Enzymes hosted in redox-active ionically cross-linked polyelectrolyte networks enable more efficient biofuel cells

Coria-Oriundo, Lucy L.; Cortez, M. Lorena; Azzaroni, Omar; Battaglini, Fernando

doi:10.1039/d1sm00221j

Cited by 10 publications

(11 citation statements)

References 56 publications

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“…The quartz crystal microbalance with dissipation (QCM-D) experiments were performed, using redox polyelectrolyte and enzyme solutions as described for graphite electrode modification, following a procedure previously reported. 21 IR Spectroscopy. Polarization modulation infrared reflection absorption spectroscopy (PM-IRRAS) experiments were performed following a procedure previously reported.…”

Section: ■ Materials and Methodsmentioning

confidence: 74%

“…The complex [Os(bpy) 2 Cl-(PyCHO)]Cl was synthesized as previously reported by Kober et al 20 The osmium-modified branched PEI (OsPEI) was synthesized as previously reported. 21 The osmium-modified PAA (OsPAA) was synthesized by adapting the procedure reported by Hermanson. 22 1 mg/mL PAA and 4.6 mM osmium complex in 0.2 M carbonate/ bicarbonate buffer solutions at pH 9.6 were prepared.…”

Section: ■ Materials and Methodsmentioning

confidence: 99%

“…23 The electrodes were modified by alternating exposure to solutions of redox polyelectrolytes (0.48 mM in osmium, OsPEI, or OsPAA, dissolved in water or sodium salts at pH 7.0) and GOx (1 mg mL −1 , water, pH 7.0). Electrodes were modified following the procedure previously described by Coria-Oriundo et al 21 Electrochemical Experiments. Cyclic voltammetry measurements were carried out in solution containing a 50 mM 4-(2- hydroxyethyl)-1-piperazineethanesulfonic acid (HEPES) + 100 mM NaCl buffer solution at pH 7.0 or in 100 mM glucose in 50 mM HEPES + 100 mM NaCl using a purpose-built potentiostat (TEQ-04, NanoTeq, Buenos Aires, Argentina).…”

Section: ■ Materials and Methodsmentioning

confidence: 99%

“…The electrode−electrolyte systems were connected through a fritted glass. Scan polarization was carried out as previously reported by Coria-Oriundo et al 21 Quartz Crystal Microbalance Measurements. The quartz crystal microbalance with dissipation (QCM-D) experiments were performed, using redox polyelectrolyte and enzyme solutions as described for graphite electrode modification, following a procedure previously reported.…”

Section: ■ Materials and Methodsmentioning

confidence: 99%

“…The electrodes were modified by alternating exposure to solutions of redox polyelectrolytes (0.48 mM in osmium, OsPEI, or OsPAA, dissolved in water or sodium salts at pH 7.0) and GOx (1 mg mL –1 , water, pH 7.0). Electrodes were modified following the procedure previously described by Coria-Oriundo et al…”

Section: Methodsmentioning

confidence: 99%

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Current Response Enhancement According to the Doping Anion’s Nature in Redox Polyelectrolyte─Enzyme Assemblies

Coria-Oriundo

Herrera

Leo

et al. 2022

ACS Appl. Polym. Mater.

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High-power density output in enzymatic fuel cells is a key feature to reduce the size of self-powered implantable medical devices. Electron transfer mediated through redox polyelectrolytes allows the transport of electrons from enzymes away from the electrode, improving the current output. It is known that doping ions in polyelectrolytes introduce relevant characteristics in the generation of assemblies regarding mass adsorption and stiffness. In this work, binary 1:1 sodium salts (NaX; X = F–, Cl–, Br–, NO3 –, ClO4 –) were studied as doping ions of two redox polyelectrolytes (osmium-based branched polyethyleneimine and osmium-based linear polyallylamine) to enhance the adsorption and electron transfer process in glucose oxidase/redox polyelectrolyte assemblies. Cyclic voltammetry, polarization modulation infrared reflection absorption spectroscopy, quartz crystal microbalance with dissipation, and atomic force microscopy were used to understand the growth mechanism of these films and their performance. Ion hydrophobicity plays a key role, bromide being the one that generates the greater absorption and the best electron transfer efficiency for both redox polyelectrolytes. Branched polyethyleneimine doped with bromide was the best combination for the construction of bioanodes. Its application on an O2–glucose enzymatic fuel cell yields a power density output of 2.5 mW cm–2, achieving state-of-the-art performance.

