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Elaboration of Prussian Blue Analogue/Silica Nanocomposites: Towards Tailor-Made Nano-Scale Electronic Devices.

ABSTRACT: The research of new molecular materials able to replace classical solid materials in electronics has attracted growing attention over the past decade. Among these compounds photoswitchable Prussian blue analogues (PBA) are particularly interesting for the elaboration of new optical memories. However these coordination polymers are generally synthesised as insoluble powders that cannot be integrated into a real device. Hence their successful integration into real applications depends on an additional processing step. Nanostructured oxides elaborated by sol-gel chemistry combined with surfactant micelle templating can be used as nanoreactors to confine PBA precipitation and organize the functional nano-objects in the three dimensions of space. In this work we present the elaboration of different CoFe PBA/silica nanocomposites. Our synthetic procedure fully controls the synthesis of PBA in the porosity of the silica matrix from the insertion of the precursors up to the formation of the photomagnetic compound. We present results on systems from the simplest to the most elaborate: from disordered xerogels to ordered nanostructured films passing through mesoporous monoliths.

SUBMITTER: Fornasieri G

PROVIDER: S-EPMC5448922 | biostudies-other | 2012 Mar

REPOSITORIES: biostudies-other

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Synthesis of Hollow Co-Fe Prussian Blue Analogue Cubes by using Silica Spheres as a Sacrificial Template.

Project description:Herein, we report a novel method for the formation of hollow Prussian blue analogue (CoFe-PBA) nanocubes, using spherical silica particles as sacrificial templates. In the first step, silica cores are coated by a CoFe-PBA shell and then removed by etching with hydrofluoric acid (HF). The cubic shape of CoFe-PBA is well-retained even after the removal of the silica cores, resulting in the formation of hollow CoFe-PBA cubes. The specific capacity of the hollow CoFe-PBA nanocubes electrodes is about two times higher than that of solid CoFe-PBA nanocubes as storage materials for sodium ions. Such an improvement in the electrochemical properties can be attributed to their hollow internal nanostructure. The hollow architecture can offer a larger interfacial area between the electrolyte and the electrode, leading to an improvement in the electrochemical activity. This strategy can be applied to develop PBAs with hollow interiors for a wide range of applications.

| S-EPMC6080567 | 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

Cerium Hexacyanocobaltate: A Lanthanide-Compliant Prussian Blue Analogue for Li-Ion Storage.

Project description:Electrode materials are the most significant components of lithium-ion batteries (LIBs) and play an important role in endowing them with high electrochemical performance. The exploration of new electrode materials and their comparative study with contemporary resources will help the design of advanced electrodes. Here, we have synthesized a new type of Prussian blue analogue (cerium(III) hexacyanocobaltate, CeHCCo) and systematically explored the effect of valence states of Fe2+ and Ce3+ on crystal structure and electrochemical properties of final products. We demonstrate that the unbalanced charge in iron(II) hexacyanocobaltate (FeHCCo), as opposed to that in CeHCCo, results in more residual K+ ions, thereby leading to the occupancy of cavities. As a result, the K+ ion-rich FeHCCo exhibits lower capacities of 55 ± 3 and 15 ± 3 mAh g-1 at 0.1 and 1 A g-1, respectively, compared with the K+ ion-deficient CeHCCo that exhibits capacities of 242 ± 3 and 111 ± 3 mAh g-1 at the same current densities. This work provides a novel contribution for the exploration of new Prussian blue analogues and bestows a newer concept for electrode material design.

| S-EPMC6921632 | biostudies-literature

Enhanced Electrochemical Water Oxidation Activity by Structural Engineered Prussian Blue Analogue/rGO Heterostructure.

Project description:Prussian blue analogue (PBA), with a three-dimensional open skeleton and abundant unsaturated surface coordination atoms, attracts extensive research interest in electrochemical energy-related fields due to facile preparation, low cost, and adjustable components. However, it remains a challenge to directly employ PBA as an electrocatalyst for water splitting owing to their poor charge transport ability and electrochemical stability. Herein, the PBA/rGO heterostructure is constructed based on structural engineering. Graphene not only improves the charge transfer efficiency of the compound material but also provides confined growth sites for PBA. Furthermore, the charge transfer interaction between the heterostructure interfaces facilitates the electrocatalytic oxygen evolution reaction of the composite, which is confirmed by the results of the electrochemical measurements. The overpotential of the PBA/rGO material is only 331.5 mV at a current density of 30 mA cm-2 in 1.0 M KOH electrolyte with a small Tafel slope of 57.9 mV dec-1, and the compound material exhibits high durability lasting for 40 h.

| S-EPMC9458107 | biostudies-literature

Boosting the activity of Prussian-blue analogue as efficient electrocatalyst for water and urea oxidation.

