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At least 847 records · Page 47

Hydrogen production via reforming of biogas over nanostructured Ni/Y catalyst: Effect of ultrasound irradiation and Ni-content on catalyst properties and performance

Highlights: • Synthesis of nanostructured Ni/Y catalyst by sonochemical and impregnation methods. • Enhancement of size distribution and active phase dispersion by employing sonochemical method. • Evaluation of biogas reforming over Ni/Y catalyst with different Ni-loadings. • Preparation of highly active and stable catalyst with low Ni content for biogas reforming. • Getting H{sub 2}/CO very close to equilibrium ratio by employing sonochemical method. - Abstract: The effect of ultrasound irradiation and various Ni-loadings on dispersion of active phase over zeolite Y were evaluated in biogas reforming for hydrogen production. X-ray diffraction, field emission scanning electron microscopy, energy dispersive X-ray, Brunauer–Emmett–Teller, Fourier transform infrared analysis and TEM analysis were employed to observe the characteristics of nanostructured catalysts. The characterizations implied that utilization of ultrasound irradiation enhanced catalyst physicochemical properties including high dispersion of Ni on support, smallest particles size and high catalyst surface area. The reforming reactions were carried out at GHSV = 24 l/g.h, P = 1 atm, CH{sub 4}/CO{sub 2} = 1 and temperature range of 550–850 °C. Activity test displayed that ultrasound irradiated Ni(5 wt.%)/Y had the best performance and the activity remained stable during 600 min. Furthermore, the proposed reaction mechanism showed that there are three major reaction channels in biogas reforming.

36 MATERIALS SCIENCE↗

Oxygen electrode bifunctional electrocatalyst NiCo2O4 spinel

A significant increase in energy density may be possible if a two-unit alkaline regenerative H2-O2 fuel cell is replaced with a single-unit system that uses passive means for H2O transfer and thermal control. For this single-unit system, new electrocatalysts for the O2 electrode will be required which are not only bifunctionally active but also chemically and electrochemically stable between the voltage range of about 0.7 and 1.5 V. NiCo2O4 spinel is reported to have certain characteristics that make it useful for a study of electrode fabrication techniques. High surface area NiCo2O4 powder was fabricated into unsupported, bifunctional, PTFE-bonded, porous gas fuel cell electrodes by commercial sources using varying PTFE contents and sintering temperatures. The object of this study is to measure the bifunctional activities of these electrodes and to observe what performance differences might result from different commercial electrode fabricators. O2 evolution and O2 reduction data were obtained at 80 C (31 percent KOH). An irreversible reaction (i.e., aging) occurred during O2 evolution at potentials greater than about 1.5 V. Anodic Tafel slopes of 0.06 and 0.12 V/decade were obtained for the aged electrodes. Within the range of 15 to 25 percent, the PTFE content was not a critical parameter for optimizing the electrode for O2 evolution activity. Sintering temperatures between 300 and 340 C may be adequate but heating at 275 C may not be sufficient to properly sinter the PTFE-NiCo2O4 mixture. Electrode disintegration was observed during O2 reduction. Transport of O2 to the NiCo2O4 surface became prohibitive at greater than about -0.02 A/sq cm. Cathodic Tafel slopes of -0.6 and -0.12 V/decade were assumed for the O2 reduction process. A PTFE content of 25 percent (or greater) appears to be preferable for sintering the PTFE-NiCo2O4 mixture.

Fielder, William L.↗

FY2016 ILAW Glass Corrosion Testing with the Single-Pass Flow-Through Method

The inventory of immobilized low-activity waste (ILAW) produced at the Hanford Tank Waste Treatment and Immobilization Plant (WTP) will be disposed of at the near-surface, on-site Integrated Disposal Facility (IDF). When groundwater comes into contact with the waste form, the glass will corrode and radionuclides will be released into the near-field environment. Because the release of the radionuclides is dependent on the dissolution rate of the glass, it is important that the performance assessment (PA) model accounts for the dissolution rate of the glass as a function of various chemical conditions. To accomplish this, an IDF PA model based on Transition State Theory (TST) can be employed. The model is able to account for changes in temperature, exposed surface area, and pH of the contacting solution as well as the effect of silicon concentrations in solution, specifically the activity of orthosilicic acid (H4SiO4), whose concentration is directly linked to the glass dissolution rate. In addition, the IDF PA model accounts for the alkali-ion exchange process as sodium is leached from the glass and into solution. The effect of temperature, pH, H4SiO4 activity, and the rate of ion-exchange can be parameterized and implemented directly into the PA rate law model. The rate law parameters are derived from laboratory tests with the single-pass flow-through (SPFT) method. To date, rate law parameters have been determined for seven ILAW glass compositions, thus additional rate law parameters on a wider range of compositions will supplement the existing body of data for PA maintenance activities. The data provided in this report can be used by ILAW glass scientists to further the understanding of ILAW glass behavior, by IDF PA modelers to use the rate law parameters in PA modeling efforts, and by Department of Energy (DOE) contractors and decision makers as they assess the IDF PA program.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

