Weak Oxidation Research Articles

Improved mechanical properties of GNPs/Al composites by eliminating alumina and obtaining a strong bonded GNPs-Al direct contact interface and Mg-rich phases

The interface between Graphene Nanosheets and Aluminum (GNPs-Al) without carbide and transition layers is referred to as a direct-contact GNPs-Al interface. In this work, the GNPs-reinforced aluminum matrix composites are fabricated by ultrasonic casting process. The interfacial structure of GNPs-Al is investigated using transmission electron microscopy, and the strength of the fabricated direct-contact GNPs-Al interface is analyzed. The results identified the presence of weak amorphous aluminum oxide at the original GNPs-Al interface. The direct contact GNPs-Al interface was obtained by introducing Mg. The migration of Al atoms formed an Al/C mixing zone between GNPs-Al, which led to the enhancement of the interface strength. The average UTS value has improved by about 20.5% due to the optimization of the interface structure. The enhancement of strength at the same toughness is achieved by the load transfer of GNPs, bridging, and the enhancement of dislocation storage capacity by the Mg-rich phase. The present work provides a new reference for the reinforcement of cast aluminum alloys by GNPs.

Elucidating the low temperature chemistry of o-xylene enhanced by the reaction pool of dimethyl ether

The branched aromatic hydrocarbon with short side chains, such as o-xylene, has weak low temperature oxidation reactivity, while it could proceed low temperature chain recycling reactions by blending a fuel component with higher oxidation reactivity. However, the study of low temperature oxidation kinetics of o-xylene is very scarce. Therefore, this work investigated the low temperature oxidation process of o-xylene in an atmospheric jet stirred reactor by adding a biofuel with higher low temperature oxidation reactivity, i.e. dimethyl ether (DME). A series of characteristic low temperature intermediates, such as phenyl hydroperoxides and ketohydroperoxide from the oxidation of o-xylene, were detected by using the synchrotron vacuum ultraviolet photoionization mass spectrometry (SVUV-PIMS). The chemical structures of representative low temperature intermediates were determined by comparing the ionization thresholds from measured photoionization efficiency curves with calculated ionization energies. A kinetic model for o-xylene and DME mixture was developed and verified by literature and present experimental data. Rate of production (ROP) and sensitivity analyses were performed, which indicate that the low temperature oxidation chemistry of o-xylene, such as the negative temperature coefficient behavior, is enhanced by the reaction pool of DME. According to the classical low temperature oxidation mechanism of n-alkanes, the low temperature reactions of o-xylene were proposed. In particular, phenyl hydroperoxides and ketohydroperoxides were revealed to be key indicators for the occurrence of first and second O2 addition reactions during the oxidation of o-xylene, respectively. In addition, the sensitivity analysis uncovers the interaction kinetics between the reaction pools of o-xylene and DME, as well as their effects on fuel consumption and products formation. In summary, present evidence elucidates the low temperature chemistry of a representative branched aromatic, which could contribute to the development of future engines and control of combustion pollutants.

Correlation Between Chang‐9 Crude Oil and Potential Source Rocks, Upper Triassic Yan‐Chang Formation, Middle Area of Ordos Basin: Correlation Between Crude Oil in the Chang‐9 Member and Potential Source Rocks

The Chang 9 oil layer deposits within Ansai District, Ordos Basin, yield considerable reserves of crude oil, yet their source remains ambiguous. This research endeavor was designed to characterize the Chang 9 crude oil and the Chang 7 and Chang 9 source rocks (SRs) of the Yan‐Chang Formation via organic geochemical analysis. The results indicate that the Chang 9 crude oil exhibits a Pr/Ph ratio of 0.84–2.29 and Ga/C30H less than 0.1, implying formed in a weak reduction to weak oxidation freshwater environment. The regular sterane C27‐C28‐C29 configuration assumes an inversed “L” type, reflecting mixed sources and dominant terrestrial plant input. Ratios such as C2920S/(20S + 20R) (0.54–0.6) and C29ββ/(ββ + αα) (0.44–0.58) indicate a mature oil stage. The depositional environment of the C7 and C9 SRs is similar, with weak oxidation to reduction conditions, and consists mainly of Type I and II organics, with a relatively higher maturity of the C9 SRs. A difference in C19/C23TT and C30D/C30H was found between the C7 and C9 SRs. The results show that the C9 crude oils have a similar C19/C23TT with the C9 SRs and similar diahopanes distribution with Class II SRs (C7 and part of the C9 SRs). Thus, the C9 crude oils most likely originate from the C9 SR mixed with the C7 SRs.

