Boosted Electrocatalytic N2 Reduction to NH3 by Defect-Rich MoS2 Nanoflower
Advanced Energy Materials, Volume 8, No. 30, Article 1801357, Year 2018
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The industrial artificial fixation of atmospheric N2 to NH3 is carried out using the Haber–Bosch process that is not only energy-intensive but emits large amounts of greenhouse gas. Electrochemical reduction offers an environmentally benign and sustainable alternative for NH3 synthesis. Although Mo-dependent nitrogenases and molecular complexes effectively catalyze the N2 fixation at ambient conditions, the development of a Mo-based nanocatalyst for highly performance electrochemical N2 fixation still remains a key challenge. Here, greatly boosted electrocatalytic N2 reduction to NH3 with excellent selectivity by defect-rich MoS2 nanoflowers is reported. In 0.1 m Na2SO4, this catalyst attains a high Faradic efficiency of 8.34% and a high NH3 yield of 29.28 µg h−1 mg−1cat. at −0.40 V versus reversible hydrogen electrode, much larger than those of defect-free counterpart (2.18% and 13.41 µg h−1 mg−1cat.), with strong electrochemical stability. Density functional theory calculations show that the potential determining step has a lower energy barrier (0.60 eV) for defect-rich catalyst than that of defect-free one (0.68 eV).