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58 result(s) for "Mikkola, Jyri‐Pekka"
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Silicalite-Supported Ni Catalysts for Efficient CO2 Conversion into CH4
The catalytic conversion of CO2 into methane (CH4) offers a sustainable solution to the worsening global warming scenario, especially for controlling CO2 levels. This study reports silicalite-1 supported Ni catalysts with different loadings for CO2 conversion to CH4, prepared via wet impregnation. The X-ray diffraction pattern revealed an increase in crystallite size at higher Ni loadings, which was further supported by N2 sorption, where the specific surface area and microporosity of the catalysts were decreased. There was a slight shift in the reducibility of the catalysts, potentially indicating the impact of loading on dispersion and spatial distribution. The catalyst performance was evaluated over a range of temperatures at 5 bar and a GHSV of 20,000 mL gcat−1 h−1. Surprisingly, the Ni(5)@Silicalite-1 exhibited higher CO2 conversion efficiency across the range of temperatures compared to Ni(10)@Silicalite-1. The NiO(5)@Silicalite-1 demonstrated a maximum CO2 conversion of 88% at 450 °C, which was approximately 14% higher than that of the catalyst with a 10 wt.% loading. Notably, the CH4 selectivity pattern was quite identical across the catalysts, underscoring that the reaction pathways were unaffected by the loadings. The higher performance of NiO(5)@Silicalite-1 could be ascribed to smaller NiO crystallites and improved textural properties.
Supercapacitors and triboelectric nanogenerators based on electrodes of greener iron nanoparticles/carbon nanotubes composites
The development of supporting materials based on carbon nanotubes (CNTs) impregnated with iron nanoparticles via a sustainable and green synthesis employing plant extract of Punica granatum L. leaves was carried out for the iron nanoparticle modification and the following impregnation into the carbon nanotubes composites (CNT-Fe) that were also coated with polypyrrole (CNT-Fe + PPy) for use as electrode for supercapacitor and triboelectric nanogenerators. The electrochemical characterization of the materials by cyclic voltammetry (CV) and galvanostatic charge–discharge (GCD) assays revealed that the CNT-Fe + PPy gave rise to better performance due to the association of double-layer capacitance behavior of carbon derivative in association with the pseudocapacitance contribution of PPy resulting in an areal capacitance value 202 mF/ cm 2 for the overall composite. In terms of the application of electrodes in triboelectric nanogenerators, the best performance for the composite of CNT-Fe + PPy was 60 V for output voltage and power density of 6 μW/cm 2 . The integrated system showed that the supercapacitors can be charged directly by the nanogenerator from 0 to 42 mV in 300 s. The successful green synthesis of iron nanoparticles on CNT and further PPy coating provides a feasible method for the design and synthesis of high-performance SCs and TENGs electrode materials. This work provides a systematic approach that moves the research front forward by generating data that underpins further research in self-powered electronic devices.
Pd Supported IRMOF-3: Heterogeneous, Efficient and Reusable Catalyst for Heck Reaction
IRMOF-3 with a high surface area prepared by a hydrothermal method was used for deposition of Pd(OAc) 2 on IRMOF-3 particles. The final catalyst was characterized with FT-IR, nitrogen physisorption, thermogravimetry, scanning electron microscopy, transmission electron microscopy combined with energy dispersive X-ray analysis, wide angle X-ray diffraction spectroscopy and X-ray photoelectron spectroscopy. The prepared porous catalyst was effectively used in the Heck coupling reaction in the presence of an organic base. The reaction parameters such as the type of base, amounts of catalyst and solvents, temperature were optimized. The catalyst was then easily separated, washed, and reused 4 times without significant losses of catalytic activity. Graphical Abstract
Synthesis and Characterization of Palladium Supported Amino Functionalized Magnetic-MOF-MIL-101 as an Efficient and Recoverable Catalyst for Mizoroki–Heck Cross-Coupling