Revealing the low to moderate temperature oxidation kinetics of 1,2,4-trimethylbenzene sensitized by dimethyl ether

Low to moderate temperature oxidation has been a vital topic in the combustion chemistry due to its critical role in controlling the combustion characteristics such as autoignition and pollutant emissions. Low temperature oxidation kinetics of alkanes and oxygenated biofuels have been widely explored, while that of branched aromatics is poorly understood. This work aims to investigate the low to moderate temperature oxidation kinetics of 1,2,4-trimethylbenzene (TMB, C9H12), which is a multi-branched alkylbenzene with weak low temperature oxidation reactivity. To enhance the low temperature oxidation reactivity of TMB, dimethyl ether (DME) was added to efficiently provide chain initiators. The oxidation experiment of TMB/DME mixture was performed with an atmospheric jet stirred reactor coupled with synchrotron vacuum ultraviolet radiation photoionization mass spectrometry. The negative temperature coefficient (NTC) behavior, as well as featured aromatic intermediates, especially phenyl hydroperoxides and unexpected highly oxygenated molecules (HOMs), were observed in the experiment. The detection of these fingerprint aromatic intermediates provide crucial evidence for revealing the low to moderate oxidation kinetics of TMB. In addition, a kinetic model was developed to provide in-depth kinetic analysis. The results demonstrate that the active chain initiators produced from DME oxidation trigger the low temperature chain-branching reactions of TMB. The chain recycling process is further sustained due to the regeneration of active intermediates such as phenyl hydroperoxides and •OH radicals. Aromatic intermediates with chemical compositions of C9H12Ox and C9H10Ox were measured and identified to be key indicators for the low temperature chemistry of TMB. In particular, the aromatic HOMs (C9H12O6 and C9H10O5) are fingerprint intermediates produced from the third O2 addition and subsequent reactions of TMB. Besides, the sensitivity analysis indicates that the interaction kinetics between TMB and DME by sharing the highly sensitive reactions of hydroperoxides and •OH radicals. The present work extends the conceptual reaction schemes proposed in alkanes towards branched aromatics, especially sequential O2 addition reactions that contributing to the formation of phenyl hydroperoxides and HOMs.

Paleoenvironmental, Paleoclimatic, and Tectonic Implications of the Yanghugou Formation in the Western Margin of the Ordos Basin, China: Evidence from Palynology and Elemental Geochemical Characteristics

This study explores the sedimentary environment and tectonic implications of the Upper Carboniferous Yanghugou Formation on the western margin of the Ordos Basin through the analysis of major elements, trace elements, and rare earth elements in 23 mudstone samples. The results indicate moderate chemical weathering conditions, as reflected in the Chemical Alteration Index (CIA) and Component Variability Index (ICV) values. Warm and humid paleoclimatic conditions are suggested by Rb/Sr, Sr/Cu, spore, and pollen fossil samples. The paleosalinity of the water is identified as a transitional phase of a brackish water environment based on Sr/Ba and Th/U ratios. Additionally, V/(V + Ni) and δU values imply a transitional phase of a weak oxidation–reduction environment for the water. In accordance with the La-Th-Sc, Th-Sc-Zr, Th-Co-Zr, (La/Yb)-∑REE, and (La/Th)-Hf discrimination diagrams, it is inferred that the study area is part of a continental marginal tectonic setting. The sediments are primarily derived from an upper-crust felsic source area. The sedimentary period of the Yanghugou Formation in the western margin of the basin is considered a marginal rift basin characterized by north–south compression and western rift extension. This setting is influenced by the active continental margin of the Alxa block and the passive continental margin of the Qilian–north Qinling orogenic belt.

