Promotion of TiO2 Nanotube-Confined Pt Nanoparticles via Surface Modification with Fe2O3 for Ethylene Oxidation at Low Temperature.
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ABSTRACT:
SUBMITTER: Li J
PROVIDER: S-EPMC8153978 | biostudies-literature |
REPOSITORIES: biostudies-literature
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Project description:Efficient and low-cost degradation of ethylene has always been a difficult problem in the storage and transportation of fruits and vegetables. Although photocatalysis is considered to be a feasible and efficient solution for ethylene degradation, the low degradation ability of conventional catalysts for small non-polar molecules limits its application. TiO2 has the advantage of tunable microstructure, but it also has the defects of wide band gap and low utilization of sunlight. The surface plasmon resonance (SPR) effect of noble metals can effectively improve the visible light absorption range of catalysts, and the synergy of noble metals further enhances the photocatalytic ability. Herein, we developed a series of AuPt catalysts through the photo-deposition method. Benefited from the SPR effect and the synergy of Au and Pt, the efficiency of AuPt-TiO2 was 19.9, 4.64 and 2.42 times that of TiO2, Au-TiO2 and Pt-TiO2, and the photocatalytic degradation ability of AuPt-TiO2 was maintained in five cyclic stability tests. Meanwhile, the transient photocurrent spectra and PL spectra proved that the light absorption capacity and carrier separation efficiency of AuPt-TiO2 were enhanced. This work provides a new direction for enhancing non-polar small-molecule photodegradation of semiconductors.
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Project description:The main goal of this study was to modify the activity of Pd/TiO2/Ti catalyst in the reaction of CO oxidation by the addition of Zn. Plasma electrolytic oxidation (PEO) of Ti wire was conducted to produce a uniform porous layer of TiO2. A mixture of Pd and Zn was then introduced by means of adsorption. After reduction treatment, the activity of the samples was examined by oxidation of 5% CO in a temperature range from 80-350 °C. Model catalysts with sufficient amounts of the metals for physico-chemical investigation were prepared to further investigate the reaction between Pd and Zn during CO oxidation. The structures and compositions of the samples were investigated using scanning electron microscopy with energy dispersive spectroscopy (SEM-EDS), time-of-flight secondary ion mass spectrometry (TOF-SIMS), inductively coupled plasma mass spectrometry (ICP-MS), Fourier transform infrared (FTIR), and X-ray diffraction (XRD). Modification of Pd/TiO2/Ti catalyst by Zn with a Pd:Zn atomic ratio of 2:1 decreased the temperature of complete CO oxidation from 220 °C for Pd/TiO2/Ti to 180 °C for Pd-Zn/TiO2/Ti. The temperature of 50% CO conversion on Pd-Zn(2:1)/TiO2/Ti was around 55 °C lower than in the reaction on monometallic Pd catalyst. The addition of Zn to the Pd catalyst lowered the binding energy of CO on the surface and improved the dissociative adsorption of oxygen, facilitating the oxidation of CO. FTIR showed that the bridging form of adsorbed CO is preferred on bimetallic systems. Analysis of the surface compositions of the samples (SEM-EDS, TOF-SIMS) showed higher amounts of oxygen on the bimetallic systems.
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Project description:Supported Pt-based catalysts have been identified as highly selective catalysts for CO oxidation, but their potential for applications has been hampered by the high cost and scarcity of Pt metals as well as aggregation problems at relatively high temperatures. In this work, nanorod structured (TiO2-Pt)/CeO2 catalysts with the addition of 0.3 at% Pt and different atomic ratios of Ti were prepared through a combined dealloying and calcination method. XRD, XPS, SEM, TEM, and STEM measurements were used to confirm the phase composition, surface morphology, and structure of synthesized samples. After calcination treatment, Pt nanoparticles were semi-inlayed on the surface of the CeO2 nanorod, and TiO2 was highly dispersed into the catalyst system, resulting in the formation of (TiO2-Pt)/CeO2 with high specific surface area and large pore volume. The unique structure can provide more reaction path and active sites for catalytic CO oxidation, thus contributing to the generation of catalysts with high catalytic activity. The outstanding catalytic performance is ascribed to the stable structure and proper TiO2 doping as well as the combined effect of Pt, TiO2, and CeO2. The research results are of importance for further development of high catalytic performance nanoporous catalytic materials.