One-pot synthesis of copper-doped graphitic carbon nitride nanosheet by heating Cu–melamine supramolecular network and its enhanced visible-light-driven photocatalysis

Here we report a novel synthetic pathway for preparation of Cu-doped g-C{sub 3}N{sub 4} (Cu-g-C{sub 3}N{sub 4}) with nanosheet morphology by using a two dimensional Cu–melamine supramolecular network as both sacrificial template and precursor. The specific surface area of Cu-g-C{sub 3}N{sub 4} is 40.86 m{sup 2} g{sup −1}, which is more than 7 times larger than that of pure g-C{sub 3}N{sub 4}. Cu-g-C{sub 3}N{sub 4} showed strong optical absorption in the visible-light region and expanded the absorption to the near-infrared region. The uniform nanosheet morphology, higher surface area and strong visible-light absorption have enabled Cu-g-C{sub 3}N{sub 4} exhibiting enhanced visible light photocatalytic activity for the photo-degradation of methylene blue (MB). The results indicate that metal–melamine supramolecular network can be promising precursors for the one step preparation of efficient metal-doped g-C{sub 3}N{sub 4} photocatalysts. - Graphical abstract: Cu-doped g-C{sub 3}N{sub 4} (Cu-g-C{sub 3}N{sub 4}) with nanosheet morphology was fabricated via a simple one step preparation by using a two dimensional Cu–melamine supra-molecular network as both sacrificial template and precursor. - Highlights: • Cu-doped g-C{sub 3}N{sub 4} (Cu-g-C{sub 3}N{sub 4}) with nanosheet morphology was prepared. • Cu-g-C{sub 3}N{sub 4} showed strong optical absorption in the visible-light region. • Cu-g-C{sub 3}N{sub 4} exhibits enhanced visible light photocatalytic activity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Analysis of MGS TES Data over Acidalia Planitia and Cydonia Mensae: Compositional Evidence for Hydrovolcanic Activity?

For this study, Mars Global Surveyor (MGS) Thermal Emission Spectrometer (TES) emissivity data for Acidalia Planitia and Cydonia Mensae (Figure 1) were assembled and used to examine the surface mineralogy of these areas. Analyzing TES data for high latitude locales such as Acidalia presents a challenge since the surface temperatures over these regions is inherently lower than for equatorial locales. In this report, analyses of TES data are described and results are evaluated for potential compositional evidence for hydrovolcanic activity in Acidalia and Cydonia.

Farrand, W. H.↗

Effects of the method of active site characterization for determining structure-sensitivity in Ag-catalyzed ethylene epoxidation

We report catalysts have been prepared on a low surface area α-Al 2 O 3 support used commercially for previous generation olefin epoxidation catalysts. Prescreening of the low surface area alumina (0.73 m 2 /g) indicated the absence of acid catalyzed isomerization of EO at an evaluation temperature of 210 °C. A 0.1 wt% Ag base material synthesized by incipient wetness impregnation of AgNO 3 was used as a base material for electroless deposition (ED) of additional Ag to increase particle sizes by controlled reduction of Ag + directly onto the preexisting Ag surface to form weight loadings between 0.3 and 5.0 wt% metal. A 12 wt% Ag/α-Al 2 O 3 using Ag 2 C 2 O 4 as the Ag precursor was also prepared to compare performance of the ED samples with a catalyst more typical of industrial formulations. Characterization by SEM, STEM, and hydrogen titration of oxygen precovered Ag characterized before and after catalytic evaluation indicated that microscopy is required to accurately represent distributions of Ag particle sizes, but H 2 titration of O-precovered Ag gives the best representation of active sites since it directly counts the number of Ag surface sites. Larger particles >100 nm are resistant to both Ag sintering and carbon foulant; TOF values were relatively insensitive to particle size with only a 2.2 × difference between the best and worst performing samples. Selectivity, which is not a function of TOF, shows the most significant structure sensitivity effect where particle sizes follow the trend 67 nm ≈ 92 nm (58% EO) < 157 nm (67% EO) < 211–542 nm (73% EO). The lower EO selectivities were also correlated with increased fouling for the smaller Ag sizes, suggesting that more strongly bound EO precursor(s) leads to combustion and CO 2 /H 2 O formation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High-surface-area corundum nanoparticles by resistive hotspot-induced phase transformation

