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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 1,333 records · Page 74
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Dry reforming of methane over Ni supported on LaMnO 3 thin films

Thin films of LaMnO 3 were deposited onto MgAl 2 O 4 by Atomic Layer Deposition (ALD) and studied as supports for Ni in the Dry Reforming of Methane (DRM). Scanning Transmission Electron Microscopy (STEM) with Energy-Dispersive X-ray Spectroscopy (EDS) demonstrated that LaMnO 3 covered the support uniformly, and X-ray diffraction (XRD) showed that the LaMnO 3 films maintained their perovskite structure after 5 redox cycles at 1073 K. The Ni also remained well dispersed after 5 redox cycles at 1073 K. The LaMnO 3 -supported catalyst was more active than Ni on the unmodified MgAl 2 O 4 and showed superior resistance against coke formation. Lastly, the results for Ni on the LaMnO 3 films are compared to previous results for Ni on LaFeO 3 , CaTiO 3 , SrTiO 3 , and BaTiO 3 films.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Molecular structure and catalytic promotional effect of Mn on supported Na 2 WO 4 /SiO 2 catalysts for oxidative coupling of methane (OCM) reaction

The structure and promotional effect of Mn in supported Mn-Na 2 WO 4 /SiO 2 catalysts for the oxidative coupling of methane (OCM) reaction has been debated for a longtime in the literature. In the current investigation, with the aid of multiple in-situ characterization studies, we show that the freshly calcined supported 1.2Mn-5Na 2 WO 4 /SiO 2 catalyst possesses crystalline Na 2 WO 4 , Mn 2 O 3 and SiO 2 (cristobalite phase) along with surface MnO x and Na-WO x sites at low temperature and oxidizing environments. Under the OCM reaction environment (T>800°C), the crystalline Na 2 WO 4 phase melts and Mn 2 O 3 phase reduces. In contrast, the surface MnO x and Na-WO x sites exhibit excellent thermal and chemical stability. Exposure of the 1.2Mn-5Na 2 WO 4 /SiO 2 catalyst to the OCM reaction environment redisperses the molten Na 2 WO 4 phase on the SiO 2 support to form new surface WO x sites. Interestingly, the stable MnO x species interacts with both molten Na 2 WO 4 phase and surface Na-WO x sites during OCM reaction. Controlled transient kinetic experiments in TAP and detailed steady state OCM fixed-bed reaction studies reveal the role and promotional effect of Mn in the 1.2Mn-5Na 2 WO 4 /SiO 2 catalyst. The W-oxides (both molten Na 2 WO 4 and surface Na-WO x sites) are the active sites for the catalytic OCM reaction and the MnO x species only function as promoters. The promotion of MnO x strongly depends on the gas phase O 2 partial pressure and the MnO x species act as mediators for oxygen exchange between the gas phase molecular O 2 and catalyst lattice oxygen. In conclusion, the temperature dependent MnO x promotion reveals that the MnO x species selectively promote the molten Na 2 WO 4 phase at lower reaction temperature and the surface Na-WO x sites at higher temperature.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Highly efficient Pt catalyst on newly designed CeO 2 -ZrO 2 -Al 2 O 3 support for catalytic removal of pollutants from vehicle exhaust

