608
Views
29
Crossref
29
WoS
26
Scopus
1
CSCD
Electrochemical reduction of nitrogen to ammonia under mild conditions provides an intriguing approach for energy conversion. A grand challenge for electrochemical nitrogen reduction reaction (NRR) is to design a superior electrocatalyst to obtain high performance including high catalytic activity and selectivity. In the NRR process, the three most important steps are nitrogen adsorption, nitrogen activation, and ammonia desorption. We take MoS2 as the research object and obtain catalysts with different electronic densities of states through the doping of Fe and V, respectively. Using a combination of experiments and theoretical calculations, it is demonstrated that V-doped MoS2 (MoS2-V) shows better nitrogen adsorption and activation, while Fe-doped MoS2 (MoS2-Fe) obtains the highest ammonia yield in experiments (20.11 µg·h-1·mgcat–1.) due to its easier desorption of ammonia. Therefore, an appropriate balance between nitrogen adsorption, nitrogen activation, and ammonia desorption should be achieved to obtain highly efficient NRR electrocatalysts.
This work was financially supported by the Beijing Municipal High Level Innovative Team Building Program (No. IDHT20180504), Beijing Outstanding Young Scientists Program (No. BJJWZYJH01201910005017), the National Natural Science Foundation of China (Nos. 51801006, 21805004, 21671011, and 21872001), Beijing Natural Science Foundation (Nos. KZ201710005002 and 2192005), Beijing Municipal Science and Natural Science Fund Project (No. KM201910005016), China Postdoctoral Science Foundation (No. 2018M641133), Beijing Postdoctoral Research Foundation (No. 2018-ZZ-021) and Chaoyang District Postdoctoral Research Foundation (No. 2018-ZZ-026). These funding agencies are acknowledged.