Semi‐metal 1T′ phase MoS2 nanosheets for promoted electrocatalytic nitrogen reduction

• Published in: EcoMat (Beijing, China) China), 2021-08, Vol.3 (4), p.n/a
• Main Authors: Xu, Xuesong, Wang, Yian, Chen, Xiaoyue, Qian, Xiu, Liang, Zhangqian, Cui, Hongzhi, Tian, Jian, Shao, Minhua
• Format: Article
• Language: English
• Subjects: Ammonia; Chemical reduction; Efficiency; Electrocatalysts; electrocatalytic nitrogen reduction; Electrolytes; Etching; Isotopic labeling; Metals; Molybdenum disulfide; MoS2; Nanoparticles; Nanosheets; Nanospheres; Nitrogen; semi‐metal 1T′ phase; Substrates; TiO2 hollow nanosphere; Titanium dioxide; urchin‐like
• ISSN: 2567-3173; 2567-3173
• DOI: 10.1002/eom2.12122

Herein, we constructed urchin‐like TiO2 hollow nanospheres (HNSs) by hydrothermal targeted etching, and used it as a substrate to load semi‐metal 1T′‐MoS2 nanosheets as effective nitrogen reduction reaction (NRR) electrocatalysts. 1T′‐MoS2/TiO2 HNSs composites display outstanding NRR activity with the highest NH3 yield of 29.62 μg h−1 mg−1cat. at −0.75 V versus RHE. Besides, the highest FE of 24.9% is obtained at −0.65 V. The remarkable NRR performance is attributed to the high conductivity of 1T′‐MoS2 and the urchin‐like structure of TiO2 hollow nanospheres. DFT calculations display that the 1T′‐MoS2 in 1T′‐MoS2/TiO2 makes the activation and further reduction of *N2 more thermodynamically favorable than pristine TiO2, contributing to better NRR catalytic activities. 15N isotopic labeling experiment reveals that N in produced NH3 comes from N2 of electrolyte. We report that 1T′‐MoS2 nanosheets loaded on urchin‐like TiO2 hollow nanospheres can achieve effectively the electrochemical conversion of N2 to NH3. In 0.1 M Na2SO4, the catalyst exhibits excellent NRR electrocatalytic performance with the highest NH3 yield of 29.62 μg h−1 mg−1cat. at −0.75 V versus RHE and the highest FE of 24.9% is achieved at −0.65 V versus RHE.