Pyrene hydrogel for promoting direct bioelectrochemistry: ATP-independent electroenzymatic reduction of N<sub>2</sub>

Hickey, David P.; Lim, Koun; Cai, Rong; Patterson, Ashlea; Yuan, Mengwei; Şahin, Selmihan; Abdellaoui, Sofiène; Minteer, Shelley D.

doi:10.1039/c8sc01638k

Cited by 64 publications

(88 citation statements)

References 39 publications

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“…Several studies have shown that photocatalytically generated electrons can be transferred to the MoFe protein of nitrogenase, thus allowing N 2 to NH 3 without the need for the Fe protein and ATP hydrolysis. [ 10b,58 ] King et al used cadmium sulfide (CdS) nanocrystals to photosensitize the MoFe protein, where electron transfer from the conduction band of CdS to the MoFe protein efficiently drove enzymatic ammonia synthesis. [ 10b ] Such bio‐photocatalysis systems allow exploitation of both photoexcited charge carrier transfer of semiconductors and the precise active sites of nitrogenase, providing a rich toolbox to improve the efficiency of ammonia synthesis under ambient conditions.…”

Section: Key Developments In Low‐temperature Nitrogen Fixationmentioning

confidence: 99%

The Journey toward Low Temperature, Low Pressure Catalytic Nitrogen Fixation

Shi

Zhang

Waterhouse

et al. 2020

Advanced Energy Materials

143

101

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Ammonia and its derived products are vital to modern societies. Artificial nitrogen fixation to ammonia via the Haber–Bosch process has been employed industrially for over 100 years. However, the Haber–Bosch process is energy intensive and not sustainable in its current form as it uses hydrogen sourced from steam methane reforming to reduce N2. The roadmap to sustainable NH3 production demands the discovery of novel approaches for nitrogen fixation under near ambient conditions that preferably use water as the reducing agent. Over the last decade, great efforts have been made to develop catalysts capable of N2 fixation under mild reaction conditions, using strategies such as low temperature thermal catalysis, nonthermal plasma catalysis, enzymatic catalysis, photocatalysis, and electrocatalysis to generate ammonia and other valuable nitrogen‐containing chemicals. In parallel with catalytic performance studies, researchers have also placed emphasis on the mechanistic understanding of natural and artificial nitrogen fixation catalysts. In this work, the various routes now being explored for nitrogen fixation are summarized. The different dinitrogen activation and hydrogenation pathways are described, whilst describing key advances made to date on the journey toward near ambient ammonia synthesis. Key obstacles that need to be overcome to attract industry interest are also discussed.

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Section: Key Developments In Low‐temperature Nitrogen Fixationmentioning

confidence: 99%

The Journey toward Low Temperature, Low Pressure Catalytic Nitrogen Fixation

Shi

Zhang

Waterhouse

et al. 2020

Advanced Energy Materials

143

101

View full text Add to dashboard Cite

show abstract

“…In order to achieve this, a novel polymer functionalized with pyrene was employed. It is reported that these studies are able to achieve N 2 fixation independent of the Fe protein and ATP‐hydrolysis, representing a new prospect for N 2 fixation by nitrogenase . However, much work is required to fully exploit MoFe protein catalysis in this system.…”

Section: Recent Examples Of Enzymatic Electrochemistry For Small Molementioning

confidence: 99%

Recent Enzymatic Electrochemistry for Reductive Reactions

Cadoux

Milton

2020

ChemElectroChem

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Enzymatic electrochemistry is the coupling of oxidoreductase enzymes to electrodes, where electrons are transferred between the electrode and an enzyme's cofactor(s). In addition to enzymatic electrochemistry enabling mechanistic study [such as the determination of cofactor reduction potential(s)], enzymatic electrocatalysis also enables substrate reduction or oxidation by exploiting the catalytic properties of enzymes. This Minireview illustrates some recent examples, in which electrodes are coupled with enzymes that catalyze the reduction of substrates such as dinitrogen (N 2 ), carbon dioxide (CO 2 ) and protons (H + ), performed by metalloenzymes such as nitrogenases, formate dehydrogenases and hydrogenases. We review some strategies to achieve electron transfer (such as mediated and direct electron transfer), as well as some key results of recent studies.

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“…Hickey et al. developed a pyrene modified linear polyethyleneimine, which promotes protein adsorption and direct electron transfer of laccase and other proteins . For instance, this polymer was used in square wave voltammetric studies to determine the redox potentials of the cofactor and the P cluster in MoFe nitrogenase, VFe nitrogenase, and FeFe nitrogenase .…”

Section: Thermodynamicsmentioning

confidence: 99%

Enzymatic Bioelectrocatalysis for Enzymology Applications

Kummer

2020

ChemElectroChem

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Enzymatic biosensors are commonly used to evaluate the concentration of individual analytes in samples (e. g., glucose in blood, lactate in sweat, etc.), where the working electrode utilizes an enzyme (a "bioelectrode") as the chemically selective agent for electrochemical analyses. However, those same enzymatic bioelectrodes can be used for the analytical characterization of enzymes as a new biophysical characterization tool for enzymologists. This Minireview will detail recent work focused on utilizing enzymatic bioelectrocataysis for enzymology applications. Specifically, it will talk about the use of enzymatic bioelectrodes for studying kinetics, inhibition, transport, and thermodynamics. It will also compare and contrast electrochemical techniques with spectrophotometric techniques for enzymology.[a] M.

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Pyrene hydrogel for promoting direct bioelectrochemistry: ATP-independent electroenzymatic reduction of N₂

Abstract: We demonstrate a novel hydrogel material to facilitate direct bioelectrochemistry of a wide range of redox proteins and enable ATP-independent electroenzymatic reduction of N2 by nitrogenase.

Cited by 64 publications

References 39 publications

The Journey toward Low Temperature, Low Pressure Catalytic Nitrogen Fixation

The Journey toward Low Temperature, Low Pressure Catalytic Nitrogen Fixation

Recent Enzymatic Electrochemistry for Reductive Reactions

Enzymatic Bioelectrocatalysis for Enzymology Applications

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Pyrene hydrogel for promoting direct bioelectrochemistry: ATP-independent electroenzymatic reduction of N2

Abstract: We demonstrate a novel hydrogel material to facilitate direct bioelectrochemistry of a wide range of redox proteins and enable ATP-independent electroenzymatic reduction of N2 by nitrogenase.

Cited by 64 publications

References 39 publications

The Journey toward Low Temperature, Low Pressure Catalytic Nitrogen Fixation

The Journey toward Low Temperature, Low Pressure Catalytic Nitrogen Fixation

Recent Enzymatic Electrochemistry for Reductive Reactions

Enzymatic Bioelectrocatalysis for Enzymology Applications

Contact Info

Product

Resources

About

Pyrene hydrogel for promoting direct bioelectrochemistry: ATP-independent electroenzymatic reduction of N₂