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"Green" Prussian Blue Analogues as Peroxidase Mimetics for Amperometric Sensing and Biosensing.

ABSTRACT: Prussian blue analogs (PBAs) are well-known artificial enzymes with peroxidase (PO)-like activity. PBAs have a high potential for applications in scientific investigations, industry, ecology and medicine. Being stable and both catalytically and electrochemically active, PBAs are promising in the construction of biosensors and biofuel cells. The "green" synthesis of PO-like PBAs using oxido-reductase flavocytochrome b₂ is described in this study. When immobilized on graphite electrodes (GEs), the obtained green-synthesized PBAs or hexacyanoferrates (gHCFs) of transition and noble metals produced amperometric signals in response to H₂O₂. HCFs of copper, iron, palladium and other metals were synthesized and characterized by structure, size, catalytic properties and electro-mediator activities. The gCuHCF, as the most effective PO mimetic with a flower-like micro/nano superstructure, was used as an H₂O₂-sensitive platform for the development of a glucose oxidase (GO)-based biosensor. The GO/gCuHCF/GE biosensor exhibited high sensitivity (710 A M^-1m^-2), a broad linear range and good selectivity when tested on real samples of fruit juices. We propose that the gCuHCF and other gHCFs synthesized via enzymes may be used as artificial POs in amperometric oxidase-based (bio)sensors.

SUBMITTER: Gayda GZ

PROVIDER: S-EPMC8229941 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Strategies for synthesis of Prussian blue analogues.

Project description:We report a comparison of different common synthetic strategies for preparation of Prussian blue analogues (PBA). PBA are promising as cathode material for a number of different battery types, including K-ion and Na-ion batteries with both aqueous and non-aqueous electrolytes. PBA exhibit a significant degree of structural variation. The structure of the PBA determines the electrochemical performance, and it is, therefore, important to understand how synthesis parameters affect the structure of the obtained product. PBA are often synthesized by co-precipitation of a metal salt and a hexacyanoferrate complex, and parameters such as concentration and oxidation state of the precursors, flow rate, temperature and additional salts can all potentially affect the structure of the product. Here, we report 12 different syntheses and compare the structure of the obtained PBA materials.

| S-EPMC7890497 | biostudies-literature

Exploration of glassy state in Prussian blue analogues.

Project description:Prussian blue analogues (PBAs) are archetypes of microporous coordination polymers/metal-organic frameworks whose versatile composition allows for diverse functionalities. However, developments in PBAs have centred solely on their crystalline state, and the glassy state of PBAs has not been explored. Here we describe the preparation of the glassy state of PBAs via a mechanically induced crystal-to-glass transformation and explore their properties. The preservation of short-range metal-ligand-metal connectivity is confirmed, enabling the framework-based functionality and semiconductivity in the glass. The transformation also generates unconventional CN- vacancies, followed by the reduction of metal sites. This leads to significant porosity enhancement in recrystallised PBA, enabled by further accessibility of isolated micropores. Finally, mechanical stability under stress for successful vitrification is correlated to defect contents and interstitial water. Our results demonstrate how mechanochemistry provides opportunities to explore glassy states of molecular framework materials in which the stable liquid state is absent.

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Ladder Mechanisms of Ion Transport in Prussian Blue Analogues.

Project description:Prussian blue (PB) and its analogues (PBAs) are drawing attention as promising materials for sodium-ion batteries and other applications, such as desalination of water. Because of the possibilities to explore many analogous materials with engineered, defect-rich environments, computational optimization of ion-transport mechanisms that are key to the device performance could facilitate real-world applications. In this work, we have applied a multiscale approach involving quantum chemistry, self-consistent mean-field theory, and finite-element modeling to investigate ion transport in PBAs. We identify a cyanide-mediated ladder mechanism as the primary process of ion transport. Defects are found to be impermissible to diffusion, and a random distribution model accurately predicts the impact of defect concentrations. Notably, the inclusion of intermediary local minima in the models is key for predicting a realistic diffusion constant. Furthermore, the intermediary landscape is found to be an essential difference between both the intercalating species and the type of cation doping in PBAs. We also show that the ladder mechanism, when employed in multiscale computations, properly predicts the macroscopic charging performance based on atomistic results. In conclusion, the findings in this work may suggest the guiding principles for the design of new and effective PBAs for different applications.

| S-EPMC8762639 | biostudies-literature

Hidden diversity of vacancy networks in Prussian blue analogues.

