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Graphitic-phase carbon nitride (g-C3N4) materials have exhibited increasingly remarkable performance as emerging electrochemiluminescence (ECL) emitters, owing to their unique optical and electronic properties; however, the ECL merits of porous g-C3N4 nanofibers doped with ternary metals are not yet explored. Deciphering the ECL properties of trimetal-doped g-C3N4 nanofibers could provide an exquisite pathway for ultrasensitive sensing and imaging with impressive advantages of minimal background signal, great sensitivity, and durability. Herein, we rationally synthesized g-C3N4 nanofibers doped atomically with Mn, Fe, and Co elements (Mn/Fe/Co/g-C3N4) in a one-pot via the protonation in ethanol and annealing process driven by the rolling up mechanism. The ECL performance of g-C3N4 with and without metal dopants was investigated and compared with standard Ru(bpy)32+ in the presence of potassium persulfate (K2S2O8) as the coreactant. Notably, g-C3N4 nanofibers doped with metal ions exhibited an ECL efficiency of 483% that was 4.83 times higher than that of Ru(bpy)32+. Mechanistic investigations unveiled that the g-C3N4 nanofibers possess a large surface area and, as a result, exhibit a reduced interfacial impedance within the porous microstructure. These factors contribute to the acceleration of charge transfer rates and the stabilization of charge carriers and excitons, ultimately facilitating the ECL process. This research endeavor may pave the way for a new hot research area and serves as a powerful tool for elucidating fundamental inquiries of ECL on one-dimensional g-C3N4 nanostructures.
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The interfacial engineering of Pd-based alloys (i.e., PdM with distinct morphologies, compositions, and strain defects) is an efficient way for enhanced catalytic activity; however, it remains a grand challenge to fabricate such alloys in aqueous solutions without heating, organic solvents, and multiple reaction steps. Herein, we present a simple, aqueous-phase, one-step, and ultrafast approach for the interfacial engineering of surfactant-free porous PdM (M = Cu, Au, and Mn) nanocrystals with well-controlled spongy-like morphology and compositions. The electronic interaction in PdM nanocrystals and their effect on the alkaline electrochemical ethanol oxidation reaction (EOR) are investigated using XRD, XPS, and electrochemical tests. Notably, integrating M metals into Pd atoms results in upshifting the d-band center of Pd and subsequently modulating the EOR activity and stability substantially. The EOR mass activity (10.78 A/mgPd (6.93 A/mgPdCu)) of PdCu was 1.83, 3.09, 4.51, and 53.90 times higher than those of AuPd (5.90 A/mgPd (3.27 A/mgAuPd)), PdMn (3.48 A/mgPd (3.19 A/mgPdMn)), Pd (2.39 A/mgPd), and Pd/C (0.20 A/mgPd), respectively, besides substantial durability after 1000 cycles. This is due to the porous two-dimensional morphology, a low synergetic effect, higher interfacial interaction, and greater active surface area of PdCu, besides a high Cu content with more oxophilicity that facilitates activation/dissociation of H2O to generate -OH species needed for quick EOR electrocatalysis. The electrochemical impedance spectroscopy (EIS) reveals better electrolyte/electrode interfacial interaction and lower charge transfer resistance on PdCu. The EOR activity of PdCu porous sponge-like nanocrystals was superior to all previously reported Pd-based alloys for electrochemical EOR. This study indicates that binary Pd-based catalysts with less synergetic effect are preferred for boosting the EOR activity, which could help in manipulating the surface properties of Pd-based alloys to optimize EOR performance.
