摘要
Electrocatalytic nitrogen reduction reaction(NRR)is a sustainable approach for NH_(3)production with low energy consumption.However,competing hydrogen reduction reaction(HER)in aqueous solution results in low NH_(3)production and Faraday efficiency(FE).Here,MoS_(2)nanostructures with a hydrophobic surface are synthesized by alkyl thiols modification.Aerophilic and hydrophobic surface facilitates an efficient three-phase contact of N_(2),H_(2)O,and catalyst.Thus,localized concentrated N_(2)molecules can overcome the mass transfer limitation of N2 and depress the HER due to lowering the proton contacts.Although the active-sites decrease with the increase of the alkyl chain since the thiol may cover the active site,the optimized electrocatalyst achieves NH_(3)yield of 12.86×10^(-11)mol·cm^(-2)·s^(-1)at-0.25 V and 22.23%FE,which are 4.3 and 24 times higher than those of MoS2-CP electrocatalyst,respectively.The increased catalytic performance is attributed to the high N_(2)adsorption and depressed HER.
基金
We acknowledge financial support from the Beijing Municipal High Level Innovative Team Building Program(No.IDHT20180504)
Beijing Outstanding Young Scientist Program(No.BJJWZYJH01201910005017)
the National Natural Science Foundation of China(Nos.51801006,21805004,21872001,and 21936001)
Beijing Natural Science Foundation(No.2192005)
Beijing Municipal Science and Natural Science Fund Project(Nos.KM201910005016 and 2017000020124G085).