Abstract

The CO2 electroreduction (CO2RR) is extensively deemed as a promising route to reach carbon neutralization, while the single-atom catalysts (SACs) are proved to be effective in CO2RR. However, most SACs cannot further amplify performance due to their powdery feature. Herein, we present numerous isolated nickel single atoms anchored on 3D interconnected N-doped carbon tubes (NiSAs@3D-INCT) network as a self-supported electrode. The NiSAs@ 3D-INCT has truly interconnected and highly ordered vertical and lateral carbon tube-channels, which promote the CO2 interaction and electrolyte transmission. The NiSAs@3D-INCT exhibits a superior CO2RR performance with an appreciable CO partial current density of 51.8 mA cm −2 at − 0.96 V versus the reversible hydrogen electrode (RHE). X-ray absorption fine structure spectroscopy and theoretical computations reveal the NiSAs are loaded on the 3D-INCT network with Ni-N4 configuration as highly active sites for CO2RR. This work will shed a new light on opening up high performance SACs for CO2RR.

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