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Tailoring the shape of Pd nanocrystals is one of the main ways to enhance catalytic activity; however, the effect of shapes and electrolyte pH on carbon monoxide oxidation (COOxid) is not highlighted enough. This article presents the controlled fabrication of Pd nanocrystals in different morphologies, including Pd nanosponge via the ice-cooling reduction of the Pd precursor using NaBH4 solution and Pd nanocube via ascorbic acid reduction at 25 °C. Both Pd nanosponge and Pd nanocube are self-standing and have a high surface area, uniform distribution, and clean surface. The electrocatalytic CO oxidation activity and durability of the Pd nanocube were significantly superior to those of Pd nanosponge and commercial Pd/C in only acidic (H2SO4) medium and the best among the three media, due to the multiple adsorption active sites, uniform distribution, and high surface area of the nanocube structure. However, Pd nanosponge had enhanced COOxid activity and stability in both alkaline (KOH) and neutral (NaHCO3) electrolytes than Pd nanocube and Pd/C, attributable to its low Pd-Pd interatomic distance and cleaner surface. The self-standing Pd nanosponge and Pd nanocube were more active than Pd/C in all electrolytes. Mainly, the COOxid current density of Pd nanocube in H2SO4 (5.92 mA/cm2) was nearly 3.6 times that in KOH (1.63 mA/cm2) and 10.3 times that in NaHCO3 (0.578 mA/cm2), owing to the greater charge mobility and better electrolyte-electrode interaction, as evidenced by electrochemical impedance spectroscopy (EIS) analysis. Notably, this study confirmed that acidic electrolytes and Pd nanocube are highly preferred for promoting COOxid and may open new avenues for precluding CO poisoning in alcohol-based fuel cells.
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Nanopartículas del Metal , Nanoestructuras , Paladio/química , Nanopartículas del Metal/química , Catálisis , Electrólitos/química , Etanol/química , Nanoestructuras/química , Concentración de Iones de HidrógenoRESUMEN
Rational synthesis of Co-ZIF-67 metal-organic framework (MOF)-derived carbon-supported metal nanoparticles is essential for various energy and environmental applications; however, their catalytic activity toward carbon monoxide (CO) oxidation in various electrolytes is not yet emphasized. Co-ZIF-67-derived hierarchical porous carbon nanosheet-supported Pd nanocrystals (Pd/ZIF-67/C) were prepared using a simple microwave-irradiation approach followed by carbonization and etching. Mechanistically, during microwave irradiation, triethyleneamine provides abundant reducing gases that promote the formation of Pd nanoparticles/Co-Nx in porous carbon nanosheets with the assistance of ethylene glycol and also form a multimodal pore size. The electrocatalytic CO oxidation activity and stability of Pd/ZIF-67/C outperformed those of commercial Pd/C and Pt/C catalysts by (4.2 and 4.4, 4.0 and 2.7, 3.59 and 2.7) times in 0.1 M HClO4, 0.1 M KOH, and 0.1 M NaHCO3, respectively, due to the catalytic properties of Pd besides the conductivity of Co-Nx active sites and delicate porous structures of ZIF-67. Notably, using Pd/ZIF-67/C results in a higher CO oxidation activity than Pd/C and Pt/C. This study may pave the way for using MOF-supported multi-metallic nanoparticles for CO oxidation electrocatalysis.
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Graphene-based nanomaterials with remarkable properties, such as good biocompatibility, strong mechanical strength, and outstanding electrical conductivity, have dramatically shown excellent potential in various applications. Increasing surface area and porosity percentage, improvement of adsorption capacities, reduction of adsorption energy barrier, and also prevention of agglomeration of graphene layers are the main advantages of functionalized graphene nanocomposites. On the other hand, Cerium nanostructures with remarkable properties have received a great deal of attention in a wide range of fields; however, in some cases low conductivity limits their application in different applications. Therefore, the combination of cerium structures and graphene networks has been widely invesitaged to improve properties of the composite. In order to have a comprehensive information of these nanonetworks, this research reviews the recent developments in cerium functionalized graphene derivatives (graphene oxide (GO), reduced graphene oxide (RGO), and graphene quantum dot (GQD) and their industrial applications. The applications of functionalized graphene derivatives have also been successfully summarized. This systematic review study of graphene networks decorated with different structure of Cerium have potential to pave the way for scientific research not only in field of material science but also in fluorescent sensing, electrochemical sensing, supercapacitors, and catalyst as a new candidate.