Pt-CeO 2 catalysts have been widely studied for the vehicle emission control. Designing novel CeO 2 based supports with improved physical-chemical properties has become a research hotspot to further promote the catalytic performance and stability of Pt-CeO 2 catalysts. In this work, through utilizing a unique, two-step incipient wetness impregnation (T-IWI) method for ceria-zirconia-alumina (CZA-T) support preparation, a Pt single site catalyst (Pt/CZA-T) with excellent thermal stability was synthesized. Higher oxidation activity and Oxygen storage capacity (OSC) were achieved on activated Pt/CZA-T, comparing to Pt catalysts on regular CeO 2 /Al 2 O 3 (Pt/CA) and one-step prepared CeZrO x /Al 2 O 3 (Pt/CZA). Via the modification of hydrophilic/hydrophobic properties of γ-Al 2 O 3 by this unique T-IWI method, finer Ce 0.9 Zr 0.1 O 2 particles with higher density of surface defects were formed on CZA-T, on which a higher Pt dispersion and stronger Pt-O-Ce interaction were achieved. Upon activation, smaller, well-dispersed Pt clusters on CZA-T were generated. It was concluded that the CO oxidation performance and OSC were highly related to the size of Pt clusters on different supports that we have developed. Finally, more Pt sites located at Pt cluster-CeZrO x interfaces, which were the real active sites, were responsible for the highest OSC function and CO oxidation activity of activated Pt/CZA-T catalyst.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Experimental and Computational Studies of the Production of 1,3-Butadiene from 2,3-Butanediol Using SiO2-Supported H3PO4 Derivatives

Silica-supported phosphoric acid and metal phosphate catalyzed 1,3-butadiene (BDE) production from 2,3-butanediol (2,3-BDO) was studied using experimental and computational techniques. The catalyst was initially tested in a continuous flow reactor using commercially available 2,3-BDO, leading to maximum BDE yields of 63C%. Quantum chemical mechanistic studies revealed 1,2-epoxybutane is a kinetically viable and thermodynamically stable intermediate, supported by experimental demonstration that this epoxide can be converted to BDE under standard reaction conditions. Newly proposed E2 and SN2' elementary steps were studied to rationalize the formation of BDE and all detected side-products. Additionally, using quantum mechanics/molecular mechanics (QM/MM) calculations, we modeled silica-supported phosphate catalysts to study the effect of the alkali metal center. Natural population analysis showed that phosphate oxygen atoms are more negatively charged in CsH2PO4/SiO2 than in H3PO4/SiO2. In combination with temperature-programmed desorption experiments using CO2, the results of this study suggest that the improved selectivity achieved when adding the metal center is related to an increase in the basicity of the catalyst.

butadiene↗
DOE OSTI2024

Acetylene ligands stabilize atomically dispersed supported rhodium complexes under harsh conditions

Facile sintering of atomically dispersed supported noble metal catalysts at catalytically relevant temperatures, particularly under reducing conditions, poses a challenge for their practical applications. Some ligands, such as carbonyls, aid in improving the stability at the expense of severely suppressing the catalytic activity. In this work, we demonstrate that substitution of the carbonyl ligands with reactive acetylene ligands can maintain the atomic dispersion of the supported mononuclear rhodium complex under harsh reducing conditions (>573 K), as confirmed by in-situ X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) spectroscopies. In contrast, the supported rhodium carbonyl complex aggregates into nanoclusters under identical conditions. Furthermore, our results indicate that the acetylene ligands provide this anti-sintering ability while retaining the hydrogenation activity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Assessing metal nitrides and metal carbides as supports for thermally stable single-atom catalysts

Single-atom catalysts supported on metal oxides have been demonstrated to exhibit exceptional activity while also maintaining single-atom stability. However, alternative supports such as metal nitrides and carbides have received far less attention. Herein, we use density functional theory to systematically investigate the relative thermal stability of single-atom catalysts over a host of transition metal nitride and carbide supports. By considering the binding and dimerization energies of isolated transition metal atoms across various surface facets, we identify transition metal/support pairs that show the most promise for high-density single-atom catalysts. We find that transition metal atoms can be stabilized on both defect sites and pristine surfaces over transition metal nitrides and carbides. Furthermore, we identify promising metal/support pairings that may be suitable for achieving both stable and high-density single-atom catalysts. Furthermore, these results provide valuable insights to guide synthesis efforts towards achieving stable single-atom transition metal catalysts.

