Abstract:Reprocessing of spent nuclear fuel for the recovery of the fi ssionable materials (mainly uranium and plutonium), is performed by solvent extraction. Thermal oxide reprocessing (THORP) is the most widely used technique in which processing fl uids gradually degrade and form stable emulsions that are referred to as interfacial crud (IFC). IFC is highly viscous and stable and its deposition in the nuclear reprocessing circuit results in blockages and plant shutdown for the recovery of IFC and cleaning of the line… Show more
“…This results in "unconstrained" crystallite growth as discussed further in Section 3. 16. Figure 19 illustrates the porous structure of Ni/Si = 1/4 Mw-AB catalyst which was obtained from the microwave irradiation of catalyst/support precursor fluid at 1 kW followed by heat treatment at 600 °C (Method-C, Section 3.8).…”
Section: Scanning Electron Microscopy (Sem) Studiesmentioning
Abstract:A novel generic method of silica supported catalyst system generation from a fluid state is presented. The technique is based on the combined flow and radiation (such as microwave, thermal or UV) induced co-assembly of the support and catalyst precursors forming nano-reactors, followed by catalyst precursor decomposition. The transformation from the precursor to supported catalyst oxide state can be controlled from a few seconds to several minutes. The resulting nano-structured micro-porous silica supported catalyst system has a surface area approaching 300 m 2 /g and X-ray Diffraction (XRD)-based catalyst size controlled in the range of 1-10 nm in which the catalyst structure appears as lamellar sheets sandwiched between the catalyst support. These catalyst characteristics are dependent primarily on the processing history as well as the catalyst (Fe, Co and Ni studied) when the catalyst/support molar ratio is typically 0.1-2. In addition, Ca, Mn and Cu were used as co-catalysts with Fe and Co in the evaluation of the mechanism of catalyst generation. Based on extensive XRD, Scanning Electron Microscopy (SEM) and Transmission Electron Microscopy (TEM) studies, the micro-and nano-structure of the catalyst system were evaluated. It was found that the catalyst and silica support form extensive 0.6-2 nm thick lamellar sheets of 10-100 nm planar dimensions. In these lamellae, the alternate silica support and catalyst layer appear in the form of a bar-code structure. When these lamellae structures pack, they form the walls of a micro-porous catalyst system which typically has a density of 0.2 g/cm 3 . A tentative mechanism of catalyst nano-structure formation is provided based on the rheology and fluid mechanics of the catalyst/support precursor fluid as well as co-assembly nano-reactor formation during processing. In order to achieve these structures and characteristics, catalyst support must be in the form of silane coated silica nano-particles dispersed in water which also contains the catalyst precursor nitrate salt. This support-catalyst precursor fluid must have a sufficiently low viscosity but high elastic modulus (high extensional viscosity) to form films and bubbles when exposed to processing energy sources such as microwave, thermal, ultra-sound or UV-radiation or their combination. The micro-to-nano structures of the catalyst system are essentially formed at an early stage of energy input. It is shown that the primary particles of silica are transformed to a proto-silica particle state and form lamellar structures with the catalyst precursor. While the nano-structure is forming, water is evaporated leaving a highly porous solid support-catalyst precursor which then undergoes decomposition to form a silica-catalyst oxide system. The final catalyst system is obtained after catalyst oxide reduction. Although the XRD-based catalyst size changes slightly during the subsequent heat treatments, the nano-structure of the catalyst system remains substantially unaltered as evaluated through TEM images. Howev...