Project description:The design and fabrication of intricate hollow architectures as cost-effective and dual-function electrocatalyst for water and urea electrolysis is of vital importance to the energy and environment issues. Herein, a facile solvothermal strategy for construction of Prussian-blue analogue (PBA) hollow cages with an open framework was developed. The as-obtained CoFe and NiFe hollow cages (CFHC and NFHC) can be directly utilized as electrocatalysts towards oxygen evolution reaction (OER) and urea oxidation reaction (UOR) with superior catalytic performance (lower electrolysis potential, faster reaction kinetics and long-term durability) compared to their parent solid precursors (CFC and NFC) and even the commercial noble metal-based catalyst. Impressively, to drive a current density of 10?mA?cm-2 in alkaline solution, the CFHC catalyst required an overpotential of merely 330?mV, 21.99% lower than that of the solid CFC precursor (423?mV) at the same condition. Meanwhile, the NFHC catalyst could deliver a current density as high as 100?mA?cm-2 for the urea oxidation electrolysis at a potential of only 1.40?V, 24.32% lower than that of the solid NFC precursor (1.85?V). This work provides a new platform to construct intricate hollow structures as promising nano-materials for the application in energy conversion and storage.

| S-EPMC6828720 | biostudies-literature

New Hybrid Nanomaterial Based on Self-Assembly of Cyclodextrins and Cobalt Prussian Blue Analogue Nanocubes.

Project description:Supramolecular self-assembly has been demonstrated to be a useful approach to developing new functional nanomaterials. In this work, we used a cobalt Prussian blue analogue (PBA, Co3[Co(CN)6]2) compound and a β-cyclodextrin (CD) macrocycle to develop a novel host-guest PBA-CD nanomaterial. The preparation of the functional magnetic material involved the self-assembly of CD molecules onto a PBA surface by a co-precipitation method. According to transmission electronic microscopy results, PBA-CD exhibited a polydisperse structure composed of 3D nanocubes with a mean edge length of 85 nm, which became shorter after CD incorporation. The supramolecular arrangement and structural, crystalline and thermal properties of the hybrid material were studied in detail by vibrational and electronic spectroscopies and X-ray diffraction. The cyclic voltammogram of the hybrid material in a 0.1 mol · L(-1) NaCl supporting electrolyte exhibited a quasi-reversible redox process, attributed to Co2+/Co3+ conversion, with an E1/2 value of 0.46 V (vs. SCE), with higher reversibility observed for the system in the presence of CD. The standard rate constants for PBA and PBA-CD were determined to be 0.07 and 0.13 s(-1), respectively, which suggests that the interaction between the nanocubes and CD at the supramolecular level improves electron transfer. We expect that the properties observed for the hybrid material make it a potential candidate for (bio)sensing designs with a desirable capability for drug delivery.

| S-EPMC4519860 | biostudies-literature

Unconventional CN vacancies suppress iron-leaching in Prussian blue analogue pre-catalyst for boosted oxygen evolution catalysis.

Project description:The incorporation of defects, such as vacancies, into functional materials could substantially tailor their intrinsic properties. Progress in vacancy chemistry has enabled advances in many technological applications, but creating new type of vacancies in existing material system remains a big challenge. We show here that ionized nitrogen plasma can break bonds of iron-carbon-nitrogen-nickel units in nickel-iron Prussian blue analogues, forming unconventional carbon-nitrogen vacancies. We study oxygen evolution reaction on the carbon-nitrogen vacancy-mediated Prussian blue analogues, which exhibit a low overpotential of 283 millivolts at 10 milliamperes per square centimeter in alkali, far exceeding that of original Prussian blue analogues and previously reported oxygen evolution catalysts with vacancies. We ascribe this enhancement to the in-situ generated nickel-iron oxy(hydroxide) active layer during oxygen evolution reaction, where the Fe leaching was significantly suppressed by the unconventional carbon-nitrogen vacancies. This work opens up opportunities for producing vacancy defects in nanomaterials for broad applications.

| S-EPMC6595008 | biostudies-literature

Mixed Cu-Fe Sulfides Derived from Polydopamine-Coated Prussian Blue Analogue as a Lithium-Ion Battery Electrode.