Density functional theory↗
DOE OSTI2025

Plastic-waste hydrogenolysis over two-dimensional MXene-supported ruthenium catalysts with tunable interlayer spacing

The hydrogenolysis of plastics is limited by active-site inaccessibility and inefficient mass transport of bulky polymer chains. To overcome these challenges, this work developed two-dimensional MXene-supported Ru (Ru@MXene) catalysts. Lyophilization of a solution containing dispersed MXene sheets and Ru precursors enabled the confinement of Ru species within the MXene interlayers, which act as pillars to expand the interlayer spacing. Building on this, a silica-pillared MXene-supported Ru (Ru@P-MXene) with even larger interlayer spacing exhibited a reaction rate of 914.9 g C5–C35 g Ru –1 h –1 for the hydrogenolysis of low-density polyethylene (LDPE) into valuable liquid chemicals (e.g., C 5 –C 35 ). A comparison of product yields between Ru@P-MXene and Ru@MXene suggests that elongated Ru particles confined within the MXene support expose their side facets for the reaction. In conclusion, this work demonstrates a new application of MXene in thermochemical catalysis, offering a solution to the challenges of active-site accessibility, mass transport, and reaction confinement in chemical plastic upcycling.

2D materials↗
DOE OSTI2013

A decision-support system for sustainable urban metabolism in Europe

Urban metabolism components define the energy and material exchanges within a city and, therefore, can provide valuable information on the environmental quality of urban areas. Assessing the potential impact of urban planning alternatives on urban metabolism components (such as energy, water, carbon and pollutants fluxes) can provide a quantitative estimation of their sustainability performance. Urban metabolism impact assessment can, therefore, contribute to the identification of sustainable urban structures with regards, for example, to building types, materials and layout, as well as to location and capacity of transportation and infrastructural developments. In this way, it enables the formulation of planning and policy recommendations to promote efficient use of resources and enhance environmental quality in urban areas. The European FP7 project BRIDGE (sustainaBle uRban plannIng Decision support accountinG for urban mEtabolism) has developed a decision-support system (DSS) that systematically integrates urban metabolism components into impact assessment processes with the aim of accurately quantifying the potential effects of proposed planning interventions. The DSS enables integration of multiple spatial and non-spatial datasets (e.g. physical flows of energy and material with variables of social and economic change) in a systematic manner to obtain spatially defined assessment results and to thus inform planners and decision-makers. This multi-criteria approach also enables incorporation of stakeholders' perceptions in order to prioritise decisive assessment criteria. This paper describes the methodological framework used to develop the DSS and critically examines the results of its practical application in five European cities. - Highlights: Black-Right-Pointing-Pointer Urban metabolism in sustainability assessment of planning alternatives. Black-Right-Pointing-Pointer European FP7 project applied to 5 real life case studies across Europe. Black-Right-Pointing-Pointer Decision support system enables incorporating scientific knowledge into planning. Black-Right-Pointing-Pointer Scale, data availability and stakeholder representativeness limit its application.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2015

Web tools concerning performance analysis and planning support for solar energy plants starting from remotely sensed optical images

We present innovative web tools, developed also in the frame of the FP7 ENDORSE (ENergy DOwnstReam SErvices) project, for the performance analysis and the support in planning of solar energy plants (PV, CSP, CPV). These services are based on the combination between the detailed physical model of each part of the plants and the near real-time satellite remote sensing of incident solar irradiance. Starting from the solar Global Horizontal Irradiance (GHI) data provided by the Monitoring Atmospheric Composition and Climate (GMES-MACC) Core Service and based on the elaboration of Meteosat Second Generation (MSG) satellite optical imagery, the Global Tilted Irradiance (GTI) or the Beam Normal Irradiance (BNI) incident on plant's solar PV panels (or solar receivers for CSP or CPV) is calculated. Combining these parameters with the model of the solar power plant, using also air temperature values, we can assess in near-real-time the daily evolution of the alternate current (AC) power produced by the plant. We are therefore able to compare this satellite-based AC power yield with the actually measured one and, consequently, to readily detect any possible malfunctions and to evaluate the performances of the plant (so-called “Controller” service). Besides, the same method can be applied to satellite-based averaged environmental data (solar irradiance and air temperature) in order to provide a Return on Investment analysis in support to the planning of new solar energy plants (so-called “Planner” service). This method has been successfully applied to three test solar plants (in North, Centre and South Italy respectively) and it has been validated by comparing satellite-based and in-situ measured hourly AC power data for several months in 2013 and 2014. The results show a good accuracy: the overall Normalized Bias (NB) is − 0.41%, the overall Normalized Mean Absolute Error (NMAE) is 4.90%, the Normalized Root Mean Square Error (NRMSE) is 7.66% and the overall Correlation Coefficient (CC) is 0.9538. The maximum value of the Normalized Absolute Error (NAE) is about 30% and occurs for time periods with highly variable meteorological conditions. - Highlights: • We developed an online service (Controller) dedicated to solar energy plants real-time monitoring • We developed an online service (Planner) that supports the planning of new solar energy plants • The services are based on the elaboration of satellite optical imagery in near real-time • The validation with respect to in-situ measured hourly AC power data for three test solar plants shows good accuracy • The maximum value of the Normalized Absolute Error is about 30% and occurs for highly variable meteorological conditions.

