| Author: | Ding, Keda |
| Title: | Atomic-scale engineering and mechanistic insights into next-generation electrocatalysts : a computational perspective |
| Advisors: | Yang, Ming (AP) Huang, Haitao (AP) |
| Degree: | Ph.D. |
| Year: | 2026 |
| Department: | Department of Applied Physics |
| Pages: | iv, 159 pages : color illustrations |
| Language: | English |
| Abstract: | This work systematically investigates the electronic structure and catalytic performance of advanced electrocatalyst systems across three representative platforms: curved and vacancy-engineered MoS₂ for the hydrogen evolution reaction (HER), heteronuclear Fe-Co single-atom catalysts (SACs) for the oxygen reduction reaction (ORR), and geminal Cu atom-doped polymeric carbon nitride (Cu/PCN) for CO reduction reaction (CORR). Through in-depth first-principles calculations, we reveal that engineering curvature and sulfur vacancies in MoS₂ narrows the band gap and optimizes the density of states near the Fermi level, which significantly enhancing HER activity. For Fe-Co SACs on 4-fold nitrogen embedded on graphene (FeN₄-C and CoN₄-C), our study illustrates the importance of the loading effect in heteronuclear SACs; and identify the best ORR performance around 16.8% wt. In the case of Cu/PCN, detailed electronic and thermodynamic analyses uncover the mechanisms underlying C₁ (methanol) versus C₂ (ethylene glycol) product selectivity; high concentrations of geminal Cu and CO availability favoring ethylene glycol formation. These findings reveal the atomic-scale engineering and mechanistic insights for the next-generation electrocatalysts. |
| Rights: | All rights reserved |
| Access: | open access |
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