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1.
Metal-support interaction and catalyst pretreatment are important for industrial catalysis. This work investigated the effect of supports (SiO2, CeO2, TiO2 and ZrO2) for Cu–Pd catalyst with high Cu/Pd ratio (Cu/Pd = 33.5) regarding catalyst cost, and the reduction temperatures of 350 °C and 550 °C were compared. The activity based on catalyst weight follows the order of Si > Ce > Zr > Ti when reduced at 350 °C. The reduction temperature leads to the surface reconstruction over the SiO2, CeO2 and TiO2 catalysts, while results in phase transition over Cu–Pd/ZrO2. The effect of reduction temperature on catalytic performance is prominent for the SiO2 and ZrO2 supported catalysts but not for the CeO2 and TiO2 ones. Among the investigated catalysts, Zr-350 exhibits the highest methanol yield. This work reveals the importance of the supports and pretreatment conditions on the physical-chemical properties and the catalytic performance of the Cu–Pd bimetallic catalysts.  相似文献   
2.
《Ceramics International》2022,48(11):15056-15063
Hydrogen (H2) sensors based on metal oxide semiconductors (MOS) are promising for many applications such as a rocket propellant, industrial gas and the safety of storage. However, poor selectivity at low analyte concentrations, and independent response on high humidity limit the practical applications. Herein, we designed rGO-wrapped SnO2Pd porous hollow spheres composite (SnO2Pd@rGO) for high performance H2 sensor. The porous hollow structure was from the carbon sphere template. The rGO wrapping was via self-assembly of GO on SnO2-based spheres with subsequent thermal reduction in H2 ambient. This sensor exhibited excellently selective H2 sensing performances at 390 °C, linear response over a broad concentration range (0.1–1000 ppm) with recovery time of only 3 s, a high response of ~8 to 0.1 ppm H2 in a minute, and acceptable stability under high humidity conditions (e. g. 80%). The calculated detection limit of 16.5 ppb opened up the possibility of trace H2 monitoring. Furthermore, this sensor demonstrated certain response to H2 at the minimum concentration of 50 ppm at 130 °C. These performances mainly benefited from the special hollow porous structure with abundant heterojunctions, the catalysis of the doped-PdOx, the relative hydrophobic surface from rGO, and the deoxygenation after H2 reduction.  相似文献   
3.
Direct Ethanol Fuel Cells (DEFCs) have fascinated remarkable attention on account of their high current density and being environmentally friendly. Developing efficient and durable catalysts with a simple and fast method is a great challenge in the practical applications of DEFCs. To this end, the bimetallic Pd–Ag with adjustable Pd:Ag ratios were synthesized via a simple and one-pot strategy on activated carbon as a support in this study. The Pd–Ag/C catalysts with different molar ratios were synthesized by simultaneous reduction of Pd and Ag ions in the presence of the ethanolic sodium hydroxide as a green reducing agent for the first time. Several different methods, including FE-SEM, HR-TEM, XRD, XPS EDX, ICP-OES, and BET were used to confirm the structure and morphology of the catalysts. The performance of catalysts was also examined in ethanol oxidation. Obtained results of electrochemical experiments revealed that the Pd3–Ag1/C catalyst had superior catalytic activity (2911.98 mAmg?1Pd), durability, and long-stability compared to the other catalysts. The excellent catalytic characteristic can be attributed to the synergistic effect between Pd and Ag. We presume that our simple method have the chance to be utilized as a proper method for the synthesis of fuel cell catalysts.  相似文献   
4.
In the present research, nanostructured Pd–Cd alloy electrocatalysts with different compositions were produced using the electrodeposition process. The morphology of the samples was studied by scanning electron microscopy analysis. Also, the elemental composition of the samples was determined by energy-dispersive X-ray spectroscopy and elemental mapping tests. Tafel polarization and electrochemical impedance spectroscopy methods were employed to determine the electrochemical corrosion properties of the synthesized samples in a solution containing 0.5 M sulfuric acid and 0.1 M formic acid. The linear sweep voltammetry, cyclic voltammetry, and chronoamperometry techniques were also employed to evaluate the electrocatalytic activity of prepared samples toward the oxidation of formic acid. In this respect, the influence of some factors such as formic acid and sulfuric acid concentrations and also potential scan rate was investigated. Compared to the pure Pd sample, the Pd–Cd samples were more reactive for the oxidation of formic acid. Besides, the sample with a lower amount of Pd (Pd1·3Cd) demonstrated much higher electrocatalytic activity than the Pd7·1Cd and Pd2·1Cd samples. The observed high mass activity of 15.06 A mg?1Pd for the Pd1·3Cd sample which is 21.1 times higher than Pd/C is an interesting result of this study.  相似文献   
5.
A novel and high-efficiency Pd/TMxOy-rGO/CFP (TMxOy = Co3O4, Mn3O4, Ni(OH)2) electrocatalyst for directly integrated membrane electrode was synthesized by controllable cyclic voltammetry electrodeposition combined with hydrothermal process. The results showed excellent performance towards methanol oxidation reduction. The Pd/Co3O4-rGO/CFP as-prepared catalyst has the best electrocatalytic activity, and mass activity is 5181 mA·mg−1Pd, which is about 40 times and 4.3 times that of the commercial Pd/C and Pt/C catalyst (JM). It can be attributed that the small size of Pd nanoparticle, uniformity of distribution, and the synergistic interaction between transition metal oxide on the support surface and Pd nanoparticles. The prepared Pd/TMxOy-rGO/CFP composite electrode is a promising catalyst for integrated membrane electrode assembly of proton exchange membrane fuel cells in the future.  相似文献   
6.