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Cerio , Grafito , Nanocompuestos , Nanoestructuras , Puntos Cuánticos , Conductividad Eléctrica , Grafito/química , Nanocompuestos/química , Nanoestructuras/químicaRESUMEN
Photocatalytic green hydrogen (H2) production through water electrolysis is deemed as green, efficient, and renewable fuel or energy carrier due to its great energy density and zero greenhouse emissions. However, developing efficient and low-cost noble-metal-free photocatalysts remains one of the daunting challenges in low-cost H2 production. Porous graphitic carbon nitride (gCN) nanostructures have drawn broad multidisciplinary attention as metal-free photocatalysts in the arena of H2 production and other environmental remediation. This is due to their impressive catalytic/photocatalytic properties (i.e., high surface area, narrow bandgap, and visible light absorption), unique physicochemical durability, tunable electronic properties, and feasibility to synthesize in high yield from inexpensive and earth-abundant resources. The physicochemical and photocatalytic properties of porous gCNs can be easily optimized via the integration of earth-abundant heteroatoms. Although there are various reviews on porous gCN-based photocatalysts for various applications, to the best of our knowledge, there are no reviews on heteroatom-doped porous gCN nanostructures for the photocatalytic H2 evolution reaction (HER). It is essential to provide timely updates in this research area to highlight the research related to fabrication of novel gCNs for large-scale applications and address the current barriers in this field. This review emphasizes a panorama of recent advances in the rational design of heteroatom (i.e., P, O, S, N, and B)-doped porous gCN nanostructures including mono, binary, and ternary dopants for photocatalytic HERs and their optimized parameters. This is in addition to H2 energy storage, non-metal configuration, HER fundamental, mechanism, and calculations. This review is expected to inspire a new research entryway to the fabrication of porous gCN-based photocatalysts with ameliorated activity and durability for practical H2 production.
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Nanoestructuras , Porosidad , Metales , HidrógenoRESUMEN
Direct alcohol fuel cells are deemed as green and sustainable energy resources; however, CO-poisoning of Pt-based catalysts is a critical barrier to their commercialization. Thus, investigation of the electrochemical CO oxidation activity (COOxid) of Pt-based catalyst over pH ranges as a function of Pt-shape is necessary and is not yet reported. Herein, porous Pt nanodendrites (Pt NDs) were synthesized via the ultrasonic irradiation method, and its CO oxidation performance was benchmarked in different electrolytes relative to 1-D Pt chains nanostructure (Pt NCs) and commercial Pt/C catalyst under the same condition. This is a trial to confirm the effect of the size and shape of Pt as well as the pH of electrolytes on the COOxid. The COOxid activity and durability of Pt NDs are substantially superior to Pt NCs and Pt/C in HClO4, KOH, and NaHCO3 electrolytes, respectively, owing to the porous branched structure with a high surface area, which maximizes Pt utilization. Notably, the COOxid performance of Pt NPs in HClO4 is higher than that in NaHCO3, and KOH under the same reaction conditions. This study may open the way for understanding the COOxid activities of Pt-based catalysts and avoiding CO-poisoning in fuel cells.
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Medicina , Nanoestructuras , Electrólitos , Oxidación-Reducción , Tomografía de Emisión de PositronesRESUMEN
The development of low-dimensional (LD) supramolecular materials with multifunctional electrocatalytic properties has sparked the attention of the catalysis community. Herein, we report the synthesis of a new class of 0D-2D heterostructures composed of boron carbon nitride nanosheets (BCN NSs) and fullerene molecules (C60/F) that exhibit multifunctional electrocatalytic properties for the hydrogen evolution/oxidation reactions (HER/HOR) and the oxygen evolution/reduction reactions (OER/ORR). The electrocatalytic properties were studied with varying F:BCN weight ratios to optimize the intermolecular electron transfer (ET) from the BCN NSs to the electron-accepting C60 molecules. The nanohybrid supramolecular material with 10 wt % F in BCN NSs (10% F/BCN) exhibited the largest Raman and C 1s binding energy shifts, which were associated with greater cooperativity interactions and enhanced ET processes at the F/BCN interface. This synergistic interfacial phenomenon resulted in highly active catalytic sites that markedly boosted electrocatalytic activity of the material. The 10% F/BCN showed the highest tetrafunctional catalytic performance, outperforming the OER catalytic activity of commercial RuO2 catalysts with a η10 of 390 mV and very competitive onset potential values of -0.042 and 0.92 V vs RHE for HER and ORR, respectively, and a current density value of 1.47 mA cm-2 at 0.1 V vs RHE with an ultralow ΔGH* value of -0.03 eV toward the HOR process. Additionally, the 10% F/BCN catalyst was also used as both cathode and anode in a water splitting device, delivering a cell potential of 1.61 V to reach a current density of 10 mA cm-2.
