Dispersion Of Pt Nanoparticles Research Articles

Green and sustainable use of macadamia nuts as support material in Pt-based direct methanol fuel cells

The successful commercialization of direct methanol fuel cells (DMFCs) is hindered by inadequate methanol oxidation activity and anode catalyst longevity. Efficient and cost-effective electrode materials are imperative in the widespread use of DMFCs. While Platinum (Pt) remains the primary component of anodic methanol oxidation reaction (MOR) electrocatalysts, its utilization alone in DMFC systems is limited due to carbon monoxide (CO) poisoning, instability, methanol crossover, and high cost. These limitations impede the economic feasibility of Pt as an electrocatalyst. Herein, we present the use of powdered activated carbon (PAC) and granular activated carbon (GAC), both sourced from macadamia nut shells (MNS), a type of biomass. These bio-based carbon materials are integrated into hybrid supports with reduced graphene oxide (rGO), aiming to enhance the performance and reduce the production cost of the Pt electrocatalyst. Electrochemical and physicochemical characterizations of the synthesized catalysts, including Pt-rGO/PAC-1:1, Pt-rGO/PAC-1:2, Pt-rGO/GAC-1:1, and Pt-rGO/GAC-1:2, were conducted. X-ray diffraction analysis revealed crystallite sizes ranging from 1.18 nm to 1.68 nm. High-resolution transmission electron microscopy (HRTEM) images with average particle sizes ranging from 1.91 nm to 2.72 nm demonstrated spherical dispersion of Pt nanoparticles with some agglomeration across all catalysts. The electrochemical active surface area (ECSA) was determined, with Pt-rGO/GAC-1:1 exhibiting the highest ECSA of 73.53 m2 g−1. Despite its high ECSA, Pt-rGO/GAC-1:1 displayed the lowest methanol oxidation reaction (MOR) current density, indicating active sites with poor catalytic efficiency. Pt-rGO/PAC-1:1 and Pt-rGO/PAC-1:2 exhibited the highest MOR current densities of 0.77 mA*cm−2 and 0.74 mA*cm−2, respectively. Moreover, Pt-rGO/PAC-1:2 and Pt-rGO/PAC-1:1 demonstrated superior electrocatalytic mass (specific) activities of 7.55 mA/mg (0.025 mA*cm−2) and 7.25 mA/mg (0.021 mA*cm−2), respectively. Chronoamperometry tests revealed Pt-rGO/PAC-1:2 and Pt-rGO/PAC-1:1 as the most stable catalysts. Additionally, they exhibited the lowest charge transfer resistances and highest MOR current densities after durability tests, highlighting their potential for DMFC applications. The synthesized Pt supported on PACs hybrids demonstrated remarkable catalytic performance, stability, and CO tolerance, highlighting their potential for enhancing DMFC efficiency.

Seafood waste derived Pt/Chitin nanocatalyst for efficient hydrogenation of nitroaromatic compounds

The fabrication of reliable, reusable and efficient catalyst is crucial for the conversion of nitroaromatic compounds into more chemically valuable amine-based molecules. In this study, a series of chitin supported platinum (Pt) catalysts with high catalytic activity, stability, and reusability were developed by using chitin derived from seafood waste as raw materials. The catalytic performance differences among these catalysts activated by different methods were investigated by hydrogenation of nitroaromatic compounds. The results showed that the multilayer hierarchical pore structure and abundance of hydroxyl and acetamido groups in chitin provided ample anchoring sites for Pt nanoparticles (NPs), ensuring the high dispersion of Pt NPs. Moreover, the interconnected channels between chitin nanofibrous microspheres facilitated rapid transport of reaction substrates. The best Pt/Chitin catalyst exhibited excellent catalytic activity and broad substrate applicability in hydrogenation of nitroaromatic compounds. Significantly, even after 20 runs, no discernible deactivation of activity was observed, demonstrating exceptional catalytic reusability. The application of seafood waste-based catalysts is conducive to the development of a green/sustainable society.