14 SOLAR ENERGY↗
DOE OSTI2025

Palm oil deoxygenation with glycerol as a hydrogen donor for renewable fuel production using nickel-molybdenum catalysts: The effect of support

Palm oil, one of the most widely used vegetable oils, offers significant potential as a sustainable feedstock for biofuel production. This study explores the deoxygenation of palm oil using glycerol as a hydrogen donor, with nickel-molybdenum (NiMo) catalysts supported on commercial alumina (Al 2 O 3 ), and zeolite (HZSM-5) comparing with self-prepared zirconia (ZrO 2 ). The catalysts were synthesized via incipient wetness impregnation and evaluated for their performance in biofuel production. NiMo/Al 2 O 3 exhibited the lowest oxygen removal efficiency (68.5 %), while NiMo/HZSM-5 achieved a higher oxygen removal (74.3 %) but also demonstrated the highest coke formation. The type of support material influenced the resulting biofuel range, with NiMo/HZSM-5 and NiMo/ZrO 2 favoring jet fuel production, whereas NiMo/Al 2 O 3 was more suitable for diesel production. Notably, NiMo/ZrO 2 exhibited the highest performance in palm oil deoxygenation while minimizing coke formation. These findings highlight NiMo/ZrO 2 as a promising catalyst for efficient and stable biofuel production, with the support material significantly influencing product yield and fuel quality.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Optimization of metal-supported solid oxide electrolysis cells with infiltrated catalysts

We report metal-supported solid oxide electrolysis cells (MS-SOECs) are being developed for steam-to-hydrogen electrolysis, especially for utilization of dynamic or intermittent electrical power from renewable sources. Various aspects of the electrocatalyst processing and composition, and metal support structure were explored. Catalyst materials, infiltration temperature and infiltration cycles were optimized for high performance and durability. Numerous catalyst materials were screened for both oxygen and steam electrodes. The oxygen catalyst had moderate impact on both initial cell performance and durability. Reducing Ni content in the steam electrode had little effect on durability, but reduced initial performance. Ex-situ XRD analysis and cell assessment of catalyst infiltration temperature revealed that the optimal range is 750–850 °C. The best cell performance and durability was achieved with LSCF-SDC oxygen electrocatalyst and SDC-Ni (60:40 vol%) steam electrocatalyst infiltrated 11 times at 800 °C and operated at 700 °C. At low steam content, a significant mass transport limitation on the steam side results in limiting current behavior. Thinner and more porous metal supports were implemented, and found to improve steam mass transport at low steam content, relevant for SOECs operating under high H 2 recycle rate or high steam utilization.

