Open AccessHighly Efficient Electrocatalytic N 2 Reduction to Ammonia over Metallic 1T Phase of MoS 2 Enabled by Active Sites Separation Mechanism
Author(s) -
Liu Ruoqi,
Guo Ting,
Fei Hao,
Wu Zhuangzhi,
Wang Dezhi,
Liu Fangyang
Publication year - 2022
Publication title -
advanced science
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.388
H-Index - 100
ISSN - 2198-3844
DOI - 10.1002/advs.202103583
Subject(s) - selectivity , catalysis , ammonia , ammonia production , phase (matter) , metal , redox , electrocatalyst , chemistry , synchronizing , materials science , hydrogen , inorganic chemistry , chemical engineering , electrochemistry , electrode , topology (electrical circuits) , organic chemistry , mathematics , combinatorics , engineering
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.