Photoexcitation of Fe 3 O Nodes in MOF Drives Water Oxidation at pH=1 When Ru Catalyst Is Present

Ezhov, Roman; Ravari, Alireza K.; Palenik, Mark; Loomis, Alexander; Meira, Debora M.; Savikhin, Sergei; Pushkar, Yulia

doi:10.1002/cssc.202202124

Title: Photoexcitation of Fe ₃ O Nodes in MOF Drives Water Oxidation at pH=1 When Ru Catalyst Is Present

Journal Article · Mon Jan 09 00:00:00 EST 2023 · ChemSusChem

DOI:https://doi.org/10.1002/cssc.202202124· OSTI ID:1908402

Ezhov, Roman ^[1]; Ravari, Alireza K. ^[1]; Palenik, Mark ^[2]; Loomis, Alexander ^[1]; Meira, Debora M. ^[3]; Savikhin, Sergei ^[1];

^[1]

Department of Physics and Astronomy Purdue University West Lafayette 47907 USA
US Naval Research Laboratory Washington 20375 USA
Argonne National Laboratory Argonne IL 60439 USA

Abstract Artificial photosynthesis strives to convert the energy of sunlight into sustainable, eco‐friendly solar fuels. However, systems with light‐driven water oxidation reaction (WOR) at pH=1 are rare. Broadly used [Ru(bpy) ₃ ] ²⁺ (bpy=2,2’‐bipyridine) photosensitizer has a fixed +1.23 V potential which is insufficient to drive most water oxidation catalysts (WOCs) in acid, while Fe ₂ O ₃ , featuring the highly oxidizing holes, is not stable at low pH. Here, the key examples of Fe‐based metal–organic framework (MOF) water oxidation photoelectrocatalysts active at pH=1 are presented. Fe‐MIL‐126 and Fe MOF‐dcbpy structures were formed with 4,4’‐biphenyl dicarboxylate (bpdc), 2,2’‐bipyridine‐5,5’‐dicarboxylate (dcbpy) linkers and their mixtures. Presence of dcbpy linkers allows integration of metal‐based catalysts via coordination to 2,2’‐bipyridine fragments. Fe‐based MOFs were doped with Ru‐based precursors to achieve highly active MOFs bearing [Ru(bpy)(dcbpy)(H ₂ O) ₂ ] ²⁺ WOC. Materials were analyzed with X‐ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infra‐red (FTIR) spectroscopy, resonance Raman, X‐ray absorption spectroscopy, fs optical pump‐probe, electron paramagnetic resonance (EPR), diffuse reflectance and electric conductivity measurements and were modeled by band structure calculations. It is shown that under reaction conditions, Fe ^III and Ru ^III oxidation states are present, indicating rate‐limiting electron transfer in MOF. Fe ₃ O nodes emerge as photosensitizers able to drive prolonged O ₂ evolution in acid. Further developments are possible via MOF's linker modification for enhanced light absorption, electrical conductivity, reduced MOF solubility in acid, Ru‐WOC modification for faster WOC catalysis, or Ru‐WOC substitution to 3d metal‐based systems. The findings give further insight for development of light‐driven water splitting systems based on Earth‐abundant metals.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1908402

Alternate ID(s):: OSTI ID: 1996057

Journal Information:: ChemSusChem, Journal Name: ChemSusChem Vol. 16 Journal Issue: 5; ISSN 1864-5631

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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