Old Sulfidic Ore Tailing Dump: Ground Features, Mineralogy, Biodiversity—A Case Study from Sibay, Russia

The Urals (Russia) are among the largest mining areas in the world, with millions of tons of mine waste deposited. An old sulfidic tailing dump formed over decades of mining activities at the Sibay ore-processing plant is a typical cause of acid mine drainage (AMD) formation, posing a threat to ecosystems of neighboring environments. In this study, the formation of oxidized surface soil layers in four zones of the Sibay tailing dump was revealed, and their chemical–mineralogical and physical–mechanical characteristics were analyzed. According to the results of the metabarcoding of hypervariable regions of the 16S rRNA genes, oxidation in soil layers was associated with the activity of sulfur- and iron-oxidizing acidophiles represented by a few genera: Ferroacidibacillus, Sulfoacidibacillus, Sulfobacillus, and Ferroplasma. The structure of the microbial communities in soil layers differed depending on the zone and depth of sampling. In the samples characterized by the weak oxidation of sulfide minerals, microbial communities were dominated by bacteria of the genus Pseudomonas. The data obtained in this research are of importance to predict the oxidation/leaching processes in mine wastes and their negative environmental impacts in the mining region, as well as to develop technologies for processing these raw materials.

Electro-Chemo-Mechanical Coupling in Hierarchical Nanoporous Gold-Polypyrrole-Water Hybrids

Nanoporous (np) metals made by dealloying is a novel class of nanostructured materials that offers numerous functionalities, ranging from sensing, energy storage, to (electro-)catalysis and beyond. A substantial amount of research in np materials has been focused on np gold due to its excellent structural and chemical stability, adjustable pore size, high conductivity, biocompatibility, and easy fabrication process via free corrosion or electrochemical dealloying. A considerable number of studies have been conducted to investigate np gold infiltrated with an aqueous electrolyte [1]. In that way, the material is considered as a hybrid so that one can reversibly tune the gold surface state by manipulating the superficial charge densities or adsorbate coverages via the applied electric potential [1]. The above-mentioned approach results in a number of intriguing properties of np Au revealed upon electrode potential variation in aqueous electrolytes such as actuation [2, 3], sensing [4], tunable strength [5] and elastic modulus [6]. The behavior is well-studied in case of weak ion adsorption and surface oxidation.One of the promising methods towards further improvement of functional and mechanical properties of np metals was implemented by Roschning and Weissmueller [7]. It was shown that the actuation strain of np Au can be enhanced via electrodeposition of a conductive polymer polypyrrole (PPy) on the gold surfaces. The actuation strain of the np Au-PPy hybrids strongly scales with the PPy phase fraction. Moreover, Li et al. [8] observed variations of effective elastic modulus in np Au-PPy-water hybrids. Thus, introducing the conductive polymer into a pore space of the np metal yields a hybrid actuator with a significantly improved actuation amplitude and yield strength.Here, we employ PPy for surface functionalization of hierarchical (hc) np Au (Figure 1) to explore the impact of the conductive polymer coating on the functional behavior of the hierarchically structured np metals. Np metals with structural hierarchy made by dealloying [9] open up new opportunities for multifunctional hard-soft hybrids. The larger pores at the higher hierarchical level (characterized by diameters around 120 nm) can promote fast mass exchange, while nanopores at the lower hierarchy level (below 30 nm) provide a large surface area and high chemical activity. Actuation behavior of the hybrid materials was analyzed in situ in a dilatometer upon potential cycling in a 1 M HClO4 aqueous electrolyte. The elastic response was examined in situ in a dynamic mechanical analyzer in the same electrolyte. We revealed pronounced changes of the macroscopic length and Young’s modulus in response to the voltage-induced redox reactions of the polymer films at the np electrodes. In the contribution, we discuss the origin of the electro-chemo-mechanical coupling phenomena.[1] Shao et al., in Nanoporous Gold: From an ancient technology to a high-tech material. RSC (2012).[2] Kramer et al. Nano Lett., 4(5) 793 (2004).[3] Jin et al. Nano Lett., 10(1) 187 (2010).[4] Stenner et al., Adv. Funct. Mater. 26 (28), 5174 (2016).[5] Jin et al., Science 332, 1179 (2011.)[6] Mameka et al., Acta Mater. 76, 272 (2014).[7] Roschning et al., Adv. Mater. Interfaces, 2001415 (2020).[8] Li et al., Acta Mater., 212 (1), 116852 (2021).[9] Shi et al., Science 371, 1026 (2021).Figure 1. Scanning electron micrograph of hierarchical nanoporous Au-PPy hybrid microstructure. Figure 1