Magnetic particles were prepared by a hydrothermal method and then successively covered by Metal–Organic-Frameworks MIL-101-NH 2 with a high surface area. This was followed by deposition of Pd(OAc) 2 on Fe 3 O 4 –NH 2 @MIL-101-NH 2 particles. The final catalyst was characterized with FT-IR, nitrogen physisorption, thermogravimetry (TGA), scanning electron microscopy (SEM) combined with energy dispersive X-ray analysis (EDX), transmission electron microscopy (TEM), vibrating sample magnetometry (VSM), wide-angle X-ray diffraction spectroscopy (XRD) and X-ray photoelectron spectroscopy (XPS). The prepared magnetic catalyst was effectively used in the Heck coupling reaction in the presence of an inorganic base. The reaction parameters such as the base type, amounts of catalyst and solvents, temperature, and substrates ratios were optimized. The catalyst was then magnetically separated, washed, and reused 7 times without losing significantly catalytic activity. Graphic Abstract
Pd Nanoparticles Stabilized on the Cross-Linked Melamine-Based SBA-15 as a Catalyst for the Mizoroki–Heck Reaction
Mesoporous SBA-15 silicate with a high surface area was prepared by a hydrothermal method, successively modified by organic melamine ligands and then used for deposition of Pd nanoparticles onto it. The synthesized materials were characterized with infrared spectroscopy (FT-IR), thermogravimetric analysis (TGA), nitrogen physisorption, scanning electron microscopy (SEM) coupled with energy dispersive X-ray analysis (EDX), transmission electron microscopy (TEM), nuclear magnetic resonance (NMR) and inductively coupled plasma (ICP-OES). The catalyst was effectively used in the Mizoroki–Heck coupling reaction of various reactants in the presence of an organic base giving the desired products in a short reaction time and with small catalysts loadings. The reaction parameters such as the base type, amounts of catalyst, solvents, and the temperature were optimized. The catalyst was easily recovered and reused at least seven times without significant activity losses.Graphic Abstract
Photocatalytic reduction of CO2 with H2O over modified TiO2 nanofibers: Understanding the reduction pathway
Nanosized metal (Pt or Pd)-decorated TiO2 nanofibers (NFs) were synthesized by a wet impregnation method. CdSe quantum dots (QDs) were then anchored onto the metal-decorated TiO2 NFs. The photocatalytic performance of these catalysts was tested for activation and reduction of CO2 under UV-B light. Gas chromatographic analysis indicated the formation of methanol, formic acid, and methyl formate as the primary products. In the absence of CdSe QDs, Pd-decorated TiO2 NFs were found to exhibit enhanced performance compared to Pt-decorated TiO2 NFs for methanol production. However, in the presence of CdSe, Pt-decorated TiO2 NFs exhibited higher selectivity for methanol, typically producing -90 ppmg^-1.h^-1 methanol. The CO2 photoreduction mechanism is proposed to take place via a hydrogenation pathway from first principles calculations, which complement the experimental observations.
Microbial mineralization of cellulose in frozen soils
High-latitude soils store ~40% of the global soil carbon and experience winters of up to 6 months or more. The winter soil CO 2 efflux importantly contributes to the annual CO 2 budget. Microorganisms can metabolize short chain carbon compounds in frozen soils. However, soil organic matter (SOM) is dominated by biopolymers, requiring exoenzymatic hydrolysis prior to mineralization. For winter SOM decomposition to have a substantial influence on soil carbon balances it is crucial whether or not biopolymers can be metabolized in frozen soils. We added 13 C-labeled cellulose to frozen (−4 °C) mesocosms of boreal forest soil and followed its decomposition. Here we show that cellulose biopolymers are hydrolyzed under frozen conditions sustaining both CO 2 production and microbial growth contributing to slow, but persistent, SOM mineralization. Given the long periods with frozen soils at high latitudes these findings are essential for understanding the contribution from winter to the global carbon balance. High latitude soils can store around 40 % of the Earth’s soil carbon. Here, the authors add 13 C-labeled cellulose to frozen mesocosms of boreal forest soils and find that cellulose biopolymers are hydrolysed under frozen conditions and therefore contribute to the slow degradation of soil organic matter.