Enhanced photocatalytic activity in H2 production from methanol aqueous solution based on the synthesized Pt-TiO2-decorated MoSe2 nanocomposites

In this work, a simple hydrothermal method to synthesize a ternary nanocomposite of Pt-TiO2 decorated on MoSe2 as a photocatalyst for hydrogen (H2) evolution from an aqueous methanol solution. The-as prepared Pt-TiO2/MoSe2 nanocomposite were characterized by XRD, Raman spectra, electron microscopy (FE-SEM/Mapping and HR-TEM), XPS UV-Vis and PL analysis. XRD patterns confirmed the presence of MoSe2 and Pt-TiO2 crystal phases in the Pt-TiO2/MoSe2 nanocomposite. Raman spectra displayed characteristic peaks corresponding to Mo-Se out-of-plane vibration and Pt-TiO2 vibration modes, confirming the successful synthesis of Pt-TiO2/MoSe2 nanocomposite. FE-SEM images showed a sheet-like morphology for MoSe2-NS and spherical Pt/TiO2 particles, with MoSe2 sparsely scattered on the Pt-TiO2 surface with EDS mapping confirmed even element distribution of Pt-TiO2/MoSe2 nanocomposite. TEM images revealed the transparent nature of MoSe2-NS with well-resolved lattice fringes. Pt-TiO2 exhibited uniform dispersion of Pt nanoparticles on TiO2, and the Pt-TiO2/MoSe2 nanocomposite showed integration of MoSe2-NS with Pt-TiO2. HRTEM images confirmed the lattice fringes of MoSe2-NS, Pt, and TiO2 particles. Tauc plot measurements revealed optical band gaps of 2.99 eV for MoSe2-NS, 3.19 eV for Pt-TiO2, and 2.78 eV for Pt-TiO2/MoSe2. XPS analysis confirmed the presence of Mo, Se, Pt, Ti, O, and C elements in the Pt-TiO2/MoSe2 nanocomposite. Based on the photoelectrochemical measurements, the Pt-TiO2/MoSe2 nanocomposite show the lower onset overpotential of 123 mV, which is much higher than Pt-TiO2 (179 mV) and MoSe2 (213 mV) at 10 mA/cm2. The photocatalytic efficiency of Pt-TiO2/MoSe2 nanocomposite in the context of H2 production through the enhancement of aqueous methanol under visible light exposure was assessed across different factors. Among these, the Pt-TiO2/MoSe2 nanocomposite exhibited the highest photoactivity in H2 production at 1337 μmolg−1 after 4 h. These results show the promising potential of the Pt-TiO2/MoSe2 nanocomposite catalyst in addressing both environmental and energy challenges in the future.

Interfacial Structures of Heterogeneous Systems Determined by Using in-Situ XAFS

During chemical reactions and catalysis, the surface and interfacial structural properties of materials are considerably important to understand and control the reactions. However, in-situ measurements have many limits during reactions. We used in-situ X-ray absorption fine structure (XAFS) to understand the local structural properties at the surface and the interface of metal catalysts on transition−metal−oxide supports. Pt nanoparticles (NPs) with a mean size of ~1 nm on TiO2 supports are synthesized using an incipient wetness method. In-situ XAFS measurements are performed from the Pt NPs/TiO2 at Pt L3 and Ti K edges during heating from room temperature to 500 ℃ in an H2 environment. Fourier−transformed extended X-ray absorption fine structure (FT−EXAFS), which is a unique tool to quantitatively determine the local structural properties of materials around a selected species element, shows a lack of oxygen atoms as the nearest neighbors of Pt atoms at T = 250 ℃; meanwhile, the wavelet-transformed EXAFS (WT-EXAFS) with enhanced resolution shows a weak but distinguishable oxygen signal around Pt atoms. Pt−O bonds likely exist at the interface of Pt/TiO2, although oxygens on the outer surfaces of Pt NPs are mostly dissociated at T > 250 ℃ in an H2 environment. This finding strongly suggests that the combination of FT−EAXFS and WT−EXAFS can more accurately describe small amounts of light elements bonding with heavy elements than FT−EXAFS can alone. DFT calculations confirm that the presence of extra oxygen atoms at the interfaces of Pt NPs/TiO2, playing a critical role in the stability and the dispersion of Pt NPs.

