Low-temperature Reaction Research Articles

A study on structural and optical properties of the synthesized PVP capped Zinc Oxide Nanoparticles

Zinc Oxide Nanoparticles, capped with a polymer, have been effectively synthesized using a chemical precipitation method at a relatively low reaction temperature of 60 °C. The present study examines the structural and optical properties of ZnO Nanoparticles (NPs) that have been synthesized and capped with different weight percentages of PVP (Polyvinyl Pyrrolidone). To investigate these properties, advanced analytical techniques including X-ray Diffraction (XRD), Field Emission Scanning Electron Microscopy (FE-SEM), Ultra Violet-visible (UV–vis) absorption spectroscopy are employed. The XRD analysis reveals that the synthesized ZnO samples have a hexagonal wurzite structure, regardless of adding capping agent. The Williamson-Hall (W-H) analysis, a commonly used method, estimates the strain present in synthesized materials. The SEM image depicts ZnO NPs that have a nearly spherical form and are seen to be agglomerated. The UV–vis absorption measurements demonstrate a phenomenon known as blue shift when compared to the absorption characteristic of bulk ZnO.

Investigation of hydrogen/air co-flow jet flame propagation mechanism in supersonic crossflow

The design of fuel injection schemes is crucial for improving the combustion performance of high-Mach number scramjet. To clarify the feasibility of the coaxial jet injection scheme, high fidelity Large Eddy Simulation of the supersonic coaxial jet flame is conducted. The simulations are in good agreement with the experimental results in terms of time-averaged velocity, temperature, and species distribution. Auto-ignition phenomenon and the characteristics of partially premixed flame are well captured. The introduction of co-flow air increases the vorticity magnitude close to the injection port and downstream near-wall region, which results in a 400 K rise in the time-averaged temperature on the downstream near-wall region and a 4% increase in the proportion of premixed combustion near the injection port. Moreover, the instantaneous distribution of hydroxy radical indicates that the spanwise width of the windward reaction shear layer is reduced utilizing the coaxial jet scheme. Chemical kinetic analysis is applied to reveal the propagation mechanism of partially premixed flames. Thermal explosion is the chemical explosion mode for all coaxial jet flame front, which are dominated by a high-temperature reaction path. The low-temperature reaction path mainly exists in the transverse jet injection port, downstream near-wall region of the single transverse jet and co-flow lifted flame base. These significant findings provide valuable insights for the potential engineering application of the coaxial jet injection scheme to a high Mach number scramjet.

Modeling of a heat-integrated biomass downdraft gasifier: Influence of feed moisture and air flow

A model for a heat-integrated biomass downdraft gasifier is developed and used to study the influence of changes in biomass moisture content and gasifier air flow. This one-dimensional steady-state model accounts for pyrolysis, combustion and gasification reaction kinetics as well as transport phenomena occurring within the gasifier and heat integration system. The gasifier is divided into four zones for solving the ordinary differential equations (ODEs), because each zone has different geometry for the reactor or heating system. The material and energy balance ODEs are solved as a boundary value problem (BVP), ensuring that conditions for the producer gas at the bottom of the reactor match the conditions of the countercurrent annulus gas, which is used for heating. The model also accounts for the preheating of the biomass using exhaust gas from an associated engine used to generate electricity from the producer gas. The model predicts the process gas temperature, flow rate and composition and was validated using two experimental runs with different control inputs. The model predictions show good agreement with the data. Simulations with the highest feed moisture result in lower reactor temperatures and simulations with the highest air flow result in the highest reactor temperatures.