Robust hierarchical 3D carbon foam electrode for efficient water electrolysis
Herein we report a 3D heterostructure comprising a hierarchical macroporous carbon foam that incorporates mesoporous carbon nanotubes decorated with cobalt oxide nanoparticles as an unique and highly efficient electrode material for the oxygen evolution reaction (OER) in electrocatalytic water splitting. The best performing electrode material showed high stability after 10 h, at constant potential of 1.7 V vs. RHE (reversible hydrogen electrode) in a 0.1 M KOH solution and high electrocatalytic activity in OER with low overpotential (0.38 V vs RHE at 10 mA cm −2 ). The excellent electrocatalytic performance of the electrode is rationalized by the overall 3D macroporous structure and with the firmly integrated CNTs directly grown on the foam, resulting in a large specific surface area, good electrical conductivity, as well as an efficient electrolyte transport into the whole electrode matrix concurrent with an ability to quickly dispose oxygen bubbles into the electrolyte. The eminent properties of the three-dimensional structured carbon matrix, which can be synthesized through a simple, scalable and cost effective pyrolysis process show that it has potential to be implemented in large-scale water electrolysis systems.
Catalytic Hydrogenation of d-Xylose Over Ru Decorated Carbon Foam Catalyst in a SpinChem® Rotating Bed Reactor
In this work the activity of ruthenium decorated carbon foam (Ru/CF) catalyst was studied in three phase hydrogenation reaction of d-xylose to d-xylitol. The developed catalyst was characterized by using scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, inductively coupled plasma optical emission spectrometry and nitrogen adsorption–desorption measurement. Kinetic measurements were carried out in a laboratory scale pressurized reactor (Parr®) assisted by SpinChem® rotating bed reactor (SRBR), at pre-defined conditions (40–60 bar H2 and 100–120 °C). The study on the influence of reaction conditions showed that the conversion rate and selectivity of hydrogenation reaction of d-xylose was significantly affected by temperature. These results have been proved by a competitive kinetics model which was found to describe the behavior of the novel system (Ru/CF catalyst used together with the SRBR) very well. Besides, it was revealed that the catalytic activity as well as the stability of our Ru/CF-SRBR is comparable with the commercial ruthenium decorated carbon catalyst (Ru/AC) under identical reaction conditions. Moreover, all steps from catalyst preparation and catalyst recycling as well as catalytic testing can be performed in an easy, fast and elegant manner without any loss of materials. Briefly, the developed Ru/CF catalyst used together with the SRBR could be used an excellent alternative for the conventional Raney nickel catalyst in a slurry batch reactor and offers an attractive concept with obvious industrial applicability.
Efficient Adsorption and Catalytic Reduction of Phenol Red Dye by Glutaraldehyde Cross-Linked Chitosan and Its Ag-Loaded Catalysts: Materials Synthesis, Characterization and Application
In this study, glutaraldehyde cross-linked chitosan support, as well as the catalysts obtained after loading Ag metal (Ag/Chitosan), were synthesised and applied for adsorption and reduction of phenol red dye in an aqueous solution. The Ag/chitosan catalysts were characterised by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FT-IR) and inductively coupled plasma-optical emission spectrometry (ICP-OES) analysis techniques. The catalytic reduction and adsorption performance of phenol red dye with Ag/chitosan and cross-linked chitosan, respectively, was performed at ambient reaction conditions. The reduction of dye was carried out using sodium borohydride (NaBH4) as the reducing agent, while the progress of adsorption and reduction study was monitored with ultraviolet-visible (UV-vis) spectrophotometry technique. The reduction of the phenol red dye varied with the amount of catalyst, the concentration of NaBH4, Ag metal loading, reaction temperature, phenol red dye concentration and initial pH of the dye solution. The dye solution with a nearly-neutral pH (6.4) allowed efficient adsorption of the dye, while acidic (pH = 4) and alkaline (pH = 8, 11, 13.8) solutions showed incomplete or no adsorption of dye. The reusability of the Ag/chitosan catalyst was applied for the complete reduction of the dye, where no significant loss of catalytic activity was observed. Hence, the applicability of cross-linked chitosan and Ag/catalyst was thus proven for both adsorption and reduction of phenol red dye in an aqueous solution and can be applied for industrial wastewater treatment.