“…This results in "unconstrained" crystallite growth as discussed further in Section 3. 16. Figure 19 illustrates the porous structure of Ni/Si = 1/4 Mw-AB catalyst which was obtained from the microwave irradiation of catalyst/support precursor fluid at 1 kW followed by heat treatment at 600 °C (Method-C, Section 3.8).…”
Section: Scanning Electron Microscopy (Sem) Studiesmentioning
Abstract:A novel generic method of silica supported catalyst system generation from a fluid state is presented. The technique is based on the combined flow and radiation (such as microwave, thermal or UV) induced co-assembly of the support and catalyst precursors forming nano-reactors, followed by catalyst precursor decomposition. The transformation from the precursor to supported catalyst oxide state can be controlled from a few seconds to several minutes. The resulting nano-structured micro-porous silica supported catalyst system has a surface area approaching 300 m 2 /g and X-ray Diffraction (XRD)-based catalyst size controlled in the range of 1-10 nm in which the catalyst structure appears as lamellar sheets sandwiched between the catalyst support. These catalyst characteristics are dependent primarily on the processing history as well as the catalyst (Fe, Co and Ni studied) when the catalyst/support molar ratio is typically 0.1-2. In addition, Ca, Mn and Cu were used as co-catalysts with Fe and Co in the evaluation of the mechanism of catalyst generation. Based on extensive XRD, Scanning Electron Microscopy (SEM) and Transmission Electron Microscopy (TEM) studies, the micro-and nano-structure of the catalyst system were evaluated. It was found that the catalyst and silica support form extensive 0.6-2 nm thick lamellar sheets of 10-100 nm planar dimensions. In these lamellae, the alternate silica support and catalyst layer appear in the form of a bar-code structure. When these lamellae structures pack, they form the walls of a micro-porous catalyst system which typically has a density of 0.2 g/cm 3 . A tentative mechanism of catalyst nano-structure formation is provided based on the rheology and fluid mechanics of the catalyst/support precursor fluid as well as co-assembly nano-reactor formation during processing. In order to achieve these structures and characteristics, catalyst support must be in the form of silane coated silica nano-particles dispersed in water which also contains the catalyst precursor nitrate salt. This support-catalyst precursor fluid must have a sufficiently low viscosity but high elastic modulus (high extensional viscosity) to form films and bubbles when exposed to processing energy sources such as microwave, thermal, ultra-sound or UV-radiation or their combination. The micro-to-nano structures of the catalyst system are essentially formed at an early stage of energy input. It is shown that the primary particles of silica are transformed to a proto-silica particle state and form lamellar structures with the catalyst precursor. While the nano-structure is forming, water is evaporated leaving a highly porous solid support-catalyst precursor which then undergoes decomposition to form a silica-catalyst oxide system. The final catalyst system is obtained after catalyst oxide reduction. Although the XRD-based catalyst size changes slightly during the subsequent heat treatments, the nano-structure of the catalyst system remains substantially unaltered as evaluated through TEM images. Howev...
“…PolyHIPE Polymers can be chemically and biologically functionalized [16][17][18][19][20] in order to achieve mimicking of nature's processing strategy and applied to tissue engineering, bioprocess intensification, and agroprocess intensification. Furthermore, nonbiological functionalization processes were used for specific applications such as separation processes [21], fast response ion-exchange resins [22], and environmental and energy conversion processes [23].…”
Section: Polyhipe Polymers As Monolithic Microreactors and Asmentioning
Monolithic nanostructured metallic porous structures with a hierarchy of pore size ranging from ca. 10 m to 1 nm are processed for use as microreactors. The technique is based on flow induced electroless deposition of metals on a porous template known as PolyHIPE Polymer. The process is conducted in a purpose built flow reactor using a processing protocol to allow uniform and efficient metal deposition under flow. Nickel chloride and sodium hypophosphite were used as the metal and reducing agent, respectively. Electroless deposition occurs in the form of grains with a composition of Ni P in which the grain size range was ca. 20-0.2 m depending on the composition of the metal deposition solution. Structure formation in the monoliths starts with heat treatment above 600 ∘ C resulting in the formation of a 3-dimensional network of capillary-like porous structures which form the walls of large arterial pores. These monoliths have a dense but porous surface providing mechanical strength for the monolith. The porous capillary-like arterial pore walls provide a large surface area for any catalytic activity. The mechanisms of metal deposition and nanostructure formation are evaluated using scanning electron microscopy, energy dispersive X-ray analysis, XRD, BET-surface area, and mercury intrusion porosimetry.
“…Due to these attributes, PHPs and their metallic, ceramic or composite forms have been used in the emerging technology of Process Intensification (PI), which facilitates the establishment of green processes. In addition to use of PHPs in analytical sciences, the important specific applications of PHPs in PI include: Agro‐PI, Bio‐PI, Chemical‐PI, including Separation processes, Energy and Environmental‐PI, and medicine and tissue engineering . A recent review of some of these applications is available…”
Section: Introductionmentioning
confidence: 99%
“…In most of the large scale applications of PHPs, such as agriculture and separation and energy‐environmental processes, the bulk and surface functionality of PHP requires ion‐exchange capacity. The required anionic or cationic characteristics are dictated by the nature of the application.…”
Section: Introductionmentioning
confidence: 99%
“…The most important difference between the commercial and PHP‐based ion‐exchangers is the accessibility of the ion‐exchange sites in PHP which accelerates the exchange kinetics and allows the utilization of full exchange capacity.…”
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