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A facile scalable approach is presented for the rational design of multidimensional, multilayered sand-clock-like UCNPs (denoted as UCCKs) bounded with high index facets, with a tunable Nd3+ content, and without a template or multiple complicated reaction steps. This was achieved using the seed-mediated growth and subsequent longitudinal direction epitaxial growth with the assistance of oleic acid and NH4F. The as-formed UCCKs composed of an inner layer (NaYF4:Yb,Er,Ca), an intermediate layer (NaYF4:Yb,Ca), and an outer layer (NaNdF4:Yb,Ca). The outer shell, enriched with Nd3+ sensitizer, augmented the near-infrared (NIR) photon absorption, whereas the intermediate shell, enriched with Yb3+, acted as a bridge for energy transfer from Nd3+ to Er3+ emitter in the inner core alongside with precluding any deleterious energy back-transfer from Er3+ or quenching effect from Nd3+. These unique structural and compositional properties of UCCKs endowed the UCL intensity of UCCKs by 22 and 10 times higher than that of hexagonal UCNP core (NaYF4:Yb,Er,Ca) and hexagonal UCNP core-shell (NaYF4:Yb,Er,Ca@NaYF4:Yb,Ca), respectively. Intriguingly, the UCL intensity increased significantly with increasing the content of Nd3+ in the outer shell. The silica-coated UCCKs were used as excellent long-term luminescence probes for the in vitro bioimaging without any noteworthy cytotoxicity. The presented approach may pave the road for controlling the synthesis of multidimensional UCCKs for various applications. Graphical abstract We developed novel multidimensional multilayered sand-clock-like upconversion nanostructures composed of a spherical inner core (NaYF4:Yb,Er,Ca), hexagonal intermediate shell (NaYF4:Yb,Ca) and two up-down outer shell (NaNdF4:Yb,Ca) with controllable Nd3+ as an efficient and safe probe for bioimaging applications without any quenching effect.
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Colorantes Fluorescentes/química , Nanopartículas del Metal/química , Fluorescencia , Colorantes Fluorescentes/efectos de la radiación , Fluoruros/química , Fluoruros/efectos de la radiación , Células HEK293 , Células HeLa , Humanos , Luz , Nanopartículas del Metal/efectos de la radiación , Microscopía Confocal , Microscopía Fluorescente , Itrio/química , Itrio/efectos de la radiaciónRESUMEN
BACKGROUND: Retention and stabilisation of a single-implant mandibular overdenture (SIMO) are influenced by the biomechanical properties and clinical performance of the attachment system. PURPOSE: To compare clinical and patient-reported outcomes following the use of two retention systems, a ball and a stud-type Equator attachment used for SIMO. MATERIAL AND METHODS: Eighteen fully edentulous participants were treated with a SIMO opposing to a maxillary complete denture. They received two retentive attachments (ball and Equator) in alternate periods (sequences A-B and B-A) and outcomes were assessed after the 1 week (initial) and 3 months (final) periods. In the final assessment, patients were also asked about their preferred retention system. RESULTS: Compared with baseline, there was an improvement in patient satisfaction using both attachments, whilst no difference was observed between initial and final periods. Similarly, no significant differences were observed when comparing the ball and Equator at the initial (P = .330) and final (P = .08) periods. The multilevel mixed-model analysis revealed that the patients' satisfaction was predicted only by their satisfaction with dentures before implant placement. Although no significant difference was found between attachments regarding patient preference, this may be biased by the sequence of attachment use, which suggests that a learning effect might be present in this crossover study design. CONCLUSION: The use of a single midline implant to retain a mandibular overdenture significantly improves patient satisfaction irrespective of the attachment used, but patients' preference for the second treatment suggested a learning effect in this study.