Ultrasound-Driven enhancement of Pt/C catalyst stability in oxygen reduction reaction

Polymer electrolyte membrane fuel cells (PEMFCs) have reached the commercialization phase, representing a promising approach to curbing carbon emissions. However, greater durability of PEMFCs is of paramount importance to ensure their long-term viability and effectiveness, and catalyst development has become a focal point of research. Pt nanoparticles supported on carbon materials (Pt/C) are the primary catalysts used in PEMFCs. Accomplishing both a high dispersion of uniform metal particles on the carbon support and robust adhesion between the metal particles and the carbon support is imperative for superior stability, and will thereby, advance the practical applications of PEMFCs in sustainable energy solutions. Ultrasound-assisted polyol synthesis (UPS) has emerged as a suitable method for synthesizing catalysts with a well-defined metal-support structure, characterized by the high dispersion and uniformity of metal nanoparticles. In this study, we focused on the effect of ultrasound on the synthesis of Pt/C via UPS and the resulting enhanced stability of Pt/C catalysts. Therefore, we compared Pt/C synthesized using a conventional polyol synthesis (Pt/C_P) and Pt/C synthesized via UPS (Pt/C_U) under similar synthesis conditions. The two catalysts had a similar Pt content and the average particle size of the Pt nanoparticles was similar; however, the uniformity and dispersion of Pt nanoparticles in Pt/C_U were better than those of Pt/C_P. Moreover, ex/in-situ analyses performed in a high-temperature environment, in which nanoparticles tend to agglomerate, have revealed that Pt/C_U exhibited a notable improvement in the adhesion of Pt particles to the carbon support compared with that of Pt/C_P. The enhanced adhesion is crucial for maintaining the stability of the catalyst, ultimately contributing to a better durability in practical applications. Ultrasound was applied to the carbon support without the Pt precursor under the same UPS conditions used to synthesize Pt/C_U to identify the reason for the increased adhesion between the Pt particles and the carbon support in Pt/C_U, and we discovered that oxygen functional groups (C-O, C = O, and O-C = O) for anchoring site of Pt particles were generated in the carbon support. Pt/C_U displayed an increase in stability in an electrochemical accelerated stress test (AST) in an acidic electrolyte. The physical and chemical effects of ultrasound on the synthesis of Pt/C via UPS were identified, and we concluded that UPS is suitable for synthesizing carbon supported electrocatalysts with high stability.

Sheet-Isolated MoS2 Used for Dispersing Pt Nanoparticles and its Application in Methanol Fuel Cells.

It is highly challenging to activate the basal plane and minimize the π-π stacking of MoS2 sheets, thus enhancing its catalytic performance. Here, we display an approach for making well-dispersed MoS2 . By using the N-doped multi-walled carbon nanotubes (NMWCNTs) as an isolation unit, the aggregation of MoS2 sheets was effectively reduced, favoring the dispersion of Pt nanoparticles (noted as Pt/NMWCNTs-isolated-MoS2 ). Excellent bifunctional catalytic performance for methanol oxidation and oxygen reduction reaction (MOR/ORR) were demonstrated by the produced Pt/NMWCNTs-isolated-MoS2 . In comparison to Pt nanoparticles supported on MoS2 (Pt/MoS2 ), the MOR activity (2314.14 mA mgpt -1 ) and stability (317.69 mA mgpt -1 after 2 h of operation) on Pt/NMWCNTs-isolatedMoS2 were 24 and 232 times higher, respectively. As for ORR, Pt/NMWCNTs-isolated-MoS2 holds large half-wave potential (0.88 V) and high stability (92.71 % after 22 h of operation). This work presents a tactic for activating the basal planes and reducing the π-π stacking of 2D materials to satisfy their applications in electrocatalysis. In addition, the proposed sheet-isolation method can be used for fabricating other 2D materials to promote the dispersion of nanoparticles, which assist its application in other fields of energy as well as the environment.