08 HYDROGEN↗
DOE OSTI2014

Interactive Decision-Support Tool for Risk-Based Radiation Therapy Plan Comparison for Hodgkin Lymphoma

Purpose: To present a novel tool that allows quantitative estimation and visualization of the risk of various relevant normal tissue endpoints to aid in treatment plan comparison and clinical decision making in radiation therapy (RT) planning for Hodgkin lymphoma (HL). Methods and Materials: A decision-support tool for risk-based, individualized treatment plan comparison is presented. The tool displays dose–response relationships, derived from published clinical data, for a number of relevant side effects and thereby provides direct visualization of the trade-off between these endpoints. The Quantitative Analyses of Normal Tissue Effects in the Clinic reports were applied, complemented with newer data where available. A “relevance score” was assigned to each data source, reflecting how relevant the input data are to current RT for HL. Results: The tool is applied to visualize the local steepness of dose–response curves to drive the reoptimization of a volumetric modulated arc therapy treatment plan for an HL patient with head-and-neck involvement. We also use this decision-support tool to visualize and quantitatively evaluate the trade-off between a 3-dimensional conformal RT plan and a volumetric modulated arc therapy plan for a patient with mediastinal HL. Conclusion: This multiple-endpoint decision-support tool provides quantitative risk estimates to supplement the clinical judgment of the radiation oncologist when comparing different RT options.

62 RADIOLOGY AND NUCLEAR MEDICINE↗
DOE OSTI2016

Enhanced Optical Head Tracking for Cranial Radiation Therapy: Supporting Surface Registration by Cutaneous Structures

Purpose: To support surface registration in cranial radiation therapy by structural information. The risk for spatial ambiguities is minimized by using tissue thickness variations predicted from backscattered near-infrared (NIR) light from the forehead. Methods and Materials: In a pilot study we recorded NIR surface scans by laser triangulation from 30 volunteers of different skin type. A ground truth for the soft-tissue thickness was segmented from MR scans. After initially matching the NIR scans to the MR reference, Gaussian processes were trained to predict tissue thicknesses from NIR backscatter. Moreover, motion starting from this initial registration was simulated by 5000 random transformations of the NIR scan away from the MR reference. Re-registration to the MR scan was compared with and without tissue thickness support. Results: By adding prior knowledge to the backscatter features, such as incident angle and neighborhood information in the scanning grid, we showed that tissue thickness can be predicted with mean errors of <0.2 mm, irrespective of the skin type. With this additional information, the average registration error improved from 3.4 mm to 0.48 mm by a factor of 7. Misalignments of more than 1 mm were almost thoroughly (98.9%) pushed below 1 mm. Conclusions: For almost all cases tissue-enhanced matching achieved better results than purely spatial registration. Ambiguities can be minimized if the cutaneous structures do not agree. This valuable support for surface registration increases tracking robustness and avoids misalignment of tumor targets far from the registration site.

62 RADIOLOGY AND NUCLEAR MEDICINE↗
DOE OSTI2012

Substrate inhibition in the heterogeneous catalyzed aldol condensation: A mechanistic study of supported organocatalysts

In this study, we demonstrate how materials science can be combined with the established methods of organic chemistry to find mechanistic bottlenecks and redesign heterogeneous catalysts for improved performance. By using solid-state NMR, infrared spectroscopy, surface and kinetic analysis, we prove the existence of a substrate inhibition in the aldol condensation catalyzed by heterogeneous amines. We show that modifying the structure of the supported amines according to the proposed mechanism dramatically enhances the activity of the heterogeneous catalyst. We also provide evidence that the reaction benefits significantly from the surface chemistry of the silica support, which plays the role of a co-catalyst, giving activities up to two orders of magnitude larger than those of homogeneous amines. This study confirms that the optimization of a heterogeneous catalyst depends as much on obtaining organic mechanistic information as it does on controlling the structure of the support.

