Nitrogen Reduction Reaction: Heteronuclear Double‐Atom Electrocatalysts

Autor: Yuanzhe Wang, Jing Wang, Heen Li, Yaguang Li, Junkai Li, Kuo Wei, Fei Peng, Faming Gao
Jazyk: angličtina
Rok vydání: 2023
Předmět:
Zdroj: Small Structures, Vol 4, Iss 4, Pp n/a-n/a (2023)
Druh dokumentu: article
ISSN: 2688-4062
20220030
DOI: 10.1002/sstr.202200306
Popis: Heteronuclear dual‐site catalysts (HDACs), inspired from single‐atom catalyst, have been proposed as advanced alternatives of noble metal catalyst, especially toward nitrogen reduction reaction (NRR). However, the search for favorable candidates with both promising NH3 yield and noble Faradaic efficiency is still challenging, due to limited experimentally available bi‐metal pairs and lack of thorough understanding of the design criteria. Herein, by theoretical screening of a family of M/Fe combinations (M = Sc, Ti, V, Cr, Mn, Co, and Ni), atomically dispersed binary V/Fe architecture anchored on nitrogen‐doped carbon matrix (VFe/NC) is proposed with a small limiting potential (0.39 V) and high selectivity over the hydrogen evolution reaction (HER). Owing to a perfect matching with N2 antibonding state, V 3dz2 orbitals, “push” electrons into adsorbed N2 antibonding stats and simultaneously Fe 3dyz “pull” extra electrons back. Benefiting from the synergistic effect from the dual‐active sites, an outstanding NH3 yield of 73.44 μg h−1 mgcat−1 (8070.32 μg h−1 mgVFe−1) and an excellent Faradaic efficiency of 43% are achieved, overwhelming literature‐reported atomic‐level catalysts. This study promotes the development of HDACs that are capable of high yield rate accompanied with high Faradaic efficiency.
Databáze: Directory of Open Access Journals
Externí odkaz: