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1.
Anal Methods ; 16(41): 6954-6963, 2024 Oct 24.
Artigo em Inglês | MEDLINE | ID: mdl-39415653

RESUMO

In this review, we explore the electroanalytical determination of mycophenolate mofetil and mycophenolic acid. Mycophenolate mofetil is a prodrug of mycophenolic acid, which is an immunosuppressive agent used to lower the body's natural immunity in patients who receive organ transplants as well as to treat autoimmune conditions. Laboratory based analytical instrumentation provide a routine methodology to measure mycophenolate mofetil and its metabolites, but there is scope to develop in-the-field analytical measurements that are comparable to those from laboratory equipment. Electroanalysis provides an opportunity to provide highly selective and sensitive outputs but are cost-efficient and can support on-site analysis. In this review, we provide an electroanalytical overview of the current research directed toward the measurement of mycophenolate mofetil and mycophenolic acid, offering insights to future research.


Assuntos
Técnicas Eletroquímicas , Imunossupressores , Ácido Micofenólico , Ácido Micofenólico/análise , Ácido Micofenólico/química , Humanos , Técnicas Eletroquímicas/métodos , Imunossupressores/análise
2.
Artigo em Inglês | MEDLINE | ID: mdl-39358698

RESUMO

Additive manufacturing electrochemistry is an ever-expanding field; however, it is limited to aqueous environments due to the conductive filaments currently available. Herein, the production of a conductive poly(propylene) filament, which unlocks the door to organic electrochemistry and electrosynthesis, is reported. A filament with 40 wt % carbon black possessed enhanced thermal stability, excellent low-temperature flexibility, and high conductivity. The filament produced highly reproducible additive manufactured electrodes that were electrochemically characterized, showing a k0 of 2.00 ± 0.04 × 10-3 cm s-1. This material was then applied to three separate electrochemical applications. First, the electroanalytical sensing of colchicine within environmental waters, where a limit of detection of 10 nM was achieved before being applied to tap, bottled, and river water. Second, the electrodes were stable in organic solvents for 100 cyclic voltammograms and 15 days. Finally, these were applied toward an electrosynthetic reaction of chlorpromazine, where the electrodes were stable for 24-h experiments, outperforming a glassy carbon electrode, and were able to be reused while maintaining a good electrochemical performance. This material can revolutionize the field of additive manufacturing electrochemistry and expand research into a variety of new fields.

3.
ACS Appl Mater Interfaces ; 16(38): 51397-51410, 2024 Sep 25.
Artigo em Inglês | MEDLINE | ID: mdl-39263982

RESUMO

Norovirus (NoV) is the predominant cause of foodborne illness globally; current detection methods are typically expensive, have inadequate sensitivities, and utilize biological receptors with poor stability. Therefore, accurate, cost-effective, and highly stable detection methods are needed to screen for NoV in foods. We developed molecularly imprinted polymer nanoparticles (nanoMIPs) to detect NoV using a small target epitope (12 amino acids) with a solid-phase synthesis approach. The performance of three batches of nanoMIPs with varying monomer compositions (nanoMIP-1, -2, and -3) were compared both experimentally and computationally. Surface plasmon resonance examined nanoMIP binding affinity to norovirus virus-like particles (NoV-LPs), whereby nanoMIP-1 had the lowest KD value of 0.512 µM. This is significant, as traditional targets for generation of norovirus ligands previously reported were generated against drastically larger norovirus capsid segments that have limitations in ease of production. Further, an electrochemical sensor was developed by covalently attaching the nanoMIPs to glassy carbon electrodes. In agreement with our predictions from density functional theory simulations, electrochemical impedance spectroscopy showed a sensitive response toward NoV-LPs for nanoMIP batches tested; however, nanoMIP-1 was optimal, with an excellent detection limit of 3.4 pg/mL (1.9 × 105 particles/mL). Due to its exceptional performance, nanoMIP-1 was immobilized to screen-printed electrodes and utilized within a thermal sensor, where it exhibited a low detection limit of 6.5 pg/mL (3.7 × 105 particles/mL). Crucially, we demonstrated that nanoMIP-1 could detect NoV in real food samples (romaine lettuce) by using electrochemical and thermal sensors. Consequently, the study highlights the exceptional potential of nanoMIPs to replace traditional biological materials (e.g., antibodies) as sensitive, versatile, and highly stable receptors within NoV sensors.


Assuntos
Polímeros Molecularmente Impressos , Nanopartículas , Norovirus , Norovirus/isolamento & purificação , Nanopartículas/química , Humanos , Polímeros Molecularmente Impressos/química , Técnicas Eletroquímicas/métodos , Impressão Molecular/métodos , Limite de Detecção
4.
ACS Omega ; 9(34): 36411-36420, 2024 Aug 27.
Artigo em Inglês | MEDLINE | ID: mdl-39220512

RESUMO

Pseudomonas aeruginosa is a multidrug-resistant Gram-negative bacterium that poses a significant threat to public health, necessitating rapid and on-site detection methods for rapid recognition. The goal of the project is therefore to indirectly detect the presence of P. aeruginosa in environmental water samples targeting one of its quorum-sensing molecules, namely, (S)-N-butyryl homoserine lactone (BHL). To this aim, molecularly imprinted polymers (MIPs) were synthesized via bulk free-radical polymerization using BHL as a template molecule. The obtained MIP particles were immobilized onto screen-printed electrodes (MIP-SPEs), and the BHL rebinding was analyzed via electrochemical impedance spectroscopy (EIS). To study the specificity of the synthesized MIPs, isotherm curves were built after on-point rebinding analysis performed via LC-MS measurements for both MIPs and NIPs (nonimprinted polymers, used as a negative control), obtaining an imprinting factor (IF) of 2.8 (at C f = 0.4 mM). The MIP-SPEs were integrated into an electrochemical biosensor with a linear range of 1 × 101-1 × 103 nM and a limit of detection (LoD) of 31.78 ± 4.08 nM. Selectivity measurements were also performed after choosing specific interferent molecules, such as structural analogs and potential interferents, followed by on-point analysis performed in spiked tap water to prove the sensor's potential to detect the presence of the quorum-sensing molecule in environmentally related real-life samples.

5.
Biomed Microdevices ; 26(3): 35, 2024 Aug 09.
Artigo em Inglês | MEDLINE | ID: mdl-39120827

RESUMO

Urinary tract infections (UTIs) represent the most prevalent type of outpatient infection, with significant adverse health and economic burdens. Current culture-based antibiotic susceptibility testing can take up to 72 h resulting in ineffective prescription of broad-spectrum antibiotics, poor clinical outcomes and development of further antibiotic resistance. We report an electrochemical lab-on-a-chip (LOC) for testing samples against seven clinically-relevant antibiotics. The LOC contained eight chambers, each housing an antibiotic-loaded hydrogel (cephalexin, ceftriaxone, colistin, gentamicin, piperacillin, trimethoprim, vancomycin) or antibiotic-free control, alongside a resazurin bulk-modified screen-printed electrode for electrochemical detection of metabolically active bacteria using differential pulse voltammetry. Antibiotic susceptibility in simulated UTI samples or donated human urine with either Escherichia coli or Klebsiella pneumoniae could be established within 85 min. Incorporating electrochemical detection onto a LOC provides an inexpensive, simple method for the sensitive determination of antibiotic susceptibility that is significantly faster than using a culture-based approach.


Assuntos
Antibacterianos , Escherichia coli , Klebsiella pneumoniae , Dispositivos Lab-On-A-Chip , Testes de Sensibilidade Microbiana , Infecções Urinárias , Infecções Urinárias/microbiologia , Infecções Urinárias/tratamento farmacológico , Infecções Urinárias/diagnóstico , Antibacterianos/farmacologia , Humanos , Testes de Sensibilidade Microbiana/instrumentação , Escherichia coli/efeitos dos fármacos , Escherichia coli/isolamento & purificação , Klebsiella pneumoniae/efeitos dos fármacos , Klebsiella pneumoniae/isolamento & purificação , Técnicas Eletroquímicas/instrumentação , Eletrodos
6.
ACS Nano ; 18(34): 23773-23784, 2024 Aug 27.
Artigo em Inglês | MEDLINE | ID: mdl-39141003

RESUMO

Al impurity is among the most likely components to enter the spent lithium-ion battery (LIB) cathode powder due to the strong adhesion between the cathode material and the Al current collector. However, high-value metal elements tend to be lost during the deep removal of Al impurities to obtain high-purity metal salt products in the conventional hydrometallurgical process. In this work, the harmful Al impurity is designed as a beneficial ingredient to upcycle high-voltage LiCoO2 by incorporating robust Al-O covalent bonds into the bulk of the cathode assisted with Ti modification. Benefiting from the strong Al-O and Ti-O bonds in the bulk, the irreversible phase transitions of the upcycled R-LCO-AT have been significantly suppressed at high voltages, as revealed by in situ XRD. Moreover, a Li+-conductive Li2TiO3 protective layer is constructed on the surface of R-LCO-AT by pinning slow-diffusion Ti on the grain boundaries, resulting in improved Li+ diffusion kinetics and restrained interface side reactions. Consequently, the cycle stability and rate performance of R-LCO-AT were significantly enhanced at a high cutoff voltage of 4.6 V, with a discharge capacity of 189.5 mAhg-1 at 1 C and capacity retention of 92.9% over 100 cycles at 4.6 V. This study utilizes the detrimental impurity element to upcycle high-voltage LCO cathodes through an elaborate bulk/surface structural design, offering a strategy for the high-value utilization of spent LIBs.

7.
Small ; : e2403320, 2024 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-39113348

RESUMO

The diagnosis of diabetes mellitus (DM) affecting 537 million adults worldwide relies on invasive and costly enzymatic methods that have limited stability. Electroactive polypyrrole (PPy)-based molecularly imprinted polymer nanoparticles (eMIPs) have been developed that rival the affinity of enzymes whilst being low-cost, highly robust, and facile to produce. By drop-casting eMIPs onto low-cost disposable screen-printed electrodes (SPEs), sensors have been manufactured that can electrochemically detect glucose in a wide dynamic range (1 µm-10 mm) with a limit of detection (LOD) of 26 nm. The eMIPs sensors exhibit no cross reactivity to similar compounds and negligible glucose binding to non-imprinted polymeric nanoparticles (eNIPs). Measurements of serum samples of diabetic patients demonstrate excellent correlation (>0.93) between these eMIPs sensor and the current gold standard Roche blood analyzer test. Finally, the eMIPs sensors are highly durable and reproducible (storage >12 months), showcasing excellent robustness and thermal and chemical stability. Proof-of-application is provided via measuring glucose using these eMIPs sensor in a two-electrode configuration in spiked artificial interstitial fluid (AISF), highlighting its potential for non-invasive wearable monitoring. Due to the versatility of the eMIPs that can be adapted to virtually any target, this platform technology holds high promise for sustainable healthcare applications via providing rapid detection, low-cost, and inherent robustness.

8.
ACS Omega ; 9(30): 33099-33110, 2024 Jul 30.
Artigo em Inglês | MEDLINE | ID: mdl-39100359

RESUMO

Herein, we present the first 3D-printed electrochemical portable biodevice for the detection of monkeypox virus (MKPV). The electrochemical device consists of two biosensors: an immunosensor and a genosensor specifically designed for the detection of the protein A29 and a target DNA of MKPV, respectively. The electrodes were manufactured using lab-made ultraflexible conductive filaments composed of carbon black, recycled PLA from coffee pods, and castor oil as a plasticizer. The sensors created through 3D printing technology exhibited good reproducibility and repeatability of analytical responses. Furthermore, both the immunosensor and genosensor demonstrated excellent MKPV detection capabilities, with a linear range from 0.01 to 1.0 µmol L-1 for the antigen and 0.1 to 20.0 µmol L-1 for the DNA target. The biosensors achieved limits of detection of 2.7 and 29 nmol L-1 for the immunosensor and genosensor, respectively. Interference tests conducted with the biosensors demonstrated their selectivity for MKPV. Moreover, analyses of fortified human serum samples showed recoveries close to 100%, confirming the absence of significant matrix effects for MKPV analysis. Therefore, the 3D-printed multiplex device represents a viable and highly promising alternative for on-site, portable, and rapid point-of-care MKPV monitoring.

9.
Glob Chall ; 8(7): 2300408, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-39006060

RESUMO

This review aims to provide an overview of sustainable approaches that can be incorporated into well-known procedures for the development of materials, pre- and post-treatments, modifications, and applications of 3D-printed objects, especially for fused filament fabrication (FFF). Different examples of conductive and non-conductive bespoke filaments using renewable biopolymers, bioplasticizers, and recycled materials are presented and discussed. The main final characteristics of the polymeric materials achieved according to the feedstock, preparation, extrusion, and treatments are also covered. In addition to recycling and remanufacturing, this review also explores other alternative approaches that can be adopted to enhance the sustainability of methods, aiming to produce efficient and environmentally friendly 3D printed products. Adjusting printing parameters and miniaturizing systems are also highlighted in this regard. All these recommended strategies are employed to minimize environmental damage, while also enabling the production of high-quality, economical materials and 3D printed systems. These efforts align with the principles of Green Chemistry, Sustainable Development Goals (SDGs), 3Rs (Reduce, Reuse, Recycle), and Circular Economy concepts.

10.
ACS Nano ; 2024 Jul 29.
Artigo em Inglês | MEDLINE | ID: mdl-39074061

RESUMO

On the basis of the sustainable concept, organic compounds and carbon materials both mainly composed of light C element have been regarded as powerful candidates for advanced electrochemical energy storage (EES) systems, due to theie merits of low cost, eco-friendliness, renewability, and structural versatility. It is investigated that the carbonyl functionality as the most common constituent part serves a crucial role, which manifests respective different mechanisms in the various aspects of EES systems. Notably, a systematical review about the concept and progress for carbonyl chemistry is beneficial for ensuring in-depth comprehending of carbonyl functionality. Hence, a comprehensive review about carbonyl chemistry has been summarized based on state-of-the-art developments. Moreover, the working principles and fundamental properties of the carbonyl unit have been discussed, which has been generalized in three aspects, including redox activity, the interaction effect, and compensation characteristic. Meanwhile, the pivotal characterization technologies have also been illustrated for purposefully studying the related structure, redox mechanism, and electrochemical performance to profitably understand the carbonyl chemistry. Finally, the current challenges and promising directions are concluded, aiming to afford significant guidance for the optimal utilization of carbonyl moiety and propel practicality in EES systems.

11.
Angew Chem Int Ed Engl ; 63(40): e202410420, 2024 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-38961660

RESUMO

The structural failure of Na2Mn[Fe(CN)6] could not be alleviated with traditional modification strategies through the adjustable composition property of Prussian blue analogues (PBAs), considering that the accumulation and release of stress derived from the MnN6 octahedrons are unilaterally restrained. Herein, a novel application of adjustable composition property, through constructing a coordination competition relationship between chelators and [Fe(CN)6]4- to directionally tune the enrichment of elements, is proposed to restrain structural degradation and induce unconventional energy coupling phenomenon. The non-uniform distribution of elements at the M1 site of PBAs (NFM-PB) is manipulated by the sequentially precipitated Ni, Fe, and Mn according to the Irving-William order. Electrochemically active Fe is operated to accompany Mn, and zero-strain Ni is modulated to enrich at the surface, synergistically mitigating with the enrichment and release of stress and then significantly improving the structural stability. Furthermore, unconventional energy coupling effect, a fusion of the electrochemical behavior between FeLS and MnHS, is triggered by the confined element distribution, leading to the enhanced electrochemical stability and anti-polarization ability. Consequently, the NFM-PB demonstrates superior rate performance and cycling stability. These findings further exploit potentialities of the adjustable composition property and provide new insights into the component design engineering for advanced PBAs.

12.
Mikrochim Acta ; 191(7): 375, 2024 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-38849611

RESUMO

The production, optimisation, physicochemical, and electroanalytical characterisation of a low-cost electrically conductive additive manufacturing filament made with recycled poly(lactic acid) (rPLA), castor oil, carbon black, and graphite (CB-G/PLA) is reported. Through optimising the carbon black and graphite loading, the best ratio for conductivity, low material cost, and printability was found to be 60% carbon black to 40% graphite. The maximum composition within the rPLA with 10 wt% castor oil was found to be an overall nanocarbon loading of 35 wt% which produced a price of less than £0.01 per electrode whilst still offering excellent low-temperature flexibility and reproducible printing. The additive manufactured electrodes produced from this filament offered excellent electrochemical performance, with a heterogeneous electron (charge) transfer rate constant, k0 calculated to be (2.6 ± 0.1) × 10-3 cm s-1 compared to (0.46 ± 0.03) × 10-3 cm s-1 for the commercial PLA benchmark. The additive manufactured electrodes were applied to the determination of ß-estradiol, achieving a sensitivity of 400 nA µM-1, a limit of quantification of 70 nM, and a limit of detection of 21 nM, which compared excellently to other reports in the literature. The system was then applied to the detection of ß-estradiol within four real water samples, including tap, bottled, river, and lake water, where recoveries between 95 and 109% were obtained. Due to the ability to create high-performance filament at a low material cost (£0.06 per gram) and through the use of more sustainable materials such as recycled polymers, bio-based plasticisers, and naturally occurring graphite, additive manufacturing will have a permanent place within the electroanalysis arsenal in the future.

13.
ACS Nano ; 18(20): 13150-13163, 2024 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-38726816

RESUMO

Layered sodium transition-metal (TM) oxides generally suffer from severe capacity decay and poor rate performance during cycling, especially at a high state of charge (SoC). Herein, an insight into failure mechanisms within high-voltage layered cathodes is unveiled, while a two-in-one tactic of charge localization and coherent structures is devised to improve structural integrity and Na+ transport kinetics, elucidated by density functional theory calculations. Elevated Jahn-Teller [Mn3+O6] concentration on the particle surface during sodiation, coupled with intense interlayer repulsion and adverse oxygen instability, leads to irreversible damage to the near-surface structure, as demonstrated by X-ray absorption spectroscopy and in situ characterization techniques. It is further validated that the structural skeleton is substantially strengthened through the electronic structure modulation surrounding oxygen. Furthermore, optimized Na+ diffusion is effectively attainable via regulating intergrown structures, successfully achieved by the Zn2+ inducer. Greatly, good redox reversibility with an initial Coulombic efficiency of 92.6%, impressive rate capability (86.5 mAh g-1 with 70.4% retention at 10C), and enhanced cycling stability (71.6% retention after 300 cycles at 5C) are exhibited in the P2/O3 biphasic cathode. It is believed that a profound comprehension of layered oxides will herald fresh perspectives to develop high-voltage cathode materials for sodium-ion batteries.

14.
Antibiotics (Basel) ; 13(5)2024 Apr 24.
Artigo em Inglês | MEDLINE | ID: mdl-38786110

RESUMO

Escherichia coli is listed as a priority 1 pathogen on the World Health Organization (WHO) priority pathogen list. For this list of pathogens, new antibiotics are urgently needed to control the emergence and spread of multidrug-resistant strains. This study assessed eighteen metal ions, graphene, and graphene oxide for their antimicrobial efficacy against E. coli in both planktonic and biofilm growth states and the potential synergy between metal ions and graphene-based compounds. Molybdenum and tin ions exhibited the greatest antimicrobial activity against the planktonic states of the isolates with minimal inhibitory concentrations (MIC) ranging between 13 mg/L and 15.6 mg/L. Graphene oxide had no antimicrobial effect against any of the isolates, while graphene showed a moderate effect against E. coli (MIC, 62.5 mg/L). Combinations of metal ions and graphene-based compounds including tin-graphene, tin-graphene oxide, gold-graphene, platinum-graphene, and platinum-graphene oxide exhibited a synergistic antimicrobial effect (FIC ≤ 0.5), inhibiting the planktonic and biofilm formation of the isolates regardless of their antibiotic-resistant profiles. The bactericidal effect of the metal ions and the synergistic effects when combined with graphene/graphene oxide against medically relevant pathogens demonstrated that the antimicrobial efficacy was increased. Hence, such agents may potentially be used in the production of novel antimicrobial/antiseptic agents.

