Electrode

Organic chemistry

Ring (chemistry)

Oxygen atom

Atom (system on chip)

Crystallography

Vacancy defect

Faraday efficiency

Catalysis

Physical chemistry

Embedded system

Chemistry

Materials science

Molecule

Computer science

Nitrogen atom

Electrochemistry

Nitrogen

Oxygen

Angewandte Chemie International Edition

The reaction of precursors containing both nitrogen and oxygen atoms with NiII under 500 °C can generate a N/O mixing coordinated Ni-N3 O 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.

Controlled Synthesis of a Vacancy‐Defect Single‐Atom Catalyst for Boosting CO<sub>2</sub> Electroreduction

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

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