Highly Efficient Electrocatalytic N<sub>2</sub> Reduction to Ammonia over Metallic 1T Phase of MoS<sub>2</sub> Enabled by Active Sites Separation Mechanism
Ruoqi Liu, Ting Guo, Hao Fei, Zhuangzhi Wu, Dezhi Wang, Fangyang Liu
Abstract
Abstract The 1T phase of MoS 2 has been widely reported to be highly active toward the hydrogen evolution reaction (HER), which is expected to restrict the competitive nitrogen reduction reaction (NRR). However, in this work, a prototype of active sites separation over 1T‐MoS 2 is proposed by DFT calculations that the Mo‐edge and S atoms on the basal plane exhibit different catalytic NRR and HER selectivity, and a new role‐playing synergistic mechanism is also well enabled for the multistep NRR, which is further experimentally confirmed. More importantly, a self‐sacrificial strategy using g‐C 3 N 4 as templates is proposed to synthesize 1T‐MoS 2 with an ultrahigh 1T content (75.44%, named as CNMS, representing the composition elements of C, N, Mo, and S), which yields excellent NRR performances with an ammonia formation rate of 71.07 µg h –1 mg –1 cat. at −0.5 V versus RHE and a Faradic efficiency of 21.01%. This work provides a promising new orientation of synchronizing the selectivity and activity for the multistep catalytic reactions.