Engineered Catalyst Support with Improved Durability at Higher Weight Percentage of Platinum

Proton Exchange Membrane (PEM) fuel cells are a suitable electrochemical power source for heavy duty vehicle (HDV) applications due to their high efficiency and durability. The cathode of the fuel cell uses a higher geometric loading of platinum (∼0.2 to 0.4 mgPt/cm2) for the electrocatalysis of the kinetically sluggish Oxygen Reduction Reaction (ORR) which requires higher weight percent loading of the metal (∼50%) on the carbon support to decrease the catalyst layer thickness and hence, the reactant transport losses. The conventionally used supports for platinum catalyst, such as the KetjenBlackTM type high surface area carbon (HSC) features limited mesopore area for the dispersion of Pt nanoparticles leading to increased aggregation and poor durability. Here, we show a new class of carbon materials known as the Engineered Catalyst Support (ECS) developed by Pajarito Powder with higher mesopore fraction for the dispersion of higher weight percentage of Pt nanoparticles. ECS materials can disperse up to 50% Pt by weight of the catalyst thereby enabling lower catalyst layer thickness with higher performance retained after durability test. A comprehensive set of physico-chemical and electrochemical studies in membrane electrode assembly (MEA) are reported to understand the performance and durability of Pt/ECS catalysts.

3D Nitrogen-Doped Porous Carbon Supported Pt Catalyst for Electrocatalytic Oxidation of Glucose

Glucose fuel cells have attracted widespread attention in the biomedical field due to their ability to generate electrical energy continuously. The development of this technology has great potential in the application of powering implantable medical devices. However, the efficiency of the glucose oxidation reaction at the anode of the fuel cell is low, and a catalyst needs to be added to improve the reaction efficiency. Platinum (Pt) catalysts are prone to agglomerate during use, which limits the improvement of their properties such as catalytic activity and stability. To address this problem, in this paper, a three-dimensional ( 3D) N-doped porous carbon (NCZIF-8) material with a large specific surface area was prepared as a catalyst carrier using ZIF-8 as a precursor. Low loading rate of platinum (10 wt. %) was prepared (10% Pt/NCZIF-8) and used as catalysts for glucose oxidation reaction. The materials were structurally characterized by XRD, SEM, TEM, Raman and FT-IR, etc. The electrocatalytic properties of the materials were characterized using an electrochemical workstation. It was shown that the incorporation of NCZIF-8 carrier promotes the dispersion of Pt nanoparticles (NPs) and the utilization of the catalyst, which enhances the catalytic activity and stability of catalysts during electrocatalytic glucose oxidation. After 300 times cyclic voltammetry (CV) tests, the peak current density of 10% Pt/NCZIF-8 only decreased by 21. 12% and 8. 59% in the double-layer region and oxygen region, respectively, indicating the excellent stability of the catalyst. This kind of catalyst with low loading rate of precious metal has great potential for its practical application by improving catalyst utilization, which not only improves the catalytic efficiency but also reduces the material cost.

