Electrocatalytic CO reduction reaction (CO RR) offers a promising strategy to lower CO emission while producing value-added chemicals. A great challenge facing CO RR is how to improve energy efficiency by reducing overpotentials. Herein, partially nitrided Ni nanoclusters (NiN ) immobilized on N-doped carbon nanotubes (NCNT) for CO RR are reported, which achieves the lowest onset overpotential of 16 mV for CO -to-CO and the highest cathode energy efficiency of 86.9% with CO Faraday efficiency >99.0% to date. Interestingly, NiN /NCNT affords a CO generation rate of 43.0 mol g h at a low potential of -0.572 V (vs RHE). DFT calculations reveal that the NiN nanoclusters favor *COOH formation with lower Gibbs free energy than isolated Ni single-atom, hence lowering CO RR overpotential. As NiN /NCNT is applied to a membrane electrode assembly system coupled with oxygen evolution reaction, a cell voltage of only 2.13 V is required to reach 100 mA cm , with total energy efficiency of 62.2%.
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