Metal-Catalyzed Thermo-Catalytic Decomposition and Continuous Catalyst Generation

In this study, metal dusting is utilized to initiate a two-stage thermo-catalytic decomposition (TCD) process. Stage 1 starts with metal-catalyzed TCD, and in stage 2 the metal-catalyzed carbon catalyzes additional TCD. TEM is presented of the early- versus late-stage TCD to qualitatively illustrate the second-stage TCD by the metal-catalyzed carbons. Corresponding SEM illustrates differences in growth type and surface density between early versus late reaction times, with backscattered imaging differentiating the first- versus second-stage TCD. TGA supports the microscopic inference of a second carbon phase by the presence of an early (low-temperature) reaction peak, characteristic of low-structure or disordered carbon as the second-stage TCD carbon. Raman analysis confirms that the second-stage carbon deposit is more disordered and unstructured, especially at 1000 °C, supported by the ID/IG and La value changes from 0.068 to 0.936 and 65 nm to 4.7 nm, respectively. To further confirm second-stage TCD occurrence upon pre-catalyzed carbons, two carbon blacks are tested. Exposing a combination of edge and basal or exclusively basal sites for the graphitized form, they afford a direct comparison of TCD carbon nanostructure dependence upon the initial carbon catalyst nanostructure. Pre-oxidation of the stainless-steel wool (SSW) prior to TCD is advantageous, accelerating TCD rates and increasing carbon yield relative to the nascent SSW for an equivalent reaction duration.

Dynamics of regime transition of autoignitive jet flames from conventional to MILD combustion

Turbulent combustion of jet flames in a hot diluted coflow of combustion products has been studied across a range of jet Reynolds numbers for propane, ethylene, and an ethylene-propane blend as fuels. The study revealed a transition from conventional autoignitive combustion to a regime of Moderate or Intense Low-oxygen Dilution (MILD) combustion, which is characterized by a nearly invisible flame. The flames studied are luminous at low jet velocities and become MILD at higher jet velocities. Planar Laser-Induced Fluorescence (PLIF) of formaldehyde (CH2O), a key intermediate species in hydrocarbon combustion, is combined with CH*-chemiluminescence imaging and Rayleigh scattering to investigate the phenomena. The transition to MILD combustion is found to accompany a broadening of the formaldehyde region, indicating a broader low-temperature reaction zone. As the transition is approached, the appearance of holes in the chemiluminescent front is also observed. Correspondence between the location and structure of these holes with regions of formaldehyde in the flame are illustrated. These regions are proposed to be signatures that precede the transition to a fully MILD flame. In other words, the transition to MILD combustion begins at a local level and the MILD region spreads to engulf the entire combusting mixture. Scalar gradients were imaged to further unravel the local turbulence/chemistry interactions that yield the MILD inception. The measured scalar gradients were found to be commensurate with scalar gradients obtained from chemical kinetic simulations at the stoichiometric mixture fractions, while being an order of magnitude larger at other locations; this suggests that the inception of MILD combustion occurs near the stoichiometric region.

Highly Sensitive 3D‐Nanoplasmonic‐Based Epidermal Growth Factor Receptor Mutation Multiplex Assay Chip for Liquid Biopsy

Economical mutation detection method with high analytical and clinical sensitivity is necessary for early cancer diagnosis and screening. In this study, a novel 3D‐nanoplasmonic‐based multiplex mutation assay chip is developed to detect epidermal growth factor receptor (EGFR) mutations. This assay kit comprises a 3D‐nanoplasmonic substrate immobilized with capture probes and primer–probe sets for recombinase polymerase amplification, wild‐type inhibition, and fluorescence detection, enabling multiplex detection of EGFR exon 19 deletions, exon 20 insertions, and exon 21 L858R point mutations. The strategy facilitates the detection of all deletions and insertions within the target region with extremely high analytical sensitivity, detecting as low as 1 × 10−9% mutation frequency, implying three copies/reactions and 100 zM. The synergistic effects of plasmon‐enhanced fluorescence from the 3D‐nanoplasmonic substrate and wild‐type inhibitor contribute to this high analytical sensitivity. Moreover, the developed chip exhibits 100% accuracy in the clinical testing of plasma samples from normal individuals and patients with benign lung tumor and malignant lung tumor. With high sensitivity and multiplexing capabilities, this assay operates at a low reaction temperature (around 37 °C) and requires a short processing time, ≈70 min post‐cell‐free DNA extraction. These features make the chip a valuable tool for easy and widespread cancer screening.