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Project description:Supported metal single atom catalysts (SACs) present an emerging class of low-temperature catalysts with high reactivity and selectivity, which, however, face challenges on both durability and practicality. Herein, we report a single-atom Pt catalyst that is strongly anchored on a robust nanowire forest of mesoporous rutile titania grown on the channeled walls of full-size cordierite honeycombs. This Pt SAC exhibits remarkable activity for oxidation of CO and hydrocarbons with 90% conversion at temperatures as low as ~160 oC under simulated diesel exhaust conditions while using 5 times less Pt-group metals than a commercial oxidation catalyst. Such an excellent low-temperature performance is sustained over hydrothermal aging and sulfation as a result of highly dispersed and isolated active single Pt ions bonded at the Ti vacancy sites with 5 or 6 oxygen ions on titania nanowire surfaces.
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Project description:Low temperature CO oxidation reaction is known to be facilitated over platinum supported on a reducible cerium oxide. Pt species act as binding sites for reactant CO molecules, and oxygen vacancies on surface of cerium oxide atomically activate the reactant O2 molecules. However, the impacts of size of Pt species and concentration of oxygen vacancy at the surface of cerium oxide on the CO oxidation reaction have not been clearly distinguished, thereby various diverse approaches have been suggested to date. Here using the co-precipitation method we have prepared pure ceria support and infiltrated it with Pt solution to obtain 0.5 atomic% Pt supported on cerium oxide catalyst, and then systematically varied the size of Pt from single atom to ∼1.7 nm sized nanoparticles and oxygen vacancy concentration at surface of cerium oxide by controlling the heat-treatment conditions, which are temperature and oxygen partial pressure. It is found that Pt nanoparticles in range of 1-1.7 nm achieve 100% of CO oxidation reaction at ∼100 °C lower temperature compared to Pt single atom owing to the facile adsorption of CO but weaker binding strength between Pt and CO molecules, and the oxygen vacancy in the vicinity of Pt accelerates CO oxidation below 150 °C. Based on this understanding, we show that a simple hydrogen reduction at 550 °C for the single atom Pt supported on CeO2 catalyst induces the formation of highly dispersed Pt nanoparticles with size of 1.7 ± 0.2 nm and the higher concentration of surface oxygen vacancies simultaneously, enabling 100% conversion from CO to CO2 at 200 °C as well as 16% conversion even at 150 °C owing to the synergistic effects of Pt nanoparticles and oxygen vacancies.
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Project description:Herein, perylene-3,4,9,10-tetracarboxylic acid-doped polyaniline (PTP) nanofibers with/without photoreactive anatase TiO2 (TiO2-PTP and PTP, respectively) have been successively synthesized and subsequently decorated by Pt nanoparticles (Pt NPs) to prepare Pt-PTP and Pt-TiO2-PTP composites. High-resolution transmission electron microscopy confirms the presence of ∼3 nm spherical-shaped Pt NPs on both the composites along with TiO2 on Pt-TiO2-PTP. Pt loading on the composites is deliberately kept similar to compare the methanol electro-oxidation in the two composites. The Pt nanocomposites along with the precursor polyanilines are characterized by optical characterization, X-ray diffraction study, X-ray fluorescence spectroscopy, and Raman spectroscopy. The ternary composite-modified (Pt-TiO2-PTP) electrode demonstrates high electrocatalytic performance for methanol oxidation reaction in acid medium than Pt-PTP and Pt-TiO2. The higher electrochemical surface area (1.7 times), high forward/backward current ratio, and the higher CO tolerance ability for Pt-TiO2-PTP make it a superior catalyst for methanol oxidation reaction in the electrochemical process than Pt-PTP. Moreover, the catalytic activity of Pt-TiO2-PTP is further enhanced significantly with light irradiation. The cooperative effects of photo- and electrocatalysis on methanol oxidation reaction in Pt-TiO2-PTP enhance the methanol oxidation catalytic activity approximately 1.3 times higher in light illumination than in dark. Therefore, the present work will be proficient to get a light-assisted sustainable approach for developing the methanol oxidation reaction activity of Pt NP-containing catalysts in direct methanol fuel cells.