Abstract High-surface-area α-Al 2 O 3 nanoparticles are used in high-strength ceramics and stable catalyst supports. The production of α-Al 2 O 3 by phase transformation from γ-Al 2 O 3 is hampered by a high activation energy barrier, which usually requires extended high-temperature annealing (~1500 K, > 10 h) and suffers from aggregation. Here, we report the synthesis of dehydrated α-Al 2 O 3 nanoparticles (phase purity ~100%, particle size ~23 nm, surface area ~65 m 2 g −1 ) by a pulsed direct current Joule heating of γ-Al 2 O 3 . The phase transformation is completed at a reduced bulk temperature and duration (~573 K, < 1 s) via an intermediate δʹ-Al 2 O 3 phase. Numerical simulations reveal the resistive hotspot-induced local heating in the pulsed current process enables the rapid transformation. Theoretical calculations show the topotactic transition (from γ- to δʹ- to α-Al 2 O 3 ) is driven by their surface energy differences. The α-Al 2 O 3 nanoparticles are sintered to nanograined ceramics with hardness superior to commercial alumina and approaching that of sapphire.

Deng, Bing (ORCID:0000000305308410)↗

Incorporating Rich Mesoporosity into a Ceria-Based Catalyst via Mechanochemistry

Ceria-based materials possessing mesoporous structures afford higher activity than the corresponding bulk materials in CO oxidation and other catalytic applications, because of the wide pore channel and high surface area. The development of a direct, template-free, and scalable technology for directing porosity inside ceriabased materials is highly welcome. Here in this paper, a family of mesoporous transition-metaldoped ceria catalysts with specific surface areas up to 122 m 2 g -1 is constructed by mechanochemical grinding. No templates, additives, or solvents are needed in this process, while the mechanochemistry-mediated restructuring and the decomposing of the organic group led to plentiful mesopores. Interestingly, the copper species are evenly dispersed in the ceria matrix at the atomic scale, as observed in high resolution scanning transmission electron microscopy in high angle annular dark field. The copper-doped ceria materials show good activity in the CO oxidation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Episodic Endogenetic-driven Atmospheric and Hydrologic Cycles and Their Influence on the Geologic Records of the Northern and Southern Hemispheres, Mars

Diverse evidence shows a direct correlation between episodic endogenetic events of the Tharsis magmatic complex (TMC)/Superplume, flood inundations in the northern plains, and glacial/ lacustrine/ice sheet activity in the south polar region, which includes Hellas and Argyre impact basins, corroborating the MEGAOUTFLO hypothesis. The TMC encompasses a total surface area of approximately 2 x 10(exp 7) sq km, which is slightly larger than the estimated size of the Southern Pacific Superplume. These hydrologic events include: (1) a Noachian to possibly Early Hesperian oceanic epoch and related atmospheric and environmental change (a water body covering about 1/3 of the planet s surface area) related to the incipient development of Tharsis Superplume and the northwestern sloping valleys (NSVs) and possibly early circum-Chryse development, the northwest and northeast watersheds of Tharsis, respectively, (2) a smaller ocean inset within the former larger ocean related to extensive Late Hesperian to Early Amazonian effusive volcanism at Tharsis and Elysium and incisement of the circum-Chryse outflow system. During this time, magmatic/plume-driven tectonic activity transitioned into more centralized volcanism. This Late Hesperian water body may have simply diminished into smaller seas and/or lakes during the Amazonian Period, or renewed activity at Tharsis and Elysium resulted in brief perturbations from the prevailing cold and dry climatic conditions to later form minor seas or lakes. All of the hydrologic phases transitioned into extensive periods of quiescence.