15.
Anal Methods ; 16(17): 2625-2634, 2024 May 03.
Artigo em Inglês | MEDLINE | ID: mdl-38639065

RESUMO

Additive manufacturing (3D-printing), in particular fused filament fabrication, presents a potential paradigm shift in the way electrochemical based biosensing platforms are produced, giving rise to a new generation of personalized and on-demand biosensors. The use of additive manufactured biosensors is unparalleled giving rise to unique customization, facile miniaturization, ease of use, economical but yet, still providing sensitive and selective approaches towards the target analyte. In this mini review, we focus on the use of fused filament fabrication additive manufacturing technology alongside different biosensing approaches that exclusively use antibodies, enzymes and associated biosensing materials (mediators) providing an up-to-date overview with future considerations to expand the additive manufacturing biosensors field.


Assuntos
Técnicas Biossensoriais , Técnicas Eletroquímicas , Técnicas Biossensoriais/métodos , Técnicas Biossensoriais/instrumentação , Técnicas Eletroquímicas/métodos , Técnicas Eletroquímicas/instrumentação , Humanos , Impressão Tridimensional , Desenho de Equipamento
16.
RSC Adv ; 14(12): 8108-8115, 2024 Mar 06.
Artigo em Inglês | MEDLINE | ID: mdl-38464694

RESUMO

The first report of conductive recycled polyethylene terephthalate glycol (rPETg) for additive manufacturing and electrochemical applications is reported herein. Graphene nanoplatelets (GNP), multi-walled carbon nanotubes (MWCNT) and carbon black (CB) were embedded within a recycled feedstock to produce a filament with lower resistance than commercially available conductive polylactic acid (PLA). In addition to electrical conductivity, the rPETg was able to hold >10 wt% more conductive filler without the use of a plasticiser, showed enhanced temperature stability, had a higher modulus, improved chemical resistance, lowered levels of solution ingress, and could be sterilised in ethanol. Using a mix of carbon materials CB/MWCNT/GNP (25/2.5/2.5 wt%) the electrochemical performance of the rPETg filament was significantly enhanced, providing a heterogenous electrochemical rate constant, k0, equating to 0.88 (±0.01) × 10-3 cm s-1 compared to 0.46 (±0.02) × 10-3 cm s-1 for commercial conductive PLA. This work presents a paradigm shift within the use of additive manufacturing and electrochemistry, allowing the production of electrodes with enhanced electrical, chemical and mechanical properties, whilst improving the sustainability of the production through the use of recycled feedstock.

17.
ACS Meas Sci Au ; 4(1): 42-53, 2024 Feb 21.
Artigo em Inglês | MEDLINE | ID: mdl-38404492

RESUMO

Mesalamine, known as 5-aminosalicylic acid, is a medication used primarily in the treatment of inflammatory bowel disease, including ulcerative colitis and Crohn's disease. 5-Aminosalicylic acid can be measured using various benchtop laboratory techniques which involve liquid chromatography-mass spectroscopy, but these are sophisticated and large, meaning that they cannot be used on-site because transportation of the samples, chemicals, and physical and biological reactions can potentially occur, which can affect the sample's composition and potentially result in inaccurate results. An alternative approach is the use of electrochemical based sensing platforms which has the advantages of portability, cost-efficiency, facile miniaturization, and rapid analysis while nonetheless providing sensitivity and selectivity. We provide an overview of the use of the electroanalytical techniques for the sensing of 5-aminosalicylic acid and compare them to other laboratory-based measurements. The applications, challenges faced, and future opportunities for electroanalytical based sensing platforms are presented in this review.

