Details

Autor(en) / Beteiligte

• Rong, Xin
• Wang, Hong‐Juan
• Lu, Xiu‐Li
• Si, Rui
• Lu, Tong‐Bu

Titel

Controlled Synthesis of a Vacancy‐Defect Single‐Atom Catalyst for Boosting CO2 Electroreduction

Ist Teil von

• Angewandte Chemie International Edition, 2020-01, Vol.59 (5), p.1961-1965

Auflage

International ed. in English

Ort / Verlag

Weinheim: Wiley Subscription Services, Inc

Erscheinungsjahr

2020

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• The reaction of precursors containing both nitrogen and oxygen atoms with NiII under 500 °C can generate a N/O mixing coordinated Ni‐N3O single‐atom catalyst (SAC) in which the oxygen atom can be gradually removed under high temperature due to the weaker Ni−O interaction, resulting in a vacancy‐defect Ni‐N3‐V SAC at Ni site under 800 °C. For the reaction of NiII with the precursor simply containing nitrogen atoms, only a no‐vacancy‐defect Ni‐N4 SAC was obtained. Experimental and DFT calculations reveal that the presence of a vacancy‐defect in Ni‐N3‐V SAC can dramatically boost the electrocatalytic activity for CO2 reduction, with extremely high CO2 reduction current density of 65 mA cm−2 and high Faradaic efficiency over 90 % at −0.9 V vs. RHE, as well as a record high turnover frequency of 1.35×105 h−1, much higher than those of Ni‐N4 SAC, and being one of the best reported electrocatalysts for CO2‐to‐CO conversion to date. A vacancy defect was controllably constructed at the Ni site in a nickel single‐atom catalyst. It shows significantly enhanced electrocatalytic activity and selectivity for CO2‐to‐CO conversion compared with the Ni‐N4 catalyst.