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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 MoS2 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 H2O 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 MoS2/MIL-100(Fe) exhibits a NH4+ yield rate of 1.29 mu molh(-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.
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JOURNAL OF CATALYSIS
ISSN: 0021-9517
Year: 2025
Volume: 451
6 . 5 0 0
JCR@2023
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ESI Highly Cited Papers on the List: 0 Unfold All
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30 Days PV: 0