted at room temperature, ambient pressure, and in water. Moreover, the rise in renewably generated electricity provides a path towards decarbonization of the chemical manufacturing industry. This project uses a combination of computational and experimental chemistry to design, synthesize, and test new catalysts for forming commercially valuable organonitrogen compounds, such as urea, acetamide, and N-methylamines. The expected outcomes are the fundamental knowledge for activating small molecules to form carbon-nitrogen bonds, the identification of design parameters for synthesizing efficient catalysts, and the broader applications of electrochemical synthesis to a new class of commodity chemicals. Additionally, the educational goal of this project is to engage young students in the STEM field via the publicly accessible video series, “Meet the Chemist,” which highlights the unique and diverse paths of undergraduate students to chemical research. Moreover, a novel theory course on applied machine learning for computational catalysis will be developed for undergraduate and graduate students. The scientific and educational merits of this project advance the frontiers of chemical synthesis, promote public engagement between researchers and young students, and align with our national interest for decarbonization. With the support of the Chemical Catalysis program in the Division of Chemistry, Professor V. Sara Thoi of Johns Hopkins University and Professor Fanglin Che of University of Massachusetts, Lowell are studying the design of catalytic materials for electrochemical synthesis of organonitrogen compounds. This project will focus on a class of metal-organic materials called boron imidazolate frameworks (BIFs) for electrochemical C-N coupling to form commercially valuable products, such as urea, acetamide, and N-methylamines. Owing to their synthetic tunability, BIFs provide facile access to a range of isostructural metal-organic materials to identify structure-function relationships, serving as an ideal materials platform for fundamental insights to catalytic mechanisms. This project has three objectives: i) identify the structure-function relationships between the electronics of the BIFs and C-N coupling, ii) observe key intermediates via in situ vibrational spectroscopy, and iii) develop physics-informed machine learning to identify design criteria for new BIF catalysts. Together, this knowledge will be used to explore the scope of C-N coupling products, using inexpensive and abundant carbon and nitrogen precursors such as carbon dioxide, aldehyde, ketones, dinitrogen, nitrite, nitrates, and amines. Additionally, we will expand an existing video series, called “Meet the Chemist,” to highlight the unique and diverse paths of undergraduate students to chemical research. The videos, which are publicly available, are designed to encourage young students to learn that people of all backgrounds can engage in STEM research. Moreover, a novel theory course on applied machine learning for computational catalysis will be developed for undergraduate and graduate students. Along with these broader outreach goals, this project aims to enhance the utility of electrochemical synthesis for a wide range of industrially relevant compounds, thereby creating opportunities to decarbonize the chemical industry. 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.