In Situ Growth of Mn-Co3O4 on Mesoporous ZSM-5 Zeolite for Boosting Lean Methane Catalytic Oxidation

The low-temperature oxidation of methane gas in coal mine exhaust gas is important for reducing the greenhouse effect and protecting the environment. Unfortunately, the carbon–hydrogen bonds in methane molecules are highly stable, requiring higher reaction temperatures to achieve effective catalytic oxidation. However, metal oxide-based catalysts face the problem of easy sintering and the deactivation of active components at high temperatures, which is an important challenge that catalysts need to overcome in practical applications. In this work, a series of Mn-Co3O4 active components were grown in situ on ZSM-5 zeolite with mesoporous pore structures treated with an alkaline solution via a hydrothermal synthesis method. Due to the presence of polyethylene glycol as a structure-directing agent, manganese can be uniformly doped into the Co3O4 lattice. The large specific surface area of ZSM-5 zeolite allows the active component Mn-Co3O4 to be uniformly dispersed, effectively preventing the sintering and growth of active component particles during the catalytic reaction process. It is worth mentioning that the Mn-Co3O4/meso-ZSM-5-6.67 catalyst has a methane conversion rate of up to 90% at a space velocity of 36,000 mL·g−1·h−1 and a reaction temperature of 363 °C. This is mainly due to the mesoporous ZSM-5 carrier with a high specific surface area, which is conducive to the adsorption and mass transfer of reaction molecules. The active component has an abundance of oxygen vacancies, which is conducive to the activation of reaction molecules and enhances its catalytic activity, which is even higher than that of noble metal-based catalysts. The new ideas for the preparation of metal oxide-based low-temperature methane oxidation catalysts proposed in this work are expected to provide new solutions for low-temperature methane oxidation reactions and promote technological progress in related fields.

A facile green synthesis of gold nanoparticles using Canthium parviflorum extract sustainable and energy efficient photocatalytic degradation of organic pollutants for environmental remediation

Organic dye and nitrophenol pollution from textiles and other industries present a substantial risk to people and aquatic life. One of the most essential remediation techniques is photocatalysis, which uses the strength of visible light to decolorize water. The present study reports Canthium Parviflorum (CNP) leaf extract utilization as an effective bio-reductant for green synthesis of Au NPs. A simple, eco-friendly process with low reaction time and temperature was adopted to synthesize CNP extract-mediated Au-NPs (CNP-AuNPs). The prepared AuNPs characterization involving X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FT-IR), energy-dispersive X-ray spectroscopy (EDX), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron microscopy (XPS) surface area analysis, ultraviolet–visible spectroscopy (UV–Vis). XRD results showed that the cubic-structured AuNPs had a crystallite size of 14.12 nm. Assessment of organic dyes performance in degrading brilliant green (BTG) and amido black 10B (AMB) under visible light irradiation highlights an impressive 83.25% and 86% degradation efficiency within 120 min, accompanied by a kinetic rate constant dyes was found to be 0.0828 min⁻1, BTG, and 0.0123 min⁻1, Furthermore, the reduction of 4-nitrophenol by NaBH4 using CNP-AuNPs as a catalyst demonstrated good catalytic performance and rapid degradation at 89.4%. and rate constant 0.099 min−1 followed pseudo-first-order. The LC-MS analysis identified various intermediates during the degradation of the CR dye. Radical trapping experiments suggest that photogenerated free electrons and hydroxyl radicals are crucial for degrading the amido black 10B dye The AuNPs influenced the significant factors responsible for the photocatalytic activity, such as the increase in range of absorbance, increased e− and h+ pair separation, improvement in the charge transfer process, and active site formation, which significantly enhanced the process of degradation. We found that the CNP-AuNPs could effectively remove dyes and nitrophenol from industrial wastewater.