36 MATERIALS SCIENCE↗
DOE OSTI2014

One- and three-dimensional silver(I)-5-sulfosalicylate coordination polymers having ligand-supported and unsupported argentophilic interactions

Four new coordination polymers, namely, (Hemim·[Ag(Hssa)(H{sub 2}O)]){sub n} (1), ([Ag(ina){sub 2} Ag(Hssa)]·CH{sub 3}OH·H{sub 2}O){sub n} (2), ([Ag{sub 2}(Hssa)(dmp){sub 1.5}]·2H{sub 2}O){sub n} (3) and [Ag{sub 2}(Hssa)(daoc)]{sub n} (4) (Hssa: 5-Sulfosalicylate, emim: 2-ethyl-4-methylimidazole, ina: isonicotinamide, dmp: 2,5-dimethylpyrazine and daoc: 1,8-diaminooctane) were synthesized and characterized by IR spectroscopy, elemental analysis, single crystal X-ray diffraction, powder X-ray diffraction (PXRD) and thermal analysis techniques. Complexes 1 and 2 are one-dimensional (1D) coordination polymers while complexes 3 and 4 are three-dimensional (3D) coordination polymers. Complex 3 consists of three dimensional (3D) 3,3,6-c net with 3,3,6T37 topology. Complex 4 exhibits a 2-fold interpenetrating 3D framework with tfc topology. Complexes 1–4 contain ligand-supported (1–3) and unsupported (4) argentophilic Ag⋯Ag interactions. Photoluminescence spectra of the complexes demonstrate that photoluminescent properties may be attributed to intraligand transition of coordinated Hssa ligand. - Graphical abstract: In this study, four new Ag(I)-coordination polymers with 5-sulfosalicylate and some N-donor ligands were synthesized and characterized. Complexes 1 and 2 are one-dimensional (1D) coordination polymers while complexes 3 and 4 are three-dimensional (3D) coordination polymers. Complex 3 consists of three dimensional (3D) 3,3,6-c net with 3,3,6T37 topology. Complex 4 exhibits a 2-fold interpenetrating 3D framework with tfc topology. The complexes 1–4 contain ligand-supported (1–3) and unsupported (4) argentophilic Ag⋯Ag interactions. Photoluminescence spectra of the complexes demonstrated that photoluminescent properties may be attributed to intraligand transition of coordinated Hssa ligand. - Highlights: • Four novel Ag(I)-coordination polymers with 5-sulfosalicylate and N-donor ligands. • Complexes 1–4 contain ligand-supported (1–3) and unsupported (4) argentophilic Ag⋯Ag interactions. • Photoluminescent properties of the complexes may be attributed to intraligand transition of coordinated Hssa ligand.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

A color-tunable luminescent material with functionalized graphitic carbon nitride as multifunctional supports

A color-tunable luminescent material was prepared based on the composition of functionalized graphitic carbon nitride (g-C{sub 3}N{sub 4}) and europium (III). The functionalized g-C{sub 3}N{sub 4} layers not only behave as multifunctional supports including ligand coordinated with europium (III) and a support structure for the formation of the luminescent material, but exhibit excitation wavelength-dependent luminescence, thus the energy transfer between the functionalized g-C{sub 3}N{sub 4} and europium (III) can match very well by controlling the emission wavelength of functionalized g-C{sub 3}N{sub 4}. The as-prepared materials was comprehensively characterized via X-ray photoelectron spectroscopy, Fourier Transform Infrared spectroscopy, X-ray scattering techniques, Ultraviolet and Visible spectrophotometer, fluorescence spectrophotometer, thermogravimetric analysis, etc. The luminescent material exhibits multi-color emissions which are consistent with the characteristic emissions of europium (III) and functionalized g-C{sub 3}N{sub 4}, and the photoluminescence quality and density of the europium (III) can be greatly enhanced. The brilliant optical properties of the materials make them suiting for multipurpose applications in practical fields. - Graphical abstract: Schematic illustration of the synthesis and basic composition of the luminescent material. Inset figures were luminescence emission spectra of g-C{sub 3}N{sub 4} (A), europium (III) complex (a) and luminescent material (b) with the same concentration in (B) (K{sub ex}=350 nm) and photographs of (left) H{sub 2}O and (right) the H{sub 2}O dispersion of luminescence emission spectra under 350 nm UV radiation. The energy transfer in the luminescent material matchs very well and it exhibits multi-color emissions simultaneously. The enhanced photoluminescence quality and density of the europium (III) makes them suiting for multipurpose applications in practical fields. - Highlights: • Luminescent material exhibits multi-color emissions when excited by single wavelength. • The energy trsnsfer between functionalized g-C{sub 3}N{sub 4} and europium matches very vell. • Functionalized g-C{sub 3}N{sub 4} exhibits excitation wavelength-depengdent bright blue luminescence. • Functionalized g-C{sub 3}N{sub 4} layer provided as multifunctional supports.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Al-doped TiO{sub 2} mesoporous material supported Pd with enhanced catalytic activity for complete oxidation of ethanol

