渣油催化临氢热转化钼铁双金属催化剂的研究

Replacement of precious single metal catalysts with cost-effective, highly-dispersed composite catalysts for catalytic hydrothermal conversion of residue holds tremendous promise for the residue upgrading technologies. Organic metals were added to the feed as the oil-soluble precursors, and transformed into the catalytic active phases in this work. Physical properties and structures of the composite catalysts had been investigated by X-ray fluorescence spectroscopy, X-ray photoelectron spectroscopy, X-ray diffraction, scanning electron microscope and transmission electron microscopy. The composite catalysts were found to be highly efficient in the catalytic hydrothermal conversion of both model compound and residue. Increased metal dispersion and synergistic effects of two metals played indispensable roles in such catalytic system. Results showed that under the test conditions in the article, the catalyst had the best catalytic performance when the mass ratio of molybdenum to iron was 1.5.     

The significant promotion of g-C3N4 on Pt/CNS catalyst for the electrocatalytic oxidation of methanol

This article reported a series of g–C₃N₄–CNS (g-C₃N₄ and carbon nanosheets) composite carriers formed by the hydrothermal method, and then the ethylene glycol reduction method was used to anchor Pt nanoparticles on the g–C₃N₄–CNS carrier to form the Pt/g–C₃N₄–CNS catalysts. The electrochemical test for the electrocatalytic oxidation of methanol (MOR) shown that the Pt/20%g–C₃N₄–CNS catalyst has the best catalytic performance and stability. These Pt/g–C₃N₄–CNS catalysts were analyzed by TEM, XRD, XPS, and BET characterization. It is discovered that the amount of g-C₃N₄ greatly influenced the structure and chemical properties of Pt/CNS precursor. As the content of g-C₃N₄ increases, the content of pyridine nitrogen and pyrrole nitrogen also increases, and N species can enhance the interaction between Pt nanoparticles and CNS, promote Pt dispersion, and increase the specific surface area of the catalyst. Similarly, an excessive addition of g-C₃N₄ will cause a sharp decline in the conductivity of the catalyst, and then led to the decline of MOR activity.     

Study of the effect of noble metal promotion in Ni-based catalyst for the Sabatier reaction

This paper reports the preparation and the evaluation of the performance of Ni-based powder catalysts with low nickel loading on the CO2 methanation reaction, that is an integral part of the power-to-gas (PtG) technology. CeO₂, CeZrO₄ and CeO₂/SiO₂ were selected as possible supports, and the results of this first screening pointed out that 10%Ni/CeO₂ catalyst could offer the best reaction performances because of ceria's peculiar characteristics. Moreover, the promotion of this promising formulation with the addition of a small amount of noble metals (Pt, Ru, Rh) was investigated, showing that platinum in particular can enhance the catalyst performances. A further study related to the noble metal loading pointed out that platinum and ruthenium have a different optimum loading condition: this result, together with the activity tests performed on monometallic formulations with only the noble metal, suggested that the two metals are able to catalyse two different reactions, thus promoting two different reaction mechanisms.     

Pt–Ru nanoparticles anchored on poly(brilliant cresyl blue) as a new polymeric support: Application as an efficient electrocatalyst in methanol oxidation reaction

The glassy carbon electrode is modified by poly(brilliant cresyl blue) (PBCB) to be applied as a new green and efficient platform for Pt and Pt–Ru alloy nanoparticles deposition. Surface composition, morphology and catalytic activity of these modified electrodes towards methanol oxidation are assessed by applying X-ray diffraction, field emission scanning electron microscopy, cyclic voltammetry and electrochemical impedance spectroscopy techniques. The X-ray diffraction patterns reveal that the highly crystalline Pt and Pt–Ru alloy and RuO₂ nanoparticles with low crystallinity are deposited on the PBCB modified glassy carbon electrodes. The microscopic images indicate smaller size and better distribution of deposited nanoparticles on the surface of PBCB modified electrodes. Cyclic voltammetry and electrochemical impedance spectroscopy results reveal that PBCB supported Pt and Pt–Ru nanoparticles have better electrocatalytic performance and durability towards methanol oxidation rather than the unsupported nanoparticles. From the obtained results it can be concluded that the presence of PBCB not only improves the stability of nanoparticles on the surface, but also leads to the formation of smaller size and more uniform distribution of nanoparticles on the surface, which, in turn, cause the nanoparticles to provide a higher accessible surface area and more active centers for the oxidation of methanol. The results will be valuable in extending the applications of this polymer in surface modification steps and in developing promising catalyst supports to be applied in direct methanol fuel cells.     

