MoS2 nanoparticles/MIL-100(Fe) heterojunction with Type II interfacial charge transfer for efficient photocatalytic nitrogen reduction

The attainment of rapid charge mobility and effective N 2 activation is of critical importance for photocatalytic nitrogen fixation but it has always been a challenge. Such challenge may be met by the construction of a Type II MoS 2 nanoparticles/ MIL-100(Fe) heterojunction photocatalyst. The new material possesses charge migration channels that facilitate the separation of photogenerated carriers. This charge redistribution during photocatalysis is confirmed by experimental results showing a decrease of charge density on the Fe species and an increase of that on Mo. Moreover, DFT calculations show that the adsorption of N 2 and H 2 O is more likely to occur on Fe sites and Mo sites, respectively. These findings clearly suggest a drastically improved spatial isolation of reduction and oxidation sites on the photocatalyst as compared to pristine MIL-100(Fe). The optimized MoS 2 /MIL-100(Fe) exhibits a NH 4 + yield rate of 1.29 μmol·h −1 as excellent utilization of photoinduced electron-hole pairs and effective adsorption and activation of N 2 become possible. This work offers an insight on the synergy of heterojunction engineering with coordinated activation for photocatalytic ammonia synthesis.