Spatial confinement: An effective strategy to improve H2O and SO2 resistance of the expandable graphite-modified TiO2-supported Pt nanocatalysts for CO oxidation

The expandable graphite (EG) modified TiO2 nanocomposites were prepared by the high shear method using the TiO2 nanoparticles (NPs) and EG as precursors, in which the amount of EG doped in TiO2 was 10 wt.%. Followed by the impregnation method, adjusting the pH of the solution to 10, and using the electrostatic adsorption to achieve spatial confinement, the Pt elements were mainly distributed on the exposed TiO2, thus generating the Pt/10EG-TiO2–10 catalyst. The best CO oxidation activity with the excellent resistance to H2O and SO2 was obtained over the Pt/10EG-TiO2–10 catalyst: CO conversion after 36 hr of the reaction was ca. 85% under the harsh condition of 10 vol.% H2O and 100 ppm SO2 at a high gaseous hourly space velocity (GHSV) of 400,000 hr−1. Physicochemical properties of the catalysts were characterized by various techniques. The results showed that the electrostatic adsorption, which riveted the Pt elements mainly on the exposed TiO2 of the support surface, reduced the dispersion of Pt NPs on EG and achieved the effective dispersion of Pt NPs, hence significantly improving CO oxidation activity over the Pt/10EG-TiO2–10 catalyst. The 10 wt.% EG doped in TiO2 caused the TiO2 support to form a more hydrophobic surface, which reduced the adsorption of H2O and SO2 on the catalyst, greatly inhibited deposition of the TiOSO4 and formation of the PtSO4 species as well as suppressed the oxidation of SO2, thus resulting in an improvement in the resistance to H2O and SO2 of the Pt/10EG-TiO2–10 catalyst.

Highly dispersed Pt clusters within ZSM-5 stabilized by alkali metal ions and Al sites for partial methane oxidation

Zeolite is an ideal material to encapsulate nanoparticles and avoid metal aggregation, but it is challenging to achieve a high degree of metal dispersion inside zeolite. In this work, the Na+ reagent was introduced to synthesize Pt@S-1 and Pt@ZSM-5 to explore the effect of Al sites and alkali metal ions on dispersion of Pt nanoparticles. The properties of four catalysts were characterized by XRD, TEM, CO-TPR, TG and FT-IR, and the effects of alkali metal ions were analyzed combined with POM test results. The introduction of a certain amount of alkali metal ions in Pt@ZSM-5 catalyst consumed part of the hydroxyl group to form stable Pt-Ox(OH)yNa active species, which further improves the stability and dispersity of platinum nanoparticles and promotes the activity of partial oxidation of methane. This stabilization strategy can be extended to other porous materials encapsulating metal nanoparticles.

Effect of Nitrogen Defects on Pt Nanoparticle Dispersion and Stability Studied by Electron Microscopy Paired with Machine Learning Image Processing for Probing Catalyst–Support Interactions

Polymer electrolyte membrane fuel cells are on the rise as a commercial technology, although Pt catalyst utilization and stability remain a challenge. N-doped carbon supports offer the opportunity to improve catalyst–support interactions, but there is limited understanding of the effects of various nitrogen functionalities on nucleation and the stabilization of Pt catalyst nanoparticles (NPs). This work uses a series of N-doped carbons with varying N chemistries and Pt NPs produced via a polyol method to investigate the effects of nitrogen on Pt catalyst that is deposited as externally nucleated and grown NPs. Samples were analyzed using X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM) to identify trends related to nitrogen speciation. TEM analysis was employed to investigate effects of nitrogen on nucleation of Pt NPs and their stability when subjected to accelerated stress testing up to 10000 cycles using identical-location TEM setup. Systematic incorporation of high throughput machine-learning-based imaging analysis paired with identical location microscopy uncovered several mechanistic insights relevant to catalysis and fuel cells applications. Within the study’s sample set, graphitic-N-rich carbons resulted in better dispersion of Pt NPs. However, these same graphitic-N-rich NC samples demonstrated significant instability, with a high degree of dissolution and some migration that correlated with a higher amount of graphitic N content. It was also found that the pyridinic-rich samples resulted in a mixed degradation mechanism where both migration and dissolution mechanisms were prominent throughout aging.

Rapid elimination of antibiotic gemifloxacin mesylate and methylene blue over Pt nanoparticles dispersed chitosan/g-C3N4 ternary visible light photocatalyst.