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Implantes Dentales , Prótesis de Recubrimiento , Estudios Cruzados , Prótesis Dental de Soporte Implantado , Retención de Dentadura , Dentadura Completa Inferior , Humanos , Mandíbula , Satisfacción del Paciente , Resultado del TratamientoRESUMEN
Biosynthesis silver nanoparticles (AgNPs) have received a lot of attention as a cytotoxic and antimicrobial activity against pathogenic bacteria. This study was carried out to evaluate the potential ability of red marine algae Corallina elongata and Gelidium amansii to biosynthesis AgNPs capping with Sodium Dodecyl Sulfate (SDS) and to determine its antibacterial efficacy. Characterization of capping AgNPs were determined by Ultra violet-Visible spectroscopy, Transmission electron microscope (TEM), Scanning electron microscopy (SEM), Fourier transforms infrared spectroscopy (FTIR), Energy dispersive X-ray spectroscopy (EDX), Zeta potential and sizer. The results indicated that there is no variation change between capping AgNPs synthesis by two red algae in plasmon resonance peak and also both stable along 3 weeks. The capping nanoparticles size were range from 8 to 25â¯nm in the case of G. amansii and 12-20â¯nmâ¯C. elongata. The results were obtained from Fourier transforms infrared spectroscopy (FTIR) indicated that same metals are present in both algae except Vanadium (V) was present with G. amansii. Capping AgNPs biosynthesis by C. elongata had more toxicity to Chlorella vulgaris than that of synthesized by G. amansii. Capping AgNPs by SDS have been shown to enhance antibacterial activity against Micrococcus leutus, Kocuria varians and Escherichia coli ATCC 8739 compared to non-capping AgNPs. The antibacterial activity and toxicity of AgNPs is affected by concentrations of capping agent and the biomaterial (red algae) that used for synthesis.
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Antibacterianos/metabolismo , Antibacterianos/farmacología , Bacterias/efectos de los fármacos , Nanopartículas del Metal/química , Rhodophyta/metabolismo , Plata/metabolismo , Dodecil Sulfato de Sodio/metabolismo , Antibacterianos/química , Estabilidad de Medicamentos , Nanopartículas del Metal/ultraestructura , Pruebas de Sensibilidad Microbiana , Microscopía Electrónica , Análisis Espectral , Resonancia por Plasmón de SuperficieRESUMEN
The precise fabrication of efficient catalysts for CO oxidation is of particular interest in a wide range of industrial and environmental applications. Herein, a scalable method is presented for the controlled synthesis of graphitic-like porous carbon nitride nanotubes (gC3N4NTs) codoped with Au and Pd (Au/Pd/gC3N4NTs) as efficient catalysts for carbon monoxide (CO) conversion. This includes the activation of melamine with nitric acid in the presence of ethylene glycol and metal precursors followed by consecutive polymerization and carbonization. This drives the formation of porous one-dimensional gC3N4NT with an outstanding surface area of (320.6 m2 g-1) and an atomic-level distribution of Au and Pd. Intriguingly, the CO conversion efficiency of Au/Pd/gC3N4NTs was substantially greater than that for gC3N4NTs. The approach thus presented may provide new avenues for the utilization of gC3N4 doped with multiple metal-based catalysts for CO conversion reactions which had been rarely reported before.
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Precise designs of low-cost and efficient catalysts for the detection of hydrogen peroxide (H2O2) over wide ranges of pH are important in various environmental applications. Herein, a versatile and ecofriendly approach is presented for the rational design of ternary bentonite-silylpropyl-polypyrrole/silver nanoarchitectures (denoted as BP-PS-PPy/Ag) via the in-situ photo polymerization of pyrrole with salinized bentonite (BP-PS) in the presence of silver nitrate. The Pyrrolyl-functionalized silane (PS) is used as a coupling agent for tailoring the formation of highly exfoliated BP-PS-PPy sheet-like nanostructures ornamented with monodispersed Ag nanoparticles (NPs). Taking advantage of the combination between the unique physicochemical properties of BP-PS-PPy and the outstanding catalytic merits of Ag nanoparticles (NPs), the as-synthesized BP-PS-PPy/Ag shows a superior electrocatalytic reduction and high-detection activity towards H2O2 under different pH conditions (from 3 to 10). Intriguingly, the UV-light irradiation significantly enhances the electroreduction activity of H2O2 substantially, compared with the dark conditions, due to the high photoelectric response properties of Ag NPs. Moreover, BP-PS-PPy/Ag achived a quick current response with a detection limit at 1 µM within only 1 s. Our present approach is green, facile, scalable and renewable.
