Engineering topics

Yu, Saerom

Publications and source records attributed to Yu, Saerom.

3 records

DOE OSTI2024

General synthesis of high-entropy single-atom nanocages for electrosynthesis of ammonia from nitrate

Given the growing emphasis on energy efficiency, environmental sustainability, and agricultural demand, there’s a pressing need for decentralized and scalable ammonia production. Converting nitrate ions electrochemically, which are commonly found in industrial wastewater and polluted groundwater, into ammonia offers a viable approach for both wastewater treatment and ammonia production yet limited by low producibility and scalability. Here we report a versatile and scalable solution-phase synthesis of high-entropy single-atom nanocages (HESA NCs) in which Fe and other five metals-Co, Cu, Zn, Cd, and In-are isolated via cyano-bridges and coordinated with C and N, respectively. Incorporating and isolating the five metals into the matrix of Fe resulted in Fe-C5 active sites with a minimized symmetry of lattice as well as facilitated water dissociation and thus hydrogenation process. As a result, the Fe-HESA NCs exhibited a high selectivity toward NH3 from the electrocatalytic reduction of nitrate with a Faradaic efficiency of 93.4% while maintaining a high yield rate of 81.4 m h -1 mg -1 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Emerging Atomistic Modeling Methods for Heterogeneous Electrocatalysis

Heterogeneous electrocatalysis lies at the center of various technologies that could help enable a sustainable future. However, its complexity makes it challenging to accurately and efficiently model at an atomic level. Herein, we review emerging atomistic methods to simulate the electrocatalytic interface with special attention devoted to the components/effects that have been challenging to model, such as solvation, electrolyte ions, electrode potential, reaction kinetics, and pH. Additionally, we review relevant computational spectroscopy methods. Then, we showcase several examples of applying these methods to understand and design catalysts relevant to green hydrogen. We also offer experimental views on how to bridge the gap between theory and experiments. Finally, we provide some perspectives on opportunities to advance the field.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Highly Selective Oxygen Reduction to Hydrogen Peroxide on a Carbon-Supported Single-Atom Pd Electrocatalyst

Selective electrochemical two-electron oxygen reduction is a promising route for renewable and on-site H 2 O 2 generation as an alternative to the anthraquinone process. In this study, we report a high-performance nitrogen-coordinated single-atom Pd electrocatalyst, which is derived from Pd-doped zeolitic imidazolate frameworks (ZIFs) through one-step thermolysis. High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) combined with X-ray absorption spectroscopy verifies atomically dispersed Pd atoms on nitrogen-doped carbon (Pd-NC). The single-atom Pd-NC catalyst exhibits excellent electrocatalytic performance for two-electron oxygen reduction to H 2 O 2 , which shows ~95% selectivity toward H 2 O 2 and an unprecedented onset potential of ~0.8 V versus revisable hydrogen electrode (RHE) in 0.1 M KOH. Density functional theory (DFT) calculations demonstrate that the Pd-N 4 catalytic sites thermodynamically prefer *–O bond breaking to O–O bond breaking, corresponding to a high selectivity for H 2 O 2 production. This work provides a deep insight into the understanding of the catalytic process and design of high-performance 2e– ORR catalysts.

36 MATERIALS SCIENCE↗