Reaction characteristics of Al–Mg alloy fuels with heterogeneous oxidation shell structures

Al–Mg alloy fuels are the most widely used Al-based alloy fuel in energetic material systems owing to their low ignition temperature and fast reaction. However, their surface oxide layer structure and oxidation, ignition, and combustion mechanisms differ from those of single-metal fuels. Furthermore, insufficient information has been reported on Al–Mg alloy fuels. In this study, Al–Mg alloy fuels were formed by introducing Mg into Al via centrifugal atomization. The microstructure and thermal reaction characteristics of the Al–Mg alloy fuel were evaluated. The ignition and combustion characteristics of the Al–Mg alloy fuels were monitored via single-particle ignition. When the Mg content was increased from 5 % to 40 %, a typical core–shell structure formed, the oxide shell thickness increased from 4.50 to 6.41 nm, and the content of the internal alloy compounds gradually increased. The surfaces of the Al–Mg alloy fuel particles with different Mg contents exhibited heterogeneous oxidation shells. Compared to Al powder, the Al–Mg alloy fuel exhibited better melting and oxidation peak temperatures and higher oxidation weight gain. As the Mg content was increased, the combustion of the Al–Mg alloy fuel intensified with more severe microexplosions and a shorter combustion time. The microexplosion of the Al–Mg alloy fuel was elucidated by theoretical calculations, and its combustion mechanism was proposed. The detailed description of the oxide layer structure, oxidation, and combustion of the Al–Mg alloy fuel provides a reliable explanation of its energy release mechanism in energetic material systems.

Tuning metastable austenite in a phase-transforming ceramic via matrix constraint

Martensitic phase-transforming ceramics can undergo reversible phase transformations under thermo-mechanical stimuli, yet brittle in their monolithic, polycrystalline form. Incorporating these ceramics into matrices thereby metastabilizing austenite gives rise to a significant toughening effect by triggering martensitic transformation. However, it remains a challenge to stabilize the austenite if the matrix is a light metal, because of its low strength, low melting temperature and high-chemical reactivity. In this study, we constructed a phase-transforming ceramic-metal (zirconia-aluminum) composite with tunable metastable austenite fractions via matrix constraint. Systematic experiments combined with thermodynamic and kinetic models uncover the effect of the matrix constraint and doping concentration on austenitization. By varying the processing parameters, we realized extensive tunability in metastable austenite content (0–100 wt.%) under different cerium doping concentrations (6–12 mol.%) in a wide range of processing temperatures (350–550°C). Our findings reveal the underlying mechanisms for promoting, stabilizing and fine-manipulating austenitization in martensitic phase-transforming ceramics under geometrical constraint, and may lay out the foundation for more extensive studies and applications of these phase-transforming ceramic-based composites.

Boosting low temperature CO2 methanation by tailoring Co species of CoAlO catalysts

The development of low-temperature CO2 methanation catalysts with excellent performance has been challenging. Herein, we report a CoAlO catalyst derived from layered double hydroxide (LDH) that modulates the Co species of a multifunctional catalyst through a reduction process. The CoAlO catalyst with a surface-coated CoO film achieved CO2 conversion up to 29.0 % at 160 °C, which was superior to that of noble metal catalysts. The multiple characterizations were used to reveal the relationship between the catalytic activity and the chemical state of Co species. The results showed that the reaction followed the H-assisted activation pathway, where the rate of formate intermediates generation determined the overall reactivity. Meanwhile, the reduction–oxidation (RO) process in the catalyst preparation and the water generated in the reaction could reduce the size of Co particles, which were favorable for CO2 activation. This work offers a promising catalyst design for low-temperature methanation reaction.