Appropriate material selection and proper understanding of bandgap modification are key factors for the development of efficient photocatalysts. Herein, we developed an efficient, well-organized visible light oriented photocatalyst based on g-C3N4 in association with polymeric network of chitosan (CTSN) and platinum (Pt) nanoparticles utilizing a straightforward chemical approach. Modern techniques like XRD, XPS, TEM, FESEM, UV-Vis, and FTIR spectroscopy were exploited for characterization of synthesized materials. XRD results confirmed the involvement of α-polymorphic form of CTSN in graphitic carbon nitride. XPS investigation confirmed the establishment of trio photocatalytic structure among Pt, CTSN, and g-C3N4. TEM examination showed that the synthesized g-C3N4 possesses fine fluffy sheets like structure (100 to 500nm in size) intermingled with a dense layered framework of CTSN with good dispersion of Pt nanoparticles on g-C3N4 and CTSN composite structure. The bandgap energies for g-C3N4, CTSN/g-C3N4, and Pt@ CTSN/g-C3N4 photocatalysts were found to be 2.94, 2.73, and 2.72eV, respectively. The photodegradation skills of each created structure have been examined on antibiotic gemifloxacin mesylate and methylene blue (MB) dye. The newly developed Pt@CTSN/g-C3N4 ternary photocatalyst was found to be efficacious for the elimination of gemifloxacin mesylate (93.3%) in 25min and MB (95.2%) just in 18min under visible light. Designed Pt@CTSN/g-C3N4 ternary photocatalytic framework exhibited ⁓ 2.20 times more effective than bare g-C3N4 for the destruction of antibiotic drug. This study provides a simple route towards the designing of rapid, effective visible light oriented photocatalyts for the existing environmental issues.

Surface-Modified CeO2-Octahedron-Supported Pt Nanoparticles as Ethylene Scavengers for Fruit Preservation

Catalytic oxidation of ethylene associated with the preservation of fruits and vegetables (F&V) at low temperatures remains challenging. To address this issue, CeO2-octahedron-supported Pt catalysts were synthesized and modified by capacitively coupled plasma for efficient catalytic oxidation of C2H4. After the plasma treatment, CeO2 with rich oxygen vacancies was created, which acted as a support to facilitate the regulation of the size and dispersion of Pt nanoparticles. Compared with Pt/pristine CeO2, the Pt/plasma-modified CeO2 catalyst (Pt/CeO2-P) showed significantly higher reactivity. More than 99.9% of ethylene conversion induced by Pt/CeO2-P could be sustained longer than 50 h at 25 °C, and 30 min even at 0 °C. Thus, Pt/CeO2 interface engineering by plasma modification technology is particularly promising for low-temperature catalytic oxidation of ethylene. Moreover, a comprehensive characterization was conducted to elucidate the reaction pathway and oxidation mechanism. From the preservation test using bananas as fruit samples, it was found that Pt/CeO2-P delayed postharvest deterioration and ripening of bananas due to the excellent ethylene scavenging effect created by the catalyst, thus demonstrating the great potential applications in F&V preservation.

Defect configuration of ceria for Pt anchoring toward efficient methanol oxidation

As a potential next-generation power source for portable electronic devices, commercialization process of direct methanol fuel cell (DMFC) technology is hindered by the high dependence of anode methanol oxidation reaction (MOR) on precious Pt catalyst. In order to improve the efficiency of Pt toward MOR catalysis, a Ni doping strategy is proposed for defect engineering on ceria substrate to achieve uniform dispersion of Pt nanoparticles. Besides, Ni could also act as electron donor for Pt and hence favor the removal of CO intermediate on Pt and act as a co-catalyst toward MOR. Superior MOR activity and great stability is therefore achieved for the as-prepared Pt/CeO2@Ni catalyst with 3 times higher peak MOR current density compared with Pt/C catalyst. Due to the evenly anchored Pt and enhanced CO oxidation ability caused from Ni doped ceria substrate, Pt utilization of the Pt/CeO2@Ni catalyst is calculated to be 3.24 times higher than that of the commercial Pt/C catalyst. By considering the significantly improved stability, the Pt/CeO2@Ni catalyst has the potential for application in DMFC devices.

