Electrocatalytic hydrogen evolution by an iron complex containing a nitro-functionalized polypyridyl ligand

Hartley, Carolyn L.; DiRisio, Ryan J.; Chang, T.; Zhang, Wanji; McNamara, William R.

doi:10.1016/j.poly.2015.11.023

Cited by 30 publications

(13 citation statements)

References 29 publications

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“…Complexes 1 – 3 were synthesized according to a literature procedure . The UV–vis spectra show absorption bands corresponding to ligand-to-metal charge transfer (LMCT), with all three complexes showing two main absorption events in the region 350–750 nm (see the Supporting Information).…”

Section: Resultsmentioning

confidence: 99%

“…To this end, we have reported a family of Fe(III) catalysts that are active electrocatalysts for proton reduction and are stable in aqueous solutions (Figure ). Complex 1 is a highly active electrocatalyst ( i c / i p = 7.8) that operates with an 800 mV overpotential . The activity of the original complex was improved ( i c / i p = 13) by incorporating a hemilabile sulfinate moiety ( 2 ) .…”

Section: Introductionmentioning

confidence: 99%

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Iron Polypyridyl Complexes for Photocatalytic Hydrogen Generation

et al. 2016

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A series of Fe(III) complexes were recently reported that are stable and active electrocatalysts for reducing protons into hydrogen gas. Herein, we report the incorporation of these electrocatalysts into a photocatalytic system for hydrogen production. Hydrogen evolution is observed when these catalysts are paired with fluorescein (chromophore) and triethylamine (sacrificial electron source) in a 1:1 ethanol:water mixture. The photocatalytic system is highly active and stable, achieving TONs > 2100 (with respect to catalyst) after 24 h. Catalysis proceeds through a reductive quenching pathway with a quantum yield of over 3%.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Iron Polypyridyl Complexes for Photocatalytic Hydrogen Generation

et al. 2016

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“…Fe12 and Fe13 have thus also been established as HECs in organic solvents, but both showed limited solubility in water. 155−157…”

Section: Homogeneous Catalysismentioning

confidence: 99%

Electro- and Solar-Driven Fuel Synthesis with First Row Transition Metal Complexes

et al. 2019

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The synthesis of renewable fuels from abundant water or the greenhouse gas CO 2 is a major step toward creating sustainable and scalable energy storage technologies. In the last few decades, much attention has focused on the development of nonprecious metal-based catalysts and, in more recent years, their integration in solid-state support materials and devices that operate in water. This review surveys the literature on 3d metal-based molecular catalysts and focuses on their immobilization on heterogeneous solid-state supports for electro-, photo-, and photoelectrocatalytic synthesis of fuels in aqueous media. The first sections highlight benchmark homogeneous systems using proton and CO 2 reducing 3d transition metal catalysts as well as commonly employed methods for catalyst immobilization, including a discussion of supporting materials and anchoring groups. The subsequent sections elaborate on productive associations between molecular catalysts and a wide range of substrates based on carbon, quantum dots, metal oxide surfaces, and semiconductors. The molecule–material hybrid systems are organized as “dark” cathodes, colloidal photocatalysts, and photocathodes, and their figures of merit are discussed alongside system stability and catalyst integrity. The final section extends the scope of this review to prospects and challenges in targeting catalysis beyond “classical” H 2 evolution and CO 2 reduction to C 1 products, by summarizing cases for higher-value products from N 2 reduction, C x >1 products from CO 2 utilization, and other reductive organic transformations.

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“…There are several examples of electrochemical H 2 evolution that are second‐order in the proton source trifluoroacetic acid (TFA); Dempsey et al. have proposed that this could be due to dimerization to form (TFA) 2 , with the dimer acting as the proton source during catalysis [81–87] . If dimerization is suspected, alternative acids can be selected, different solvents can be employed, or studies to quantify the dimerization constant and determine E A/B values could be developed.…”

Section: The Thermodynamic Potential Ea/bmentioning

confidence: 99%

Determining the Overpotential of Electrochemical Fuel Synthesis Mediated by Molecular Catalysts: Recommended Practices, Standard Reduction Potentials, and Challenges

2021

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Molecular catalysts capable of performing electrochemical transformations are frequently utilized in the synthesis of fuels. A common benchmark for evaluating catalysts for electrochemical reactions is overpotential (η) and minimizing η remains an active goal in catalysis. This Review details approaches for the determination of thermodynamic potentials for common fuel‐forming reactions and for the determination of electrochemical overpotential, and underscores the need to employ methods that enable meaningful comparisons between molecular catalysts. Strategies for minimizing overpotential while maintaining high activity are highlighted.

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Electrocatalytic hydrogen evolution by an iron complex containing a nitro-functionalized polypyridyl ligand

Cited by 30 publications

References 29 publications

Iron Polypyridyl Complexes for Photocatalytic Hydrogen Generation

Iron Polypyridyl Complexes for Photocatalytic Hydrogen Generation

Electro- and Solar-Driven Fuel Synthesis with First Row Transition Metal Complexes

Determining the Overpotential of Electrochemical Fuel Synthesis Mediated by Molecular Catalysts: Recommended Practices, Standard Reduction Potentials, and Challenges

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