T. N. Nguyen, S. Kampouri, B. Valizadeh, W. Luo, D. Ongari, O. M. Planes, A. Zuttel, B. Smit, and K. C. Stylianou, Photocatalytic Hydrogen Generation from a Visible-light Responsive Metal-organic Framework System: Stability versus Activity of Molybdenum Sulfide Co-catalysts ACS Appl Mater Interfaces 10 (36), 30035 (2018) doi: 10.1021/acsami.8b10010
Abstract: We report the use of two earth abundant molybdenum sulfide-based co-catalysts, Mo3S132- clusters and 1T-MoS2 nanoparticles (NPs), in combination with the visible-light active metal-organic framework (MOF) MIL-125-NH2 for the photocatalytic generation of hydrogen (H2) from water splitting. Upon irradiation (λ ≥ 420 nm), the best-performing mixtures of Mo3S132-/MIL-125-NH2 and 1T-MoS2/MIL-125-NH2 exhibit high catalytic activity, producing H2 with evolution rates of 2094 and 1454 µmol h-1 g-1MOF and apparent quantum yields of 11.0 and 5.8 % at 450 nm, respectively, which are among the highest values reported to date for visible-light-driven photocatalysis with MOFs. The high performance of Mo3S132-can be attributed to the good contact between these clusters and the MOF and the large number of catalytically active sites, whilst the high activity of 1T-MoS2 NPs is due to their high electrical conductivity leading to fast electron transfer processes. Recycling experiments revealed that although the Mo3S132-/MIL-125-NH2 slowly loses its activity, the 1T-MoS2/MIL-125-NH2 retains its activity for at least 72 hours. This work indicates that earth-abundant compounds can be stable and highly catalytically active for photocatalytic water splitting, and should be considered as promising co-catalysts with new MOFs besides the traditional noble metal NPs.
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