Details

Autor(en) / Beteiligte

• Huang, Senhe
• Tranca, Diana
• Rodríguez-Hernández, Fermin
• Zhang, Jichao
• Lu, Chenbao
• Zhu, Jinhui
• Liang, Hai-Wei
• Zhuang, Xiaodong

Titel

Well-defined N3 C1 -anchored Single-Metal-Sites for Oxygen Reduction Reaction

Ist Teil von

• Angewandte Chemie (International ed.), 2024-01, Vol.63 (1), p.e202314833-e202314833

Erscheinungsjahr

2024

Link zum Volltext

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• N-, C-, O-, S-coordinated single-metal-sites (SMSs) have garnered significant attention due to the potential for significantly enhanced catalytic capabilities resulting from charge redistribution. However, significant challenges persist in the precise design of well-defined such SMSs, and the fundamental comprehension has long been impeded in case-by-case reports using carbon materials as investigation targets. In this work, the well-defined molecular catalysts with N3 C1 -anchored SMSs, i.e., N-confused metalloporphyrins (NCPor-Ms), are calculated for their catalytic oxygen reduction activity. Then, NCPor-Ms with corresponding N4 -anchored SMSs (metalloporphyrins, Por-Ms), are synthesized for catalytic activity evaluation. Among all, NCPor-Co reaches the top in established volcano plots. NCPor-Co also shows the highest half-wave potential of 0.83 V vs. RHE, which is much better than that of Por-Co (0.77 V vs. RHE). Electron-rich, low band gap and regulated d-band center contribute to the high activity of NCPor-Co. This study delves into the examination of well-defined asymmetric SMS molecular catalysts, encompassing both theoretical and experimental facets. It serves as a pioneering step towards enhancing the fundamental comprehension and facilitating the development of high-performance asymmetric SMS catalysts.