Five hundred ppm Pd/CeO2 catalyst was prepared and evaluated in selective hydrogenation of acetylene in large excess of ethylene since ceria has been recently found to be a reasonable stand-alone catalyst for this reaction. Pd/CeO2 catalyst could be activated in situ by the feed gas during reactions and the catalyst without reduction showed much better ethylene selectivity than the reduced one in the high temperature range due to the formation of oxygen vacancies by reduction. Excellent ethylene selectivity of ~100% was obtained in the whole reaction temperature range of 50°C–200°C for samples calcined at temperatures of 600°C and 800°C. This could be ascribed to the formation of PdxCe1xO2−y or Pd-O-Ce surface species based on the X-ray diffraction and X-ray photoelectron spectroscopy results, indicating the strong interaction between palladium and ceria.  相似文献   
7.
8.
Pd catalysts supported on activated carbon (Pd/C–NH3) toward HCOOH dehydrogenation were prepared by a simple adsorption method using ammonia (NH3) and Ar as the working gas. The results show that the TOFinitial of Pd/C–NH3 was 459.8 h−1 at 50 °C. When the reaction was carried out for 4 h, the HCOOH dehydrogenation ratio over Pd/C–NH3 was about 81.2%, which was 1.15 and 1.13 times, respectively, as that of the as-prepared Pd/C catalyst without any treatment (Pd/C–As) and the Pd/C catalyst purchased from Sigma-Aldrich (Pd/C-CM). The total amount of H2 and CO2 produced by using Pd/C–NH3 to decompose HCOOH in the third cycle was 99.4% of the gas produced by the first reaction cycle, and 1.80 and 12.60 times, respectively, as that of Pd/C–As and Pd/C-CM. The characterization results indicated that the Pd active species in Pd/C–NH3 migrated to the outer surface of the carbon support during the reaction, and the pore volume of the carbon support became larger, which were beneficial to the reaction. These factors made Pd/C–NH3 exhibit excellent HCOOH dehydrogenation activity and stability. NH3 adsorption is a simple and effective method for preparing high-performance Pd/C HCOOH dehydrogenation catalysts, and has important guiding significance for the preparation of other carbon supported noble metal catalysts.  相似文献   
9.
Decomposition of formic acid biomass to generate hydrogen is vital for coping with fossil energy depletion, environmental pollution, and developing clean, efficient, safe, and sustainable modern energy system. In this study, a PdAu/C−C bimetallic catalyst was prepared by the co-impregnation method followed by an atmospheric pressure (AP) cold plasma treatment to synthesize PdAu/C−P catalysts. The resulting PdAu/C−P showed excellent catalytic activity for the formic acid dehydrogenation (FAD) reaction. The total volume of H2 and CO2 released from the FAD reaction was about 375 mL after 4 h at 50 °C, and the initial turnover frequency (TOFinitial) was 808.6 h−1. We used X−ray diffractometry (XRD), temperature programmed reduction (TPR) and high-resolution transmission electron microscopy (HRTEM) to show that plasma can effectively promote the redispersion of Pd−Au particles on the surface of the support. The average particle size of PdAu/C−P (3.5 ± 1.5 nm) was less than PdAu/C−C (4.4 ± 1.9 nm) and uniformly distributed. X-ray photoelectron spectroscopy (XPS), TPR, and HRTEM showed that PdAu/C−P has a higher degree of alloying. In addition, the strong electric field in the plasma facilitated more metal sites located on the outer surface of the support in PdAu/C−P, and the atomic ratio of M/C (M = Pd and Au) (0.0134) was much larger than that of PdAu/C−C (0.0060). The apparent activation energy (Ea) of PdAu/C−P for the FAD reaction was only 27.25 kJ mol−1, and it had much higher activity and stability than the commercial Pd/C (Sigma−Aldrich). The total volume of H2 and CO2 produced over the PdAu/C−P for three cycles was 1.33, 5.87, and 8.56 times that of commercial Pd/C. Overall, the cold plasma enhanced the degree of alloying, promoted the redispersion of agglomerated particles, and regulated the surface enrichment of the active metal components. This is of great significance for guiding the preparation of high−performance multi-metal catalysts by cold plasma.  相似文献   
10.
Two-dimensional self-assembled nanostructures of palladium nanosheets are created during one-step strategies at room temperature. Palladium nanosheets are synthesized in the absence and presence of surfactant (CTAB) agent with the aim of considering the surfactant effect on the morphology and electrocatalytic activity of palladium nanosheets. In both reactions, carbon monoxide and acetic acid act as reducing agent and solvent, respectively. Both palladium nanosheets serve as two-dimensional advanced supportless electrocatalysts for oxidation of formic acid, and clarify higher mass activity and durability in comparison to the palladium anchored on carbon. The exceptional performance of both palladium nanosheets is ascribed to their self-support and huge surface area characteristics. Moreover, the paper well proves that the morphology and electrocatalytic efficiency of palladium nanosheets were seriously affected by the presence of surfactant. Palladium nanosheets synthesized in the absence and presence of surfactant display the flat and stack nanosheets with thicknesses of 3.48 and 4.22 nm, respectively. In addition, comparison of both palladium nanosheets demonstrates that palladium nanosheets synthesized in the absence of surfactant reflect better catalytic efficiency and durability. The presence and bonding of surfactant to the surface of palladium nanosheets lead to the occupancy of active sites and degradation of palladium nanosheets performance. We believe that these palladium nanosheets can be applied as advanced electrocatalysts for diverse applications, especially direct formic acid fuel cells.  相似文献   
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