18.
Talanta ; 272: 125761, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38364564

RESUMO

The biggest allure of heterogeneous electro-Fenton (HEF) processes largely fails on its high efficiency for the degradation of a plethora of hazardous compounds present in water, but still challenging to search for good and cost-effective electrocatalyst. In this work, carbon black (CB) and oxidised carbon black (CBox) materials were investigated as cathodes in the electrochemical production of hydrogen peroxide involved in HEF reaction for the degradation of 2-phenylphenol (2PP) as a target pollutant. The electrodes were fabricated by employing carbon cloth as support, and the highest H2O2 production yields were obtained for the CBox, pointing out the beneficial effect of the hydrophilic character of the electrode and oxygen-type functionalization of the carbonaceous surface. HEF degradation of 2PP was explored at -0.7 V vs. Ag/AgCl exhibiting the best conversion rates and degradation grade (total organic carbon) for the CBox-based cathode. In addition, the incorporation of an electrochemical sensor of 2PP in line with the HEF reactor was accomplished by the use of screen-printed electrodes (SPE) in order to monitor the pollutant degradation. The electrochemical sensor performance was evaluated from the oxidation of 2PP in the presence of Fe2+ ions by using square wave voltammetry (SWV) technique. The best electrochemical sensor performance was based on SPE modified with Meldola Blue showing a high sensitivity, low detection limit (0.12 ppm) and wide linear range (0.5-21 ppm) with good reproducibility (RSD 2.3 %). The all-in-one electrochemical station has been successfully tested for the degradation and quantification of 2PP, obtaining good recoveries analysing spiked waters from different water matrices origins.

19.
Mikrochim Acta ; 191(2): 96, 2024 01 15.
Artigo em Inglês | MEDLINE | ID: mdl-38225436

RESUMO

The combination of multi-walled carbon nanotubes (MWCNT) and carbon black (CB) is presented to produce a high-performance electrically conductive recycled additive manufacturing filament. The filament and subsequent additively manufactured electrodes were characterised by TGA, XPS, Raman, and SEM and showed excellent low-temperature flexibility. The MWCNT/CB filament exhibited an improved electrochemical performance compared to an identical in-house produced bespoke filament using only CB. A heterogeneous electrochemical rate constant, [Formula: see text] of 1.71 (± 0.19) × 10-3 cm s-1 was obtained, showing an almost six times improvement over the commonly used commercial conductive CB/PLA. The filament was successfully tested for the simultaneous determination of acetaminophen and phenylephrine, producing linear ranges of 5-60 and 5-200 µM, sensitivities of 0.05 µA µM-1 and 0.14 µA µM-1, and limits of detection of 0.04 µM and 0.38 µM, respectively. A print-at-home device is presented where a removable lid comprised of rPLA can be placed onto a drinking vessel and the working, counter, and reference components made from our bespoke MWCNT/CB filament. The print-at-home device was successfully used to determine both compounds within real pharmaceutical products, with recoveries between 87 and 120% over a range of three real samples. This work paves the way for fabricating new highly conductive filaments using a combination of carbon materials with different morphologies and physicochemical properties and their application to produce additively manufactured electrodes with greatly improved electrochemical performance.


Assuntos
Acetaminofen , Nanotubos de Carbono , Acetaminofen/análise , Nanotubos de Carbono/química , Fuligem , Fenilefrina , Técnicas Eletroquímicas
20.
Anal Chem ; 95(40): 15086-15093, 2023 Oct 10.
Artigo em Inglês | MEDLINE | ID: mdl-37768700

RESUMO

Mixing of graphite and carbon black (CB) alongside recycled poly(lactic acid) and castor oil to create an electrically conductive additive manufacturing filament without the use of solvents is reported herein. The additively manufactured electrodes (AMEs) were electrochemically benchmarked against a commercial conductive filament and a bespoke filament utilizing only CB. The graphite/CB produced a heterogeneous rate constant, k0, of 1.26 (±0.23) × 10-3 cm s-1 and resistance of only 155 ± 15 Ω, compared to 0.30 (±0.03) × 10-3 cm s-1 and 768 ± 96 Ω for the commercial AME. Including graphite within the filament reduced the cost of printing each AME from £0.09, with the CB-only filament, to £0.05. The additive manufacturing filament was successfully used to create an electroanalytical sensing platform for the detection of oxalate within a linear range of 10-500 µM, achieving a sensitivity of 0.0196 µA/µM, LOD of 5.7 µM and LOQ of 18.8 µM was obtained. Additionally, the cell was tested toward the detection of oxalate within a spiked synthetic urine sample, obtaining recoveries of 104%. This work highlights how, using mixed material composites, excellent electrochemical performance can be obtained at a reduced material cost, while also greatly improving the sustainability of the system.

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