Project description:Prussian blue analogues (PBAs) are a diverse family of microporous inorganic solids, known for their gas storage ability1, metal-ion immobilization2, proton conduction3, and stimuli-dependent magnetic4,5, electronic6 and optical7 properties. This family of materials includes the double-metal cyanide catalysts8,9 and the hexacyanoferrate/hexacyanomanganate battery materials10,11. Central to the various physical properties of PBAs is their ability to reversibly transport mass, a process enabled by structural vacancies. Conventionally presumed to be random12,13, vacancy arrangements are crucial because they control micropore-network characteristics, and hence the diffusivity and adsorption profiles14,15. The long-standing obstacle to characterizing the vacancy networks of PBAs is the inaccessibility of single crystals16. Here we report the growth of single crystals of various PBAs and the measurement and interpretation of their X-ray diffuse scattering patterns. We identify a diversity of non-random vacancy arrangements that is hidden from conventional crystallographic powder analysis. Moreover, we explain this unexpected phase complexity in terms of a simple microscopic model that is based on local rules of electroneutrality and centrosymmetry. The hidden phase boundaries that emerge demarcate vacancy-network polymorphs with very different micropore characteristics. Our results establish a foundation for correlated defect engineering in PBAs as a means of controlling storage capacity, anisotropy and transport efficiency.

| S-EPMC7025896 | biostudies-literature

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Project description:Ordered nanoperforated TiO2 monolayers fabricated through sol-gel chemistry were used to grow isolated particles of Prussian blue analogues (PBA). The elaboration of the TiO2/CoFe PBA nanocomposites involves five steps. The samples were characterized by scanning electron microscopy (SEM), atomic force microscopy (AFM), infrared spectroscopy and X-ray photoelectron spectroscopy (XPS) all along the synthesis process. Selected physico-chemical parameters have been varied in order to determine the key steps of the synthesis process and to optimize it. This study is an important step towards the full control of the fabrication process.

| S-EPMC4222400 | biostudies-other

Portable amperometric immunosensor for histamine detection using Prussian blue-chitosan-gold nanoparticle nanocomposite films.

Project description:Histamine (HA) is a biogenic amine that can accumulate to high concentration levels in food as a result of microbial activity and can cause toxic effects in consumers. In this work, a portable electrochemical immunosensor capable of detecting HA with high sensitivity and selectivity was developed. Prussian blue-chitosan-gold nanoparticle (PB-CS-AuNP) nanocomposite films with excellent biocompatibility were synthesized and characterized by scanning electron microscopy and energy dispersive X-ray analysis. The PB-CS-AuNP were coated onto a screen-printed electrode by one-step electrodeposition and used to conjugate the HA ovalbumin conjugate (HA-Ag). HA was determined by a competition between the coating HA-Ag and the HRP labeled HA antibody (HRP-HA-Ab). After careful optimization of assay conditions and Box-Behnken analysis, the developed immunosensor showed a linear range from 0.01 to 100μg/mL for HA in fish samples. The average recoveries from spiked samples ranged from 97.25% to 105%. The biosensor also showed good specificity, reproducibility, and stability, indicating its potential application in monitoring HA in a simple and low cost manner.

| S-EPMC5762249 | biostudies-literature

Thermal efficiency of a thermocell made of Prussian blue analogues.

