Molybdenum Sulfide within a Metal–Organic Framework for Photocatalytic Hydrogen Evolution from Water

Noh, Hyunho; Yang, Ying; Ahn, Sol; Peters, Aaron W.; Farha, Omar K.; Hupp, Joseph T.

doi:10.1149/2.0261905jes

Title: Molybdenum Sulfide within a Metal–Organic Framework for Photocatalytic Hydrogen Evolution from Water

Journal Article · Thu Jan 24 00:00:00 EST 2019 · Journal of the Electrochemical Society

DOI:https://doi.org/10.1149/2.0261905jes· OSTI ID:1491951

; Yang, Ying; Ahn, Sol; Peters, Aaron W.; Farha, Omar K.;

A representative metal–organic framework, NU-1000, was functionalized with MoS_x. The previously determined crystal structure of the material, named MoS_x-SIM, consists of monometallic Mo(IV) ions with two sulfhydryl ligands. The metal ions are anchored to the framework by displacing protons presented by the –OH/–OH₂ groups on the Zr₆ node. As shown previously, the MOF-supported complexes are electrocatalytic for hydrogen evolution from acidified water. The earlier electrocatalysis results, together with the nearly ideal formal potential of the Mo(IV/II) couple (i.e., nearly coincident with that of the hydrogen couple), and the physical proximity of UV-absorbing MOF linkers to the complexes, suggested to us that the linkers might behave photosensitizers for catalyst reduction, and subsequently, for H₂ evolution from water. To our surprise, MoS_x-SIM, when UV-illuminated in an aqueous buffer at near-neutral pH, displays a biphasic photocatalytic response: an initially slow rate of reaction, i.e. 0.56 mmol g^-1 h^-1, followed by an increase to 4 mmol g^-1 h^-1. Ex-situ catalyst examination revealed that nanoparticulate MoSx suspended within the reaction mixture is the actual catalyst. Thus, photo-assisted restructuring and detachment of the catalyst or pre-catalyst from the MOF node appears to be necessary for the catalyst to reduce water at neutral pH.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Light Energy Activated Redox Processes (LEAP); Northwestern Univ., Evanston, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001059

OSTI ID:: 1491951

Alternate ID(s):: OSTI ID: 1566728

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Vol. 166 Journal Issue: 5; ISSN 0013-4651

Publisher:: The Electrochemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 14 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: Molybdenum Sulfide within a Metal–Organic Framework for Photocatalytic Hydrogen Evolution from Water

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