Sulfur vacancies-doped Sb2S3 nanorods as high-efficient electrocatalysts for dinitrogen fixation under ambient conditions
Xuyan Wang, Jianwei Bai, Yantao Wang, Xiaoying Lü, Zehua Zou, Junfeng Huang, Cailing Xu
Abstract
Tuning surface electron transfer process by sulfur (S)-vacancies engineering is an efficient strategy to develop high-efficient catalysts for electroreduction N2 reaction (NRR). Herein, the distinct Sb2S3 nanorods with S-vacancies (Sv-Sb2S3) have been synthesized by a simple two-step method including hydrothermal and hydrogenation in H2/Ar atmosphere, which shows improved performance for NRR with the NH3 yield rate of 10.85 μg h−1 mgcat−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 Sv-Sb2S3, which can not only facilitate the N2 molecule adsorption, but also activate the NN, resulting in the enhanced performance for NRR.