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

Abstract 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.