Spray autoignition study of bio-oxygenated additives blended with aviation kerosene under engine-like cold-start conditions

Abstract Bio-oxygenated fuels are expected to be used as a clean alternative energy source to improve the ignition behavior and pollutant emissions of RP-3 kerosene in compression ignition engines. In this study, the spray autoignition of PR-3 blended with different types of oxygenated fuels (including n-pentanol (PeOH), methyl propionate (MP), methyl ethyl ketone (MEK), 1,2-dimethoxyethane (1,2-DME), and 2-Ethylhexyl nitrate (EHN)) was measured using a constant-volume combustion chamber. Experiments were performed on three sets of blended fuels with different oxygen contents (2.5 wt%, 5 wt%, 10 wt%) in the temperature range of 723∼863 K and at ambient pressures of 2.2 and 4 MPa. A kinetic analysis utilized a merged RP-3 low-temperature kinetic model containing various oxygenated components. The ignition delay of blended fuels increases with the addition of PeOH, MP, and MEK, particularly PeOH, which demands more energy absorption at low temperatures due to its higher specific heat and latent heat of vaporization. As ambient pressure increased, the ignition delay period shortened for all blended fuels; however, PeOH and MEK demonstrated more significant low-temperature suppression. The combined kinetic model can reasonably predict the trend of the effect of oxygenated additives. 1,2-DME showed significantly more low-temperature reactivity versus PeOH, MP, and MEK. The variability is because the products of secondary O2 addition and isomerization of 1,2-DME undergo low-temperature branched chain reactions, but other oxygenated fuels produce more inert components.

Improved ignition and combustion performance of Al-Zn-Mg ternary alloys by incorporating Mg into Al-Zn alloys

Al-Zn alloys exhibited lower reaction temperature and micro-explosion phenomenon when compared to Al which benefited from the low melting point and boiling point of Zn. To further improve the energetic performance of Al-Zn alloys, Mg with low reaction temperature was originally incorporated into Al-Zn alloys via centrifugal atomization. The addition of Mg results in the production of Mg32(Al,Zn)49 with the low melting point and stepwise oxidation, which can effectively improve the reactivity and combustion. The results show that the prepared Al-Zn-Mg alloys display uniform particle size distribution, regular morphology, and excellent sphericity, which are composed of α-Al and Mg32(Al,Zn)49 compounds. The initiation oxidation temperature of AlZn10Mg5 and AlZn10Mg10 alloy powders is lower than that of AlZn10 alloy powders, and the oxidation efficiency is higher than that of AlZn10 alloys, which may be attributed to the oxidation of Mg32(Al,Zn)49. Adding Mg to the AlZn10 alloy significantly increases the peak pressure and pressurization rate during combustion. In the meanwhile, Al-Zn-Mg alloys burn faster, more intensely, and more completely when compared to AlZn10 alloys. The combustion of the spherical AlZn10Mg10 alloy powders is the most intense visually. It can be ascribed that during the combustion, a large amount of melt and gas breaks through the oxide layer, increasing the contact intimacy between oxygen and the alloy, which can significantly shorten the combustion time. In summary, the spherical AlZn10Mg5 and AlZn10Mg10 alloy powders prepared in this study show promising applications in fuels with high reactivity and better combustion performance.

Expanding the Scope of C-Glycoside Synthesis from Unstable Organolithium Reagents Using Flow Microreactors.

C-glycosides are versatile scaffolds for drugs and bioactive compounds. The common organolithium-based synthesis of C-glycosides is limited by low reaction temperatures and a restricted substrate scope. To address these issues, a flow microreactor (FMR) was utilized for rapid mixing and precise temperature control, enabling C-glycoside synthesis at temperatures up to 40 °C and expanding the substrate scope. Continuous C-glycoside synthesis was achieved with a throughput of 21.9 g h-1, demonstrating the industrial potential of FMRs.

Rational Design of Phase-Engineered WS2/WSe2 Heterostructures by Low-Temperature Plasma-Assisted Sulfurization and Selenization toward Enhanced HER Performance.