Pt/NiCo2O4 nanowire arrays on Ni foam as catalysts for efficient formaldehyde oxidation at room temperature

Catalytic oxidation of formaldehyde (HCHO) at room temperature is a low-cost and efficient solution for indoor HCHO removal. In this work, NiCo2O4 nanowires were in-situ synthesized on nickel foam (NF) by a simple hydrothermal reaction and then decorated with platinum nanoparticles (NPs). The Pt/NiCo2O4-NF catalyst exhibited excellent HCHO oxidation capacity at ambient temperature, realizing a conversion rate of 90 % within 60 min. The nickel foam substrate prevents the aggregation of NiCo2O4 nanowire arrays. It also enables the growth of large-area and aligned nanowires, contributing to the uniform dispersion of Pt NPs. Moreover, due to the unique redox property and high reactivity of NiCo2O4, numerous surface oxygen vacancies and active oxygen species are generated together with Pt by NaBH4 reduction, which is beneficial to the adsorption and oxidation of HCHO. Moreover, the hierarchical macro-/mesoporous structure of Pt/NiCo2O4-NF facilitates the diffusion of gaseous reactants and provides easily accessible active sites. In contrast with nanosized catalysts, the three-dimensional (3D) Pt/NiCo2O4-NF catalyst possesses high machinability and practicability. This work may shed light on the fabrication of 3D hierarchical catalysts for oxidative HCHO removal and indoor air purification.

A facile approach to direct preparation of Pt nanocatalysts from oxidative dechloridation of supported H2PtCl6 by oxygen plasma

Effective dechlorination, as well as high dispersion, is necessary in the Pt nanocatalyst preparation from cheap chlorine-containing precursors like H2PtCl6. We herein report a facile approach to direct preparation of Pt nanocatalysts from oxidative dechloridation of the TiO2 (P25) supported H2PtCl6 by O2 plasma. Oxygen plasma can completely dechlorinate, enhance the dispersion of Pt nanoparticles, and create large number of low-coordinated sites, thus leading to the highest activity in WGS reaction. At 200 oC, the O2 plasma treated Pt nanocatalyst achieves CO reaction rate of 1.07 mmol·mg−1·h−1 in WGS reaction, which is significantly higher than that of H2 and N2 plasmas treated samples. The oxidative dechloridation mechanism of O2 plasma and structure–activity relationship of the supported Pt nanocatalysts were demonstrated.

Heteroatom doping effect of Pt/rGO catalysts for formaldehyde abatement at ambient temperature

The effect of doping with different heteroatoms (N, P, S, and F atoms) on physicochemical properties of reduced graphene oxide (rGO) catalysts and their performances on formaldehyde (HCHO) oxidation is investigated in this study. Nitrogen-doped rGO with a loading of 1 wt% Pt (Pt/N-rGO) sample exhibits a superior HCHO conversion of 82% at a gas hourly space velocity (GHSV) of 50,000 mL/(g × h) at ambient temperature. In addition, the Pt/N-rGO catalyst remained an outstanding activity and stability at room temperature after testing continuously for 48 h. A series of characterization results showed that nitrogen-doping significantly increased the defect degree and specific surface area of rGO compared with rGOs doped with other heteroatoms, promoted the dispersion of Pt nanoparticles (NPs), and produced more zero-valent Pt (Pt0). In addition, the average particle size of the Pt NPs in the samples doping with heteroatoms decreased from 36.4 nm to 4.4 nm. Combined with the results of HCHO-DRIFTS, the highly dispersed Pt NPs on the surface of Pt/N-rGO sample was conducive to activate oxygens and further transfer the formate intermediate.