Project description:Recently, it was reported that a thermocell can convert temperature into electric energy by using the difference in the thermal coefficient (??=?dV/dT) of the redox potential (V) between the cathode and anode materials. Among battery materials, Prussian blue analogues (PBAs) are promising materials for thermocell, because ? changes from approximately -0.3?mV/K in NaxMn[Fe(CN)6]0.83 3.5 H2O (NMF83) to approximately 1.3?mV/K in NaxCo[Fe(CN)6]0.92,9H2O (NCF90). In this work, we systematically investigated the thermal efficiency (?) of the NMF83/NCF90 thermocell relative to the difference (?T) between low (TL?=?282?K) and high (TH?=?292-338?K) temperatures. We found that the thermal efficiency (?) increased proportionally with ?T. The linear increase in ? is ascribed to the linear increase in the cell voltage (Vcell) and the charge (QNCF90) extracted from NCF90. Moreover, ? reached 3.19% at ?T?=?56?K, which corresponds to 19% of the Carnot efficiency (?carnot?=?17.0%). We further confirmed that the magnitude of QNCF90 is quantitatively reproduced by the slopes of the discharge curves of NMF83 and NCF90.

| S-EPMC6170380 | biostudies-literature

Development of amperometric glucose biosensor based on Prussian Blue functionlized TiO2 nanotube arrays.

Project description:Amperometric biosensors consisting of oxidase and peroxidase have attracted great attention because of their wide application. The current work demonstrates a novel approach to construct an enzymatic biosensor based on TiO2 nanotube arrays (TiNTs) as a supporting electrode on which Prussian Blue (PB)-an "artificial enzyme peroxidase" and enzyme glucose oxidase (GOx) have been immobilized. For this, PB nanocrystals are deposited onto the nanotube wall photocatalytically using the intrinsic photocatalytical property of TiO2, and the GOx/AuNPs nanobiocomposites are subsequently immobilized into the nanotubes via the electrodeposition of polymer. The resulting electrode exhibits a fast response, wide linear range, and good stability for glucose sensing. The sensitivity of the sensor is as high as 248 mA M(-1) cm(-2), and the detection limit is about 3.2 μM. These findings demonstrate a promising strategy to integrate enzymes and TiNTs, which could provide an analytical access to a large group of enzymes for bioelectrochemical applications including biosensors and biofuel cells.

| S-EPMC4219169 | biostudies-other

The structures of ordered defects in thiocyanate analogues of Prussian Blue.

Project description:We report the structures of six new divalent transition metal hexathiocyanatobismuthate frameworks with the generic formula , M = Mn, Co, Ni and Zn. These frameworks are defective analogues of the perovskite-derived trivalent transition metal hexathiocyanatobismuthates MIII[Bi(SCN)6]. The defects in these new thiocyanate frameworks order and produce complex superstructures due to the low symmetry of the parent structure, in contrast to the related and more well-studied cyanide Prussian Blue analogues. Despite the close similarities in the chemistries of these four transition metal cations, we find that each framework contains a different mechanism for accommodating the lowered transition metal charge, making use of some combination of Bi(SCN)6 3- vacancies, MBi antisite defects, water substitution for thiocyanate, adventitious extra-framework cations and reduced metal coordination number. These materials provide an unusually clear view of defects in molecular framework materials and their variety suggests that similar richness may be waiting to be uncovered in other hybrid perovskite frameworks.

| S-EPMC8159453 | biostudies-literature

In situ IR spectroscopy during oxidation process of cobalt Prussian blue analogues.

Project description:Cobalt Prussian blue analogues (Co-PBA; NaxCo[Fe(CN)6]y), consisting of cyano-bridged transition metal network, -Fe-CN-Co-NC-Fe-, are promising cathode materials for Na-ion secondary batteries. In the oxidation process, oxidization of Fe and/or Co are compensated by Na+ deintercalation. Here, we investigated the oxidization process of three Co-PBAs by means of in situ infrared absorption (IR) spectroscopy. With use of an empirical rule of the frequencies of the CN- stretching mode in ferrocyanide ([FeII(CN)6]4-) and ferricyanide ([FeIII(CN)6]3-), the oxidation processes of Co-PBAs were determined against the Fe concentration (y) and temperature (T). We will discuss the interrelation between the oxidation processes and Fe concentration (y).

| S-EPMC7892820 | biostudies-literature

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