Sulfur vacancies-doped Sb2S3 nanorods as high-efficient electrocatalysts for dinitrogen fixation under ambient conditions

Tuning surface electron transfer process by sulfur (S)-vacancies engineering is an efficient strategy to develop high-efficient catalysts for electroreduction N-2 reaction (NRR). Herein, the distinct Sb2S3 nanorods with S-vacancies (S-v-Sb2S3) have been synthesized by a simple two-step method including hydrothermal and hydrogenation in H-2/Ar atmosphere, which shows improved performance for NRR with the NH3 yield rate of 10.85 mu g h(-1) mg(cat)(-1) at -0.4 V vs. RHE, the faradaic efficiency (FE) of 3.75% at -0.3 V vs. RHE and excellent stability for 24 h, largely outperforming bulk Sb2S3. X-ray photoelectron spectroscopy (XPS) and density function theory (DFT) calculations demonstrate that the abundant S-vacancies can create an electron-deficient environment and modulate the electron delocalization in S-v-Sb2S3, which can not only facilitate the N-2 molecule adsorption, but also activate the N N resulting in the enhanced performance for NRR. (C) 2020 Institute of Process Engineering, Chinese Academy of Sciences. Publishing services by Elsevier B.V. on behalf of KeAi Communications Co., Ltd.