Enhancing Oxygen Reduction Reaction Electrocatalytic Performance of Nickel-Nitrogen-Carbon Catalysts through Coordination Environment Engineering
Hui-Jian Zou , Yan Leng , Chen-Shuang Yin , Xikun Yang , Chun-Gang Min , Feng Tan , Ai-Min Ren
Chinese Journal of Chemistry ›› 2025, Vol. 43 ›› Issue (3) : 297 -307.
Enhancing Oxygen Reduction Reaction Electrocatalytic Performance of Nickel-Nitrogen-Carbon Catalysts through Coordination Environment Engineering
Single-atom catalysts (SACs) have attracted significant attention due to their high atomic utilization and tunable coordination environment. However, the catalytic mechanisms related to the active center and coordination environment remain unclear. In this study, we systematically investigated the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) catalytic activities of NiN 4, NiN 3, NiN 3H 2, NiN 4X, NiN 3X, and NiN 3H 2X (X denotes axial ligand) through density functional theory (DFT) calculations. This study unveils two distinct reaction pathways for ORR and OER, involving proton-electron pairs adsorbed from both the solution and the catalyst surface. The overpotential is the key parameter to evaluate the catalytic performance when proton-electron pairs are adsorbed from the solution. NiN 3 and NiN 3H 2 show promise as pH-universal bifunctional electrocatalysts for both ORR and OER. On the other hand, when proton-electron pairs are adsorbed from the catalyst surface, the reaction energy barrier becomes the crucial metric for assessing catalytic activity. Our investigation reveals that NiN 3H 2 consistently exhibits optimal ORR activity across a wide pH range, regardless of the source of proton-electron pair (solvent or catalyst surface).
Nickel-nitrogen-carbon / Axial ligands / N-defect / First-principles / Oxygen evolution reaction / Oxygen reduction reaction / Local coordination environment / Electrocatalysis
2024 SIOC, CAS, Shanghai, & WILEY-VCH GmbH
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