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To develop low-cost and efficient oxygen reduction reaction (ORR) catalysts, a novel hybrid comprising cobalt-embedded nitrogen-doped carbon nanotubes and nitrogen-doped reduced graphene oxide (Co-NCNT/NrGO-800) was simply prepared by pyrolysis. The combination of nanotubes and graphene, and the efficient doping with cobalt and nitrogen, greatly contribute to the excellent ORR performance. This optimized Co-NCNT/NrGO catalyst exhibits a positive onset potential of 0.91â V and a half-wave potential of 0.82â V, combined with a relatively low peroxide yield, better durability, and better methanol tolerance than commercially available Pt/C, which makes it a promising candidate as a low-cost and effective non-precious-metal ORR catalyst.
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Control of structure and morphology of Pt-based nanomaterials is of great importance for electrochemical energy conversions. In this work, we report an efficient one-step synthesis of bimetallic porous AuPt nanoparticles (PAuPt NPs) in an aqueous solution. The proposed synthesis is performed by a simple stirring treatment of an aqueous reactive mixture including K2PtCl4, HAuCl4, Pluronic F127 and ascorbic acid at a pH value of 1 without organic solvent or high temperature. Due to their porous structure and bimetallic composition, as-made PAuPt NPs exhibit excellent electrocatalytic activity for oxygen reduction reaction.
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Electrocatalytic hydrogen evolution reactions (HER) are envisaged as the most promising sustainable approach for green hydrogen production. However, the considerably high cost often associated with such reactions, particularly upon scale-up, poses a daunting challenge. Herein, a facile, effective, and environmentally benign one-pot scalable approach is developed to fabricate MnM (MâCo, Cu, Ni, and Fe) nanocrystals supported over in situ formed carbon nanofibers (MnM/C) as efficient noble-metal-free electrocatalysts for HER. The formation of carbon nanofibers entails impregnating cellulose in an aqueous solution of metal precursors, followed by annealing the mixture at 550 °C. During the impregnation process, cellulose acts as a reactor for inducing the in situ reductions of MnM salts with the assistance of ether and hydroxyl groups to drive the mass production (several grams) of ultralong (5 ± 1 µM) carbon nanofibers ornamented with MnM nanoparticles (10-14 nm in size) at an average loading of 2.87 wt %. For better electrocatalytic HER benchmarking, the fabricated catalysts were tested over different working electrodes, i.e., carbon paper, carbon foam, and glassy carbon, in the presence of different electrolytes. All the fabricated MnM/C catalysts have demonstrated an appealing synergetic-effect-dependent HER activity, with MnCo/C exhibiting the best performance over carbon foam, close to that of the state-of-the-art commercial Pt/C (10 wt % Pt), with an overpotential of 11 mV at 10 mA cm-2, a hydrogen production rate of 2448 mol g-1 h-1, and a prolonged stability of 2 weeks. The HER performance attained by MnCo/C nanofibers is among the highest reported for Pt-free electrocatalysts, thanks to the mutual alloying effect, higher synergism, large surface area, and active interfacial interactions over the nanofibers. The presented findings underline the potential of our approach for the large-scale production of cost-effective electrocatalysts for practical HER.