CO2 abatement and CH4 recovery at vehicle exhausts: Comparison and characterization of Ru powder and pellet catalysts

The catalytic conversion of CO₂ to CH₄ (Sabatier reaction) has been studied to develop an after-treatment process at vehicles exhausts. Three different formulations of Ru commercial catalysts, two in powder and one in pellets shape, were tested and characterized by means of X-ray powder diffraction, scanning electron microscopy (SEM-EDX), N₂ adsorption at −196 °C and temperature-programmed reduction (TPR).Experimental results show a high CO₂ conversion (X_CO2 = 0.96 @ T = 280 °C) for one powder catalyst formulation whereas the other one has maximum CO₂ conversion = 0.69. In both cases a high CH₄ selectivity is measured. High CO₂ conversion (X_CO2 = 0.92 @ T = 300 °C) is obtained also with pellet catalysts but only at lower GHSV values. The different behavior of the catalysts was ascribed to the different physicochemical properties and the key parameters for the application development of the process were identified. In particular, the possibility to use pellets or monolithic reactors, thus minimizing the pressure drops in the reactor, makes possible a commercial application in the treatment of vehicles exhausts.     

Investigation of flame spray synthesized La1-xSrxCoO3 perovskites with promotional catalytic performances on CO oxidation

To enhance the activity of catalysts for CO removal, the perovskite-type catalysts La_1-xSr_xCoO₃ (x = 0, 0.2, 0.4, 0.6, and 0.8) with different Sr²⁺ doping amount were synthesized by flame spray synthesis (FSS) method. The perovskite-type catalyst synthesized by FSS has a much larger specific surface area (SSA) than that prepared by other conventional methods. The SSA of catalyst increases with the increase of Sr²⁺ doping amount and the SSA of La_0.2Sr_0.8CoO₃ reaches 31.65 m²/g. Compared with other conventional methods, FSS method significantly improves the activity of catalyst and makes it close to the performances of catalysts with surface modification. The substitution of La³⁺ by Sr²⁺ promotes the generation of secondary phase Co₃O₄ and SrCO₃. The catalytic activity of La_1-xSr_xCoO₃ increases with the addition of Sr²⁺, which results from the increasing active sites and oxygen vacancies. Interestingly, La_0.4Sr_0.6CoO₃ performs the highest activity for CO oxidation and the CO conversion reaches 50% at 148.6 °C and 90% at 165.9 °C. The oxidation of CO over La_1-xSr_xCoO₃ catalyst may follow a combination of MvK and L-H mechanisms according to the experimental results of H₂-TPR. Moreover, the catalyst exhibits good catalytic activity in consecutive oxidation cycles. In consecutive oxidation experiments with La_0.4Sr_0.6CoO₃, the CO conversion reaches 50% at 168.8 °C and 90% at 197.8 °C in the eighth oxidation cycle. These results prove that FSS method can further improve the activity of catalysts and is suitable for the preparation of efficient catalysts.     

Effect of Supports and Promoters on the Performance of Ni-Based Catalysts in Ethanol Steam Reforming

Ethanol steam reforming (ESR) is one of the potential processes to convert ethanol into valuable products. Hydrogen produced from ESR is considered as green energy for the future and can be an excellent alternative to fossil fuels with the aim of mitigating the greenhouse gas effect. The ESR process has been well studied, using transition metals as catalysts coupled with both acidic and basic oxides as supports. Among various reported transition metals, Ni is an inexpensive material with activity comparable to that of noble metals, showing promising ethanol conversion and hydrogen yields. Additionally, different promoters and supports were utilized to enhance the hydrogen yield and the catalyst stability. This review summarizes and discusses the influences of the supports and promoters of Ni-based catalysts on the ESR process.     

Anchoring single Pt atoms on hollow Ag3VO4 spheres for improved activity towards photocatalytic H2 evolution reaction

The high cost of noble metal catalysts has been a great bottleneck for the catalyst industry. Using the noble metal at a single-atom level for catalytic applications could dramatically decrease the cost. The impacts of single Pt atoms on the photocatalytic performance of Ag₃VO₄ have been investigated and reported. In this report, single Pt atoms were anchored on the surface of Ag₃VO₄ (AVO) as a cocatalyst, and the resultant composite photocatalyst has been studied for photocatalytic H₂ production from water driven by visible light. The as-prepared AVO particles are hollow nanospheres in the monoclinic phase with a bandgap of 2.20 eV. The light absorption edge of AVO/Pt is slightly red-shifted compared to that of the pristine AVO, indicating more visible light absorption of AVO/Pt. The XPS peaks of Ag, V, and Pt exhibit a significant shift after AVO and Pt get into contact, suggesting the strong interaction between the surface Ag and V atoms, and single Pt atoms. After 3-h illumination, the photocatalytic H₂ evolution amount from AVO/Pt is improved up to 1400 μmol, which is 2.8 times that on the bare AVO. Such efficient photocatalytic H₂ evolution on AVO/Pt is still maintained after five reaction cycles. The better photocatalytic performance of AVO/Pt has been attributed to the more efficient visible light utilization and the lower interfacial charge transfer resistance, as demonstrated in the DRS and EIS spectra. The presence of the surface Pt atoms also leads to a higher amount of reactive radicals, which could efficiently promote the surface redox reactions.