(Invited) Dye-Sensitized Molecular Photoelectrodes for CO2 Reduction Using Water as a Reductant

Photocatalytic CO2 reduction using visible light and water as a reductant has been one of the important targets for solving global warming problem and shortage of energy and carbon resources. In this presentation, I talk about two projects, i.e., (1) supramolecular photocatalysts with both functions as photosensitizer and catalysts and (2) photocatalytic CO2 reduction coupled to water oxidation.(1) Highly efficient supramolecular photocatalysts for CO2 reduction1-3 Since CO2 is the most oxidized state of carbon, one-electron reduction of CO2 is an extraordinarily high endergonic reaction. From the viewpoints of low-energy light application, the multi-electron reduction of CO2 via chemical reactions promises to be a more valuable process. This is a main reason why both a photosensitizer and a catalyst are required to promote efficient photocatalytic CO2 reduction. We have developed so-called supramolecular photocatalyts that have both the photosensitizer and the catalyst units. This bonding in the supramolecular photocatalysts can accelerate electron transfer between the two units, which improves the performance of the photocatalytic system, especially on the surface of photofunctional solid materials as described below.(2) Molecular photoelectrodes for photocatalytic CO2 reduction with water as a reductant 1,4 The molecular photocatalytic systems have a weakness, i.e., weak oxidation power in the excited state. For practical application, water should be used as an electron donor. For overcoming this problem, we have developed a hybrid system consisting of the supramolecular photocatalyst and semiconductor electrodes. The hybrid photoelectrochemical cell consisting of this hybrid photocathode and n-type semiconductor photoanode induced visible-light-driven CO2 reduction with water as a reductant to generate CO and O2. References “Photocatalytic Systems for CO2 Reduction: Metal-Complex Photocatalysts and Their Hybrids with Photofunctional Solid Materials” Kumagai, H.; Tamaki, Y.; Ishitani, O., Acc. Chem. Res. 2022, 55, 978-990.“Mechanistic study of photocatalytic CO2 reduction using a Ru(II)-Re(I) supramolecular photocatalyst” Kamogawa, K.; Shimoda, Y.; Miyata, K.; Onda, K.; Yamazaki, Y.; Tamaki, Y.; Ishitani, O., Chem. Sci. 2021, 12, 9682-9693.“Supramolecular Photocatalysts for the Reduction of CO2” Tamaki, Y.; Ishitani, O., ACS Cat. 2017, 7, 3394-3409.“Supramolecular photocatalysts fixed on the inside of the polypyrrole layer in dye sensitized molecular photocathodes: application to photocatalytic CO2 reduction coupled with water oxidation. Kuttassery, F.; Kumagai, H.; Kamata, R.; Ebato, Y.; Higashi, M.; Suzuki, H.; Abe, R.; Ishitani, O., Chem. Sci. 2021, 12, 13216-13232. Figure 1

Synergistic reduction on PM and NO source emissions during preheating-combustion of pulverized coal