Project description:Batteries employing transition-metal sulfides enable high-charge storage capacities, but polysulfide shuttling and volume expansion cause structural disintegration and early capacity fading. The design of heterostructures combining metal sulfides and carbon with an optimized morphology can effectively address these issues. Our work introduces dopamine-coated copper Prussian blue (CuPB) analogue as a template to prepare nanostructured mixed copper-iron sulfide electrodes. The material was prepared by coprecipitation of CuPB with in situ dopamine polymerization, followed by thermal sulfidation. Dopamine controls the particle size and favors K-rich CuPB due to its polymerization mechanism. While the presence of the coating prevents particle agglomeration during thermal sulfidation, its thickness demonstrates a key effect on the electrochemical performance of the derived sulfides. After a two-step activation process during cycling, the C-coated KCuFeS2 electrodes showed capacities up to 800 mAh/g at 10 mA/g with nearly 100% capacity recovery after rate handling and a capacity of 380 mAh/g at 250 mA/g after 500 cycles.

| S-EPMC9631889 | biostudies-literature

Self-powered fluorescence display devices based on a fast self-charging/recharging battery (Mg/Prussian blue).

Project description:Stimuli-responsive (such as voltage and/or light) fluorescence display systems have attracted particular attention in their promising fields of application. However, there are few examples of self-powered fluorescence display devices. Here we designed and fabricated a self-powered fluorescence display device based on a fast-charging/recharging battery. The specially designed battery was composed of a Prussian blue (PB) cathode and a magnesium metal anode with a high theoretical redox potential difference (∼2.8 V). Moreover, smartly adding a trace amount of NaClO in the electrolyte could realize oxidizing PW to PB ∼480 times faster than when oxidizing without NaClO, leading to the fast self-charging and high power density (maximum power density of 13.34 mW cm-2, about two to three orders of magnitude larger than previous bio-fuel cells) of the Mg/PB battery. Most importantly, PB was used as not only the cathodic catalyst but also as an electrochromic material, making it possible to construct a self-powered and rechargeable electrochromic fluorescence display with only two electrodes. Besides, fluorescent [Ru(bpy)3]2+-doped silica nanoparticles (Ru@SiO2), were selected as the fluorescence resonance energy transfer (FRET) donor to match PB (FRET acceptor). To the best of our knowledge, we demonstrated a self-powered and rechargeable electrochromic fluorescence display with only two electrodes for the first time.

| S-EPMC5355813 | biostudies-literature

Spiderweb-Like Fe-Co Prussian Blue Analogue Nanofibers as Efficient Catalyst for Bisphenol-A Degradation by Activating Peroxymonosulfate.

Project description:Prussian blue and its analogues (PBA) based nanomaterials have been widely applied to removing pollutants in the recent years. However, easy aggregation and poor recycling largely limit their practical applications. In this work, spiderweb-like Fe-Co Prussian blue analogue/polyacrylonitrile (FCPBA/PAN) nanofibers were prepared by electrospinning and applied to degrading bisphenol-A (BPA) by activating peroxymonosulfate (PMS). Detailed characterization demonstrated that a high loading of FCPBA (86% of FCPBA in FCPBA/PAN) was successfully fixed on the PAN nanofibers. 67% of BPA was removed within 240 min when 500 mg·L-1 PMS and 233 mg·L-1 FCPBA/PAN were introduced in 20 mg·L-1 BPA solution at initial pH of 2.8. Electron paramagnetic resonance (EPR) and radical inhibition experiments were performed to identify the possible degradation mechanism. For comparison, a low loading of FCPBA nanofibers (0.6FCPBA/PAN nanofibers, 43% of FCPBA in FCPBA/PAN) were also prepared and tested the catalytic performance. The results showed that the activity of FCPBA/PAN was much higher than 0.6FCPBA/PAN. Furthermore, a FCPBA/PAN packed column was made as a reactor to demonstrate the reusability and stability of FCPBA/PAN nanofibers, which also exhibited the bright future for the industrial application. This work makes it possible to fabricate efficient PBA nanocatalysts with excellent recyclability and promotes the application of PBA in industrial areas.

| S-EPMC6473942 | biostudies-literature

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