Efficient hydrogen generation from water splitting underpins chemistry to realize hydrogen economy. The electrocatalytic activity can be effectively modified by two-dimensional (2D) heterostructures, which offer great flexibility. Furthermore, they are useful in enhancing the exposure of the active sites for the hydrogen evolution reaction. Although the 1T-metallic phase of the transition metal dichalcogenides (TMDs) is important for the hydrogen evolution reaction (HER) catalyst, its practical application has not yet been much utilized because of the lack of stability of the 1T phase. Here, we introduce a novel approach to create a 1T-WS2/1T-WSe2 heterostructure using a low-temperature plasma-assisted chemical vapor reaction (PACVR), namely plasma-assisted sulfurization and plasma-assisted selenization processes. This heterostructure exhibits superior electrocatalytic performance due to the presence of the metallic 1T phase and the beneficial synergistic effect at the interface, which is attributed to the transfer of electrons from the underlying WS2 layer to the overlying WSe2 layer. The WS2/WSe2 heterostructure catalyst demonstrates remarkable performance in the HER as evidenced by its small Tafel slope of 57 mV dec-1 and exceptional durability. The usage of plasma helps in replacing the top S atoms with Se atoms, and this ion bombardment also increases the roughness of the thin film, thus adding another factor to enhance the HER performance. This plasma-synthesized low-temperature metallic-phase heterostructure brings out a novel method for the discovery of other catalysts.

Low-Temperature Methane Activation Reaction Pathways over Mechanochemically-Generated Ce4+/Cu+ Interfacial Sites.

Methane is a valuable resource and its valorization is an important challenge in heterogeneous catalysis. Here it is shown that CeO2/CuO composite prepared by ball milling activates methane at a temperature as low as 250°C. In contrast to conventionally prepared catalysts, the formation of partial oxidation products such as methanol and formaldehyde is also observed. Through an in situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) and operando Near Edge X-Ray Absorption Fine Structure Spectroscopy (NEXAFS) approach, it can be established that this unusual reactivity can be attributed to the presence of Ce4+/Cu+ interfaces generated through a redox exchange between Ce3+ and Cu2+ atoms facilitated by the mechanical energy supplied during milling. DFT modeling of the electronic properties confirms the existence of a charge transfer mechanism. These results demonstrate the effectiveness and distinctiveness of the mechanical approach in creating unique and resilient interfaces thereby enabling the optimization and refining of CeO2/CuO catalysts in methane activation reactions.

Microenvironment tailoring mediated highly dispersed Mn-O-Ce interface for low-temperature NH3-SCR of NOx

In creating Ce-Mn oxide catalysts for low-temperature NH3-SCR reactions, conventional pyrolysis usually leads to agglomeration on the catalyst surface, making it difficult to expose its active components. The realization of microenvironmental modulation to expose more Mn-O-Ce active interfaces remains a formidable task. In this work, we successfully synthesized Ce-Mn oxides with abundant and highly dispersed Mn-O-Ce interfaces via microwave radiation. This microwave-mediated microenvironmental modulation promotes high surface area, surface oxygen adsorption and acidic sites, which exhibit outstanding low-temperature NH3-SCR reaction performance. Meanwhile, this work also provides new ideas for microenvironmental modulation to synthesize high-performance catalysts.

The Structure Characteristics of Laminar Premixed Flames of Gasoline-like Fuel Under CI Engine-Relevant Conditions.