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Porous Pd-based electrocatalysts are promising materials for alkaline direct ethanol fuel cells (ADEFCs) and ethanol sensors in the development of renewable energy and point-of-contact ethanol sensor test kits for drunk drivers. However, experimental and theoretical investigations of the interfacial interaction among Pd nanocrystals on supports (i.e., carbon black (CB), onion-like carbon (OLC), and CeO2/OLC) toward ADEFC and ethanol sensors are not yet reported. This is based on the preparation of Pd-CeO2/OLC nanocrystals by the sol-gel and impregnation methods. Evidently, the porous Pd-CeO2/OLC significantly increased membrane-free micro-3D-printed ADEFC performance with a high peak power density (Pmax = 27.15 mW cm-2) that is 1.38- and 7.58-times those of Pd/OLC (19.72 mW cm-2) and Pd/CB (3.59 mW cm-2), besides its excellent stability for 48 h. This is due to the excellent interfacial interaction among Pd, CeO2, and OLC, evidenced by density functional theory (DFT) simulations that showed a modulated Pd d-band center and facile active oxygenated species formation by the CeO2 needed for ethanol fuel cells. Similarly, Pd-CeO2/OLC gives excellent sensitivity (0.00024 mA mM-1) and limit of detection (LoD = 8.7 mM) for ethanol sensing and satisfactory recoveries (89-108%) in commercial alcoholic beverages (i.e., human serum, Amstel beer, and Nederberg Wine). This study shows the excellent possibility of utilizing Pd-CeO2/OLC for future applications in fuel cells and alcohol sensors.
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The tailored design of tri-metallic Pt-based porous nanodendrites (PNDs) is crucial for green energy production technologies, ascribed to their fancy features, great surface areas, accessible active sites, and stability against aggregation. However, their aqueous-phase one-step synthesis at room temperature remains a daunting challenge. Herein, we present a facile, green, and template-free approach for the one-step synthesis of PtPdCu PNDs by ultrasonication of an aqueous solution of metal salts and Pluronic F127 at 25 â, based on natural isolation among nucleation and growth step driven by the disparate reduction kinetics of the metals and acoustic cavitation mechanism of ultrasonic waves. The resultant PtPdCu PNDs formed in a spatial nanodendritic shape with a dense array of branches, open corners, interconnected pores, high surface area (46.9 m2/g), and high Cu content (21 %). The methanol oxidation reaction (MOR) mass activity of PtPdCu PNDs (3.66 mA/µgPt) is 1.45, 2.73, and 2.83 times higher than those of PtPd PNDs, PtCu PNDs, and commercial Pt/C, respectively based on equivalent Pt mass, which is superior to previous PtPdCu catalysts reported elsewhere, besides a superior durability and CO-poisoning tolerance. This study may pave the way for the controlled fabrication of ternary Pt-based PNDs for various electrocatalytic applications.
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Morphologically controlled Pd-based nanocrystals are the most efficient strategies for improving the electrocatalytic ethanol oxidation reaction (EOR) performance; however, their morphological-EOR activity relationship and effect of electrolytes at a wide pH range are still ambiguous. Here, we have synthesized porous self-standing Pd clustered nanospheres (Pd-CNSs) and Pd nanocubes (Pd-NCBs) for the EOR in acidic (H2SO4), alkaline (KOH), and neutral (NaHCO3) electrolytes compared to commercial spherical-like Pd/C catalysts. The fabrication process comprises the ice-cooling reduction of Pd precursor by sodium borohydride (NaBH4) and l-ascorbic acid to form Pd-CNSs and Pd-NCBs, respectively. The EOR activity of Pd-CNSs significantly outperformed those of Pd-NCBs, and Pd/C in all electrolytes, but the EOR activity was better in KOH than in H2SO4 and NaHCO3. This is due to the 3D porous clustered nanospherical morphology that makes Pd active centers more accessible and maximizes their utilization during EOR. The EOR specific/mass activities of Pd-CNSs reached (8.51 mA/cm2/2.39 A/mgPd) in KOH, (2.98 mA/cm2/0.88 A/mgPd) in H2SO4, and (0.061 mA/cm2/0.0083 A/mgPd) in NaHCO3, in addition to stability after 1000 cycles. This study affirms that porous 3D spherical Pd nanostructures are preferred for the EOR than those of 0D spherical-like and multi-dimensional cube-like nanostructures.