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Section: ■ Materials and Methodsmentioning

confidence: 74%

Section: ■ Materials and Methodsmentioning

confidence: 99%

Section: ■ Materials and Methodsmentioning

confidence: 99%

Section: ■ Materials and Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

See 3 more Smart Citations

Current Response Enhancement According to the Doping Anion’s Nature in Redox Polyelectrolyte─Enzyme Assemblies

Coria-Oriundo

Herrera

Leo

et al. 2022

ACS Appl. Polym. Mater.

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Supramolecular Electroactive Materials via Ionic Self‐assembly of Polyelectrolyte–surfactant Complexes – Chemistry, Practical Aspects, and Applications

Cortez

Marmisollé

Battaglini

et al. 2023

Supramolecular Nanotechnology

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A Mediator‐Free Multi‐Ply Biofuel Cell Using an Interfacial Assembly between Hydrophilic Enzymes and Hydrophobic Conductive Oxide Nanoparticles with Pointed Apexes

Kang,

Nam,

Ahn

et al. 2023

Advanced Materials

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Biofuel cells (BFCs) based on enzymatic electrodes hold great promise as power sources for biomedical devices. However, their practical use is hindered by low electron transfer efficiency and poor operational stability of enzymatic electrodes. Here, a novel mediator‐free multi‐ply BFC that overcomes these limitations and exhibits both substantially high‐power output and long‐term operational stability is presented. The approach involves the utilization of interfacial interaction‐induced assembly between hydrophilic glucose oxidase (GOx) and hydrophobic conductive indium tin oxide nanoparticles (ITO NPs) with distinctive shapes, along with a multi‐ply electrode system. For the preparation of the anode, GOx and oleylamine‐stabilized ITO NPs with bipod/tripod type are covalently assembled onto the host fiber electrode composed of multi‐walled carbon nanotubes and gold (Au) NPs. Remarkably, despite the contrasting hydrophilic and hydrophobic properties, this interfacial assembly approach allows for the formation of nanoblended GOx/ITO NP film, enabling efficient electron transfer within the anode. Additionally, the cathode is prepared by sputtering Pt onto the host electrode. Furthermore, the multi‐ply fiber electrode system exhibits unprecedented high‐power output (≈10.4 mW cm−2) and excellent operational stability (2.1 mW cm−2, ≈49% after 60 days of continuous operation). The approach can provide a basis for the development of high‐performance BFCs.

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Enzymes hosted in redox-active ionically cross-linked polyelectrolyte networks enable more efficient biofuel cells

Abstract: Self-assembled nanobiocatalyst. Phosphate-mediated cross-linking of redox polyelectrolytes and glucose oxidase leads to self-assembled nanostructures with higher output power density per mol of mediator, thus enabling more efficient biofuel cells.

Cited by 10 publications

References 56 publications

Current Response Enhancement According to the Doping Anion’s Nature in Redox Polyelectrolyte─Enzyme Assemblies

Current Response Enhancement According to the Doping Anion’s Nature in Redox Polyelectrolyte─Enzyme Assemblies

Supramolecular Electroactive Materials via Ionic Self‐assembly of Polyelectrolyte–surfactant Complexes – Chemistry, Practical Aspects, and Applications

A Mediator‐Free Multi‐Ply Biofuel Cell Using an Interfacial Assembly between Hydrophilic Enzymes and Hydrophobic Conductive Oxide Nanoparticles with Pointed Apexes

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