Pd catalysts supported on Al-doped TiO{sub 2} mesoporous materials were evaluated in complete oxidation of ethanol. The catalysts synthesized by wet impregnation based on evaporation-induced self-assembly were characterized by X-ray diffraction, measurement of pore structure, XPS, FT-IR, temperature programmed reduction and TEM. Characteristic results showed that the aluminium was doped into the lattice of mesoporous anatase TiO{sub 2} to form Al-O-Ti defect structure. Catalytic results revealed that Al-doped catalysts were much more active than the pristine one, especially at low temperature (≤200 °C). This should be ascribed to the introduction of aluminium ions that suppressed the strong metal-support interaction and increased the active sites of Pd oxides, enhanced the stabilized anatase TiO{sub 2}, improved well dispersed high valence palladium species with high reducibility and enriched chemisorption oxygen. - Graphical abstract: Al-doped Pd/TiO{sub 2} exhibited optimal catalytic performance for ethanol oxidation and CO{sub 2} yield by the suppression of SMSI. - Highlights: • Palladium catalysts supported on Al-doped TiO{sub 2} mesoporous materials were studied. • The introduction of Al can enhance anatase stabilization and increase defect TiO{sub 2}. • The Pd/Al-TiO{sub 2} catalysts show higher ethanol conversion and CO{sub 2} yield than Pd/TiO{sub 2}. • The influence of Al on SMSI and catalytic performance were evaluated by TPR and XPS.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2012

Electroless preparation and characterization of Ni-B nanoparticles supported on multi-walled carbon nanotubes and their catalytic activity towards hydrogenation of styrene

Graphical abstract: The MWCNT/Ni-B catalyst has been successfully prepared by an electroless deposition process. The Ni-B nanoparticles on the supporter are amorphous and are well-distributed. The catalytic conversion towards hydrogenation of styrene shows excellent catalytic activity of the obtained materials. Highlights: Black-Right-Pointing-Pointer A two-step treatment of MWCNTs enabled the homogeneous growth of Ni-B nanoparticles. Black-Right-Pointing-Pointer Ni-B nanoparticles were amorphous with an average size of 60 nm. Black-Right-Pointing-Pointer There were electron transfer between Ni and B. Black-Right-Pointing-Pointer The catalyst had excellent catalytic activity towards hydrogenation of styrene. -- Abstract: Nickel-boron (Ni-B) nanoparticles supported on multi-walled carbon nanotubes (MWCNTs) were successfully synthesized through an electroless deposition process using the plating bath with sodium borohydride as a reducing agent. The structural and morphological analyses using field-emission scanning electron microscopy, X-ray diffractometry and high-resolution transmission electron microscopy have shown that the Ni-B nanoparticles deposited on the sidewalls of MWCNTs are fine spheres comprised of amorphous structure with the morphologically unique fine-structure like flowers, and homogenously dispersed with a narrow particle size distribution centered at around 60 nm diameter. The catalytic activity of MWCNT/Ni-B nanoparticles was evaluated with respect to hydrogenation of styrene. The hydrogenation catalyzed by MWCNT-supported Ni-B nanoparticles has been found to make styrene selectively converted into ethylbenzene. The highest conversion reaches 99.8% under proper reaction conditions, which demonstrates the high catalytic activity of MWCNT/Ni-B nanoparticles.

36 MATERIALS SCIENCE↗