Dohm, J. M.↗

Parametric Study of Variable Emissivity Radiator Surfaces

The goal of spacecraft thermal design is to accommodate a high function satellite in a low weight and real estate package. The extreme environments that the satellite is exposed during its orbit are handled using passive and active control techniques. Heritage passive heat rejection designs are sized for the hot conditions and augmented for the cold end with heaters. The active heat rejection designs to date are heavy, expensive and/or complex. Incorporating an active radiator into the design that is lighter, cheaper and more simplistic will allow designers to meet the previously stated goal of thermal spacecraft design Varying the radiator's surface properties without changing the radiating area (as with VCHP), or changing the radiators' views (traditional louvers) is the objective of the variable emissivity (vary-e) radiator technologies. A parametric evaluation of the thermal performance of three such technologies is documented in this paper. Comparisons of the Micro-Electromechanical Systems (MEMS), Electrochromics, and Electrophoretics radiators to conventional radiators, both passive and active are quantified herein. With some noted limitations, the vary-e radiator surfaces provide significant advantages over traditional radiators and a promising alternative design technique for future spacecraft thermal systems.

Grob, Lisa M.↗

Synthesis of belt-like BiOBr hierarchical nanostructure with high photocatalytic performance

Highlights: • BiOBr hierarchical nanobelts (NBs) were solvothermally prepared. • NBs show higher specific surface area and photoabsorption than BiOBr nanosheets. • NBs exhibit higher photoactivity than the nanosheets. - Abstract: One-dimensional (1D) bismuth oxyhalide (BiOX) hierarchical nanostructures are always difficult to prepare. Herein, we report, for the first time, a simple synthesis of BiOBr nanobelts (NBs) via a facile solvothermal route, using bismuth subsalicylate as the template and bismuth source. The BiOBr nanobelts are composed of irregular single crystal nanoparticles with highly exposed (0 1 0) facets. Compared with the BiOBr nanosheets (NSs) with dominant exposed (0 0 1) facets, they exhibit higher photocatalytic activity toward degradation of Rhodamine B and Methylene Blue under visible light irradiation. The higher photocatalytic performance of BiOBr NBs arises from their larger specific surface area and higher photoabsorption capability. This study provides a simple route for synthesis of belt-like Bi-based hierarchical nanostructures.

36 MATERIALS SCIENCE↗

Acido-basicity of lanthana/alumina catalysts and their activity in ethanol conversion

Lanthana on alumina samples (0.2, 0.8 and 4.7 theoretical monolayers) were prepared by incipient wetness impregnation using γ-Al 2 O 3 as support. Characterization has been performed by BET, XRD, skeletal FT-IR, DR-UVvis, XPS, HR-TEM, IR spectra of the surface OH, adsorbed pyridine and CO 2 , and isopropanol TPD. Here ethanol conversion was investigated both in temperature-programmed surface reaction (TPSR) dynamic conditions as well as in steady-state flow reactor tests. Lanthanum addition stabilizes alumina with respect to sintering and loss of surface area and La- containing phases are observed only for the high-La loaded catalyst. La-alumina catalysts are less active in ethanol dehydration than alumina but more selective to diethyl ether at partial conversion. 5%La 2 O 3 /Al 2 O 3 is also equally or more selective than alumina to ethylene at high conversion, producing less carbonaceous material during reaction. Thus, this catalytic system might be a good candidate for (bio)ethylene production through (bio)ethanol dehydration.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

3D Printed TiO 2 Negative Electrodes for Sodium-Ion and Lithium-ion Batteries using Vat Photopolymerization

Additive manufacturing, also called 3D printing, represents a unique approach to develop three dimensional shape-conformable batteries with enhanced electrodes, specific surface area, improved ion diffusion, and power. For the first time, the formulation of a composite photocurable resin loaded with battery electrochemically active components was designed to feed a vat photopolymerization (VPP) 3D printer. In direct alignment with NASA’s Artemis mission goals to develop sustainable lunar energy storage infrastructure necessary to support long-term human operations, TiO 2 was here selected as an active material for the negative electrode for sodium-ion and lithium-ion batteries due to its abundance on the lunar surface. The TiO 2 loading in the composite photocurable resin and in the resulting VPP-printed negative electrode was increased as high as possible to enhance the electrochemical performance, while simultaneously ensuring the printability and acceptable mechanical strength for sample handling. The effect of thermal post-processing on the electrical, electrochemical and mechanical performance is reported. Finally, a configurational study is implemented to identify the impact of two different electrode designs (cubic and gyroid lattice unit cells) on the electrochemical performance. This work addresses the difficulties related to the introduction of solid particles within a VPP photocurable resin and the need for a compromise between the electrochemical performances and printability to obtain fully functional VPP-printed electrodes.

sodium-ion battery↗

Air Dispersion Modeling of Radioactive Releases During Proposed 236Z Rubble Pile Removal Activities