Fe2+/Fe3+ Cycling for Coupling Self‐Powered Hydrogen Evolution and Preparation of Electrode Catalysts

AbstractA novel Zn−Fe flow battery featuring an Fe3+ reduction reaction (Fe3+RR)‐coupled zinc oxidation, and an Fe2+ oxidation reaction (Fe2+OR)‐coupled hydrogen evolution reaction (HER) system as well, was established. This battery is capable of driving two Fe2+OR‐coupled HER systems in series based on the above Fe2+/Fe3+ cycling, for efficient self‐powered hydrogen evolution. Meanwhile, this Fe2+/Fe3+ cycling enables the preparation of a multifunctional catalyst, Pt‐3@SXNS (siloxene nanosheet), by the Fe2+OR‐promoted dispersion of Pt nanoparticles on SXNS; alternatively, this support could be obtained by Fe3+RR‐assisted exfoliation using Fe3+ from the anolyte of Fe2+OR‐coupled HER. The Pt‐3@SXNS catalyst exhibits excellent catalytic activities toward Fe3+RR in the Zn−Fe flow battery, HER, and Fe2+OR in the electrolyzer, which is attributed to the strong electronic interaction between Pt and Si. This work offers a new strategy for energy storage and low‐cost hydrogen production from acidic wastewater.

Fe2+ /Fe3+ Cycling for Coupling Self-Powered Hydrogen Evolution and Preparation of Electrode Catalysts.

A novel Zn-Fe flow battery featuring an Fe3+ reduction reaction (Fe3+ RR)-coupled zinc oxidation, and an Fe2+ oxidation reaction (Fe2+ OR)-coupled hydrogen evolution reaction (HER) system as well, was established. This battery is capable of driving two Fe2+ OR-coupled HER systems in series based on the above Fe2+ /Fe3+ cycling, for efficient self-powered hydrogen evolution. Meanwhile, this Fe2+ /Fe3+ cycling enables the preparation of a multifunctional catalyst, Pt-3@SXNS (siloxene nanosheet), by the Fe2+ OR-promoted dispersion of Pt nanoparticles on SXNS; alternatively, this support could be obtained by Fe3+ RR-assisted exfoliation using Fe3+ from the anolyte of Fe2+ OR-coupled HER. The Pt-3@SXNS catalyst exhibits excellent catalytic activities toward Fe3+ RR in the Zn-Fe flow battery, HER, and Fe2+ OR in the electrolyzer, which is attributed to the strong electronic interaction between Pt and Si. This work offers a new strategy for energy storage and low-cost hydrogen production from acidic wastewater.

Revealing the role of Ni2+ ions in inducing the synthesis of porous carbon balls: A novel substrate to enhance the Pt catalytic activity towards methanol-oxidation

Carbon-based materials have been often employed as electrocatalytic substrates because of their large surface area/highly porous structure. Similar to carbon substrates, the non-carbon related materials such as transition metals also play an important role in improving catalytic performance. However, the simultaneous synthesis and metallic functionalization of carbon substrates is a highly challenging issue. Herein, a hydrothermal method has been used for the preparation of Ni-functionalized porous carbon balls. The significant role of Ni2+ ions in the synthesis of porous carbon balls has been confirmed. The results of transmission electron microscopy indicate that, the as-prepared porous carbon balls were suitable for the dispersion of Pt nanoparticles with small particle size (less than 4 nm). In addition to providing the OHads species, the Ni can also modify the surface electronic structure of Pt. Electrochemical measurements results reveal that, under the strong interactions between Ni and Pt, the as-prepared porous carbon balls supported Pt nanoparticles (Pt/Ni-CB) catalyst possesses excellent electrocatalytic activity, stability and CO anti-poisoning capability towards methanol electrooxidation reaction (MOR). This work opens a novel idea for the construction of the metal functionalization of carbon substrates and their subsequent applications in other electrocatalytic reactions.