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Project description:This study presents a TiO2/C hybrid material with biomimetic channels fabricated using a wood template. Repeated impregnations of pretreated wood chips in a Ti precursor were conducted, followed by calcination at 400-600 °C for 4 hours under a nitrogen atmosphere. The generated TiO2 nanocrystals were homogenously distributed inside a porous carbon framework. With an extremely low Pt catalyst loading (0.04-0.1 wt%), the obtained porous catalyst could effectively oxidize formaldehyde to CO2 and H2O even under room temperature (conv. ∼100%). Wood acted as both a structural template and reduction agent for Pt catalyst generation in sintering. Therefore, no post H2 reduction treatment for catalyst activation was required. The hierarchal channel structures, including 2-10 nm mesopores and 20 μm diameter channels, could be controlled by calcination temperature and atmosphere, which was confirmed by SEM and BET characterizations. Based on the abundant availability of wood templates and reduced cost for low Pt loading, this preparation method shows great potential for large-scale applications.
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Project description:As one of the crystal phases of titania, TiO2(B) was first utilized as a catalyst carrier for the oxidation of formaldehyde (HCHO). The mesoporous TiO2(B) loaded with Pt nanoparticles enhanced the HCHO oxidation reaction whose reaction rate was 4.5-8.4 times those of other crystalline TiO2-supported Pt catalysts. Simultaneously, Pt/TiO2(B) exhibited long-term stable HCHO oxidation performance. The structural characterization results showed that in comparison with Pt/anatase, Pt/TiO2(B) had more abundant hydroxyls, facilitating increasing the content of oxygen species. Studies on the role of hydroxyls in HCHO oxidation of Pt/TiO2(B) illustrated that synergistic involvement of terminally bound hydroxyls and bridging hydroxyls in HCHO oxidation accelerated the transformation from HCHO to formate via dioxymethylene. Moreover, hydroxyls could avoid the accumulation of excessive formate on Pt/TiO2(B) and promote the rapid oxidation of CO. Accordingly, the hydroxyl groups could accelerate each substep of formaldehyde oxidation, which enabled Pt/TiO2(B) to exhibit excellent formaldehyde oxidation performance.
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Project description:Pt nanoparticles are typically decorated as co-catalyst on semiconductors to enhance the photocatalytic performance. Due to the low abundance and high cost of Pt, reaching a high activity with minimized co-catalyst loadings is a key challenge in the field. We explore a dewetting-dealloying strategy to fabricate on TiO2 nanotubes nanoporous Pt nanoparticles, aiming at improving the co-catalyst mass activity for H2 generation. For this, we sputter first Pt-Ni bi-layers of controllable thickness (nm range) on highly ordered TiO2 nanotube arrays, and then induce dewetting-alloying of the Pt-Ni bi-layers by a suitable annealing step in a reducing atmosphere: the thermal treatment causes the Pt and Ni films to agglomerate and at the same time mix with each other, forming on the TiO2 nanotube surface metal islands of a mixed PtNi composition. In a subsequent step we perform chemical dealloying of Ni that is selectively etched out from the bimetallic dewetted islands, leaving behind nanoporous Pt decorations. Under optimized conditions, the nanoporous Pt-decorated TiO2 structures show a>6 times higher photocatalytic H2 generation activity compared to structures modified with a comparable loading of dewetted, non-porous Pt. We ascribe this beneficial effect to the nanoporous nature of the dealloyed Pt co-catalyst, which provides an increased surface-to-volume ratio and thus a more efficient electron transfer and a higher density of active sites at the co-catalyst surface for H2 evolution.
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Project description:Aligned TiO2 nanotube layers (TiNTs) grown by self-organizing anodization of a Ti-substrate in a fluoride-based electrolyte were decorated with graphitic-phase C3N4 (g-C3N4) via a facile chemical vapor deposition approach. In comparison with classical TiO2 nanotubes (anatase), the g-C3N4/TiNTs show an onset of the photocurrent at 2.4?eV (vs. 3.2?eV for anatase) with a considerably high photocurrent magnitude in the visible range. After further decoration with Pt nanoparticles, we obtained a visible-light responsive platform that showed, compared with g-C3N4-free TiNTs, a strong enhancement for photoelectrochemical and bias-free H2 evolution (15.62??Lh-1?cm-2), which was almost a 98-fold increase in the H2 production rate of TiNTs (0.16??Lh-1?cm-2). In a wider context, the g-C3N4-combined 3?D nanoporous/nanotubular structure thus provides a platform with significant visible-light response in photocatalytic applications.
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