This report is part of the planning process for the removal of the 236Z rubble remaining as of January 1, 2018, at the Plutonium Finishing Plant (PFP) on the Hanford Site. This report documents an analysis considering standard techniques for the removal of demolition rubble. It does not document any decisions about the removal approaches. This document is intended to guide the establishment of a boundary for the application of an air monitoring regime. Atmospheric dispersion modeling using estimated release rates has been conducted to provide information on the location and levels of radioactive contamination that may be expected as the result of rubble removal activities. Hourly meteorological data collected over a 6-year period (2004–2009) were used to examine the effects of wind speed, direction, and stability on projected concentrations of contaminants in air and deposited on nearby surfaces. The source terms modeled in this report were based on the residual transuranic contamination levels that are anticipated to remain in the 236Z rubble following building demolition. The potential airborne concentrations were established using the five-factor formula from DOE-HDBK-3010 (DOE 1994) considering material-at-risk, damage ratio, airborne release fraction, respirable fraction, and leak path factor. Radioactive contamination emissions were calculated by release mechanism and rubble pile area for on-shift and off-shift activities. The emissions from the applicable sources were combined to provide emissions estimates for each day from each cleanup area. The U.S. Environmental Protection Agency’s (EPA’s) AERMOD computer code was used to estimate atmospheric dispersion and deposition of the released radioactive materials in the immediate vicinity of the planned rubble removal activities Both airborne and surface concentrations were modeled with AERMOD. Hourly derived air concentrations (DAC) were modeled for an array of receptors covering the rubble pile site and surrounding area. Peak (95th and 99th percentile) values of time-integrated air concentrations at these receptor points are derived from these hourly values, with modeling results reported as total incremental air concentrations in DAC-hours occurring over the selected time period. Total accumulated deposition amounts were also evaluated with AERMOD using the same array of receptors, with results reported as disintegrations per minute (dpm) per 100 cm2. Each rubble pile was considered in terms of its size, location, and estimated contamination levels. The modeling was based on the assumed sequence of the rubble removal activities. The results in this report are based on cleanup schedules and methods proposed by CHPRC. As of January 1, 2018, there are broadly three large rubble piles (west, footprint, and east) remaining of the 236Z Building process cell. It is assumed that the overall cleanup will require either 1) 30 days over a 6-week period, or 2) 60 days over a 12-week period. Work was assumed to be performed during 10-hour day shifts. The analysis shows that some releases of radioactive material are to be anticipated during the cleanup of the 236Z rubble piles. The modeling results presented here are closely tied to the details of how the rubble removal is to be conducted. The results indicate that for the rubble removal, the radiological exposures from the planned activities are predicted to be well below the designated limits for air and soil exposures. The cleanup of the 236Z main process cell rubble is expected to release some alpha-emitting radionuclides. However, results based on 6 years of hourly climatological data, two representative cleanup periods, realistic mitigating actions, and a bounding source term indicate that concentrations at the fence line of the PFP facilities should remain well below 12 DAC-hours/week. The results presented in this report are a reevaluation of a subset of the results presented in PNNL-20173 Rev. 4.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Rapid microwave-assisted sol-gel preparation of Pd-substituted LnFeO 3 (Ln = Y, La): phase formation and catalytic activity

We present a rapid microwave-assisted sol–gel approach to Pd-substituted LnFeO 3 (Ln = Y, La) for applications in C–C coupling reactions. These materials could be prepared in household microwave ovens in less than 15 minutes of reaction time with the final materials displaying well-defined structure and morphology. Phase evolution was studied using time-dependent microwave heatings and then compared with the results obtained from thermogravimetric analyses. Materials were confirmed to be phase pure by laboratory and synchrotron X-ray diffraction. Substituted Pd is ionic as shown by the binding energy shift from X-ray photoelectron spectroscopy. The short heating periods required for phase purity allow these materials less time for sintering as compared to conventional solid state preparation methods, making relatively high surface areas achievable. These materials have been successfully used as catalyst precursor materials for C–C coupling reactions in which the active species is Pd 0 . Pd-substituted LnFeO 3 (Ln = Y, La) provides Pd 0 in solution which can be complexed by the ligand SPhos, allowing for aryl chloride coupling.