Gasoline compression ignition characterized by partially premixed and long ignition delays typically features complex flame structures such as deflagration or spontaneous ignition fronts. In this study, the flame structure and propagation characteristics of PRF90/air mixtures under compression ignition engine-relevant conditions are investigated numerically. Similar to other types of fuels, under such conditions, the propagation speed of PRF90 laminar premixed flames depends not only on the unburnt mixture properties but also on the residence time, and the transition of the flame regime depends only on the residence time. Nevertheless, due to the temperature-dependent autoignition chemistry of PRF90, flames with excessively high unburnt temperatures show different combustion behaviors after the transition from deflagration to autoignition-assisted flames. Sensitivity analysis showed that, the dominant chain branching reactions in the deflagration mode are H + O2 = OH + O and CO + OH = CO2 + H, and that in the autoignition-assisted flames with lower unburnt temperature are H2O2(+M) = 2OH(+M) and IC8H18 + HO2 = AC8H17 + H2O2, while for higher unburnt temperatures, the reactions C3H5 + HO2 = C2H3 + CH2O + OH and IC8H18 = IC4H9 + TC4H9 are more important than the fuel low-temperature oxidation reactions. In addition, a criterion based on chemical explosive mode analysis is used to analyze the local combustion mode. The results show that the difference in diffusion/chemical structure at the crossover progress variables C 0 and crossover temperature allows both C 0 and to be used as a flame location for distinguishing propagation modes in premixed flame. However, the effects of the equivalence ratio on C 0 are different from that on , which means that the selection of C 0 and may lead to different discriminant results for stratified mixtures. Comparing the applicability of C 0-based and -based locations in three-dimensional gasoline compression ignition flame, it is found that the flame location based on the value of C 0 at ϕ = 1.0 can more completely reflect the flame development characteristics in stratified premixed combustion.

Heat and mass transfer mechanistic investigation of wall intervention on spray ignition characteristics under aviation piston engine-like conditions

The interaction between spray and walls significantly influences the mixture formation and ignition characteristics in aviation piston engines, primarily due to the dynamics of heat and mass transfer. To elucidate the wall’s influence on the impingement spray ignition process and reconcile discrepancies in the extant literature, we conducted a comprehensive suite of optical experiments encompassing free and impinging sprays with wide ambient temperature conditions (680 to 1200 K). Numerical simulations were utilized to dissect the flow field’s distribution patterns, as well as heat and mass transfer dynamics. Our investigation reveals that impinging sprays exhibit markedly shorter ignition delay times than free sprays under comparable conditions, with this divergence becoming more pronounced at lower ambient temperatures. Notably, impingement sprays are capable of auto-ignition at reduced ambient temperatures. The spray-wall interaction effect accelerates the accumulation of heat from the low-temperature reaction, facilitating swifter attainment of the threshold temperature for the high-temperature reaction. This is attributable to the generation of a higher quantity of high-temperature mixtures with a diminished local equivalence ratio. The disparity in the ignition delay times between impinging and free sprays is exacerbated by the elevated heat demand for the transition from low-temperature reaction to high-temperature reaction at lower ambient temperature conditions, predominantly driven by the exothermic nature of low-temperature reaction.

Constructing highly active vanadyl species for efficient selective catalytic reduction of NOx

Vanadia-based catalysts have been commercially applied for selective catalytic reduction with NH3 of NOx (NH3-SCR). Considering the biotoxicity of V2O5, V-based catalysts are demanded to exhibit high catalytic activity with low V2O5 loadings. However, at low vanadium contents, surface VOx primarily present in the form of monomers, which show poor low-temperature activity. Here, efficient low-vanadium-loading catalysts were designed via constructing highly reactive polymeric vanadyl species by introducing disparate forms of niobia species. Niobia species were found to promote the polymerization of surface VOx, and the disparate forms of niobia species had a key influence on the formation of polymeric vanadyl species. Crystalline Nb2O5 promoted the formation of polymeric vanadyl species, induced by a structural effect. By contrast, uniformly dispersed niobium species on the surface of a Nb-Ti-O solid solution support served as new anchoring sites for VOx and promoted a greater extent of polymerization of VOx species via electronic interactions among V, Nb and Ti. Ultimately, Nb-Ti-O solid solution-supported V2O5 exhibited much higher low-temperature reaction rates than TiO2-supported Nb2O5 and V2O5 due to more polymeric vanadyl species. This study provides new methods to design low-vanadium-loading catalysts, offering new perspectives for the modification of transition metal oxides to design efficient catalysts.