Misch, Lauren M.↗

Construction of Boron‐ and Nitrogen‐Enriched Nanoporous π‐Conjugated Networks Towards Enhanced Hydrogen Activation

Abstract Boron‐enriched scaffolds have demonstrated unique features and promising performance in the field of catalysis towards the activation of small gas molecules. However, there is still a lack of facile approaches capable of achieving high B doping and abundant porous channels in the targeted catalysts. Herein, construction of boron‐ and nitrogen‐enriched nanoporous π‐conjugated networks (BN‐NCNs) was achieved via a facile ionothermal polymerization procedure with hexaazatriphenylenehexacarbonitrile [HAT(CN) 6 ] sodium borohydride as the starting materials. The as‐produced BN‐NCN scaffolds were featured by high heteroatoms doping (B up to 23 wt. % and N: up to 17 wt. %) and permanent porosity (surface area up to 759 m 2 g −1 mainly contributed by micropores). With the unsaturated bonded B species acting as the active Lewis acid sites and defected N species acting as the active Lewis base sites, those BN‐NCNs delivered attractive catalytic performance towards H 2 activation/dissociation in both gaseous and liquid phase, acting as efficient metal‐free heterogeneous frustrated Lewis pairs (FLPs) catalysts in hydrogenation procedures.

Li, Meijia↗

Soft chemical synthesis of Ag{sub 3}SbS{sub 3} with efficient and recyclable visible light photocatalytic properties

Highlights: • Highly crystalline Ag{sub 3}SbS{sub 3} synthesized using soft chemical approach. • First time report of photocatalytic activity of Ag{sub 3}SbS{sub 3}. • Ag{sub 3}SbS{sub 3} degraded the harmful organic dyes rapidly under visible radiation. • Pseudo first order kinetics have been followed in these sets of reactions. • Up to 90% of Methylene Blue degraded even after 4th cycle of catalyst reuse. • Structure of catalyst is intact after reuse. • As the catalyst is heavy, its separation after use is quite simple. - Abstract: Application of Ag{sub 3}SbS{sub 3}, obtained by soft chemical approach involving rapid reaction of air stable metal–thiourea complexes in ethylene glycol medium, as visible light photocatalyst for the degradation of dye solutions was investigated. Ag{sub 3}SbS{sub 3} was confirmed by high resolution powder X-ray diffraction pattern and its no defined morphology was present in SEM images. From UV–vis spectroscopy measurements, optical band gap of 1.77 eV was deduced for Ag{sub 3}SbS{sub 3}. Rapid degradation kinetics and recyclability was exhibited by Ag{sub 3}SbS{sub 3} towards Methylene Blue, Methyl Orange, Malachite Green, and Rhodamine 6G dye solutions under visible radiation. All these processes followed pseudo first order kinetics. High surface area (6.39 m{sup 2}/g), with mesopores (3.81 nm), arising from solvent mediated synthesis of Ag{sub 3}SbS{sub 3} has been correlated to its catalytic activity.

36 MATERIALS SCIENCE↗

High performance carbon/silica co-decorated TiO{sub 2} nanotubes for visible-light driven water splitting

Graphical abstract: Using amino-propyl-triethoxy silane (KH570) as silane couplers, a novel carbon/silica dots co-decorated TiO{sub 2} nanotube (CS@TNT) is prepared through silane modification and thermal calcination approach. The CS@TNT retains its tubular morphology at as high as 500 °C, and presents a high activity (0.096 mmol/h) towards photocatalytic water splitting. - Highlights: • A novel route of silane-modification then H{sub 2} calcination is developed. • Carbon and silica dots are highly dispersed on the TNT. • The CS@TNT retains its tubular morphology at as high as 500 °C. • A high activity (0.096 mmol/h) is achieved towards photocatalytic water splitting. • Effect of carbon/silica modification is investigated in detail. - Abstract: A novel carbon/silica co-decorated TiO{sub 2} nanotubes (TNT) photocatalyst (CS@TNT) was prepared for visible light driven water splitting by a facile two-steps process of amino-propyl-triethoxy silane modification and calcination. Structure characterizations (XRD, STEM, XPS, UV–vis spectra and PL spectra) revealed that the silica and carbon dots were homogeneously dispersed on the surfaces of TNT. The introduced silica resists crystallization of TNT, and keeps the tubular morphology intact and high surface area; the co-existence of carbon dots increases the visible light absorbance capacity and promotes the electron-hole separation efficiency. The CS@TNT preserves intact tubular morphology during calcination (500 °C), and a high activity of 0.096 mmol/h is achieved, which was 1.7 times higher than that of actual catalyst made of gold nanoparticles loading on TNT.

36 MATERIALS SCIENCE↗