The present research focuses on the synergistic source control of particulate matter (PM) and NOx formation from pulverized coal combustion. Comparative experiments of preheating-combustion and conventional combustion were conducted in a lab-scale high-temperature preheating-combustion furnace, and PM10 and NO were measured by an electrical low pressure impactor and a flue gas analyzer, respectively. The results of the experiment indicate that preheating-combustion has a significant reduction in PM10 (especially PM0.3 up to 37.51 %) and NO, which can achieve the synergistic control of PM10 and NO source emissions during the combustion process. The fragmentation in preheating-combustion was weaker compared to the conventional combustion. Meanwhile, the relatively weak preheating-combustion coal char oxidation reaction leads to a decrease in ultrafine mode PM yielded due to the inhibition on vaporization of mineral inclusions. The PM0.3/PM1 mass ratio of the preheating-combustion has a decreasing trend, implying an elevated yield of PM0.3-1 and a shift of the average PM1 particle size toward a larger particle size. Higher preheating temperature (Tp) presented the potential to further reduce NO formation, and the NO reduction efficiency increased from 46.59 % to 56.60 % when the Tp was increased from 1200 K to 1600 K. All our preliminary results throw light on the nature of synergistic source control of preheating-combustion PM and NO formation.

Color origin and its sedimentary and paleoenvironmental significance of the Permian-Triassic strata in the Ordos Basin, China

The Permian-Triassic strata in the Ordos Basin deposit a colorful set of strata. Although there have been many studies on oil and gas resources here, little attention has been paid to the genesis mechanism of its color. To analyze the color origin of the Permian-Triassic claystones and to clarify the dialectical relationship between rock color and sedimentary environment, petrological and geochemical methods such as polarization microscope, scan electron microscope, X-ray diffractometer, and inductively coupled plasma-mass spectrometer are used. The results indicate that the minerals with different colors, composition, and content serve as colorants in sedimentary rocks, with the predominant dyeing component in dark claystones being the organic matter, whereas red beds primarily acquire their color from hematite and other ferric minerals. In addition, different rock colors correspond to distinct chemical composition variations. The black-gray rocks of the Yanchang and Shihezi Formations have high total organic carbon content, Fe2+/Fe3+, V/Cr, and low CaO/(MgO × Al2O3) and Sr/Cu, whereas the red-brown rocks of the Liujiagou and Heshanggou Formations exhibit the opposite. Therefore, different colors of the rocks stem from their different mineral and chemical compositions, which in turn influenced by the changes in the paleoclimate, paleoenvironment, and tectonic movements. Comprehensive analysis of color, mineral, and chemical composition reveals the evolution process of paleoclimate and paleoenvironment in the Ordos Basin from the late Permian to Triassic, beginning with a warm humid climate characterized by a weak oxidation environment in the Shihezi and Shiqianfeng Formations, transitioning to a hot arid climate in the Liujiagou and Heshanggou Formations, and returning to a warm humid climate with a weak oxidation environment in the Zhifang and Yanchang Formations. This evolution history aligns with the global tectonic and climate evolution. Overall, systematic analysis of sedimentary rock color can provide an important basis for the study of the paleoclimate and paleoenvironment.

Structure, mechanical, tribological properties and corrosion resistance of C/N dual doping Mo-S-C-N films

Transition metal dichalcogenides (TMDs) show poor mechanical properties and weak corrosion and oxidation resistance in ambient atmosphere, which results in the limit application and the lower work life. Doping TMDs based films with the enhanced performance show the potential to apply in harsh environment. The C/N dual-doping Mo-S-C-N films were deposited by magnetron sputtering, and the evolution of alternative microstructure composed of TMDs phase and amorphous inclusions was analyzed. The enhancement on mechanical, tribological and anti-corrosion properties of films with C/N dual-doping were evaluated. The strengthened TMDs phase and inclusions with MoCx/MoNx hard phase result in the improvement of mechanical properties (hardness 8.57–19.09 GPa). The superior tribological performance was obtained from film with 10.67 at. % of C and 17.36 at. % of N (wear rate 8.24 × 10-7 mm3/Nm, average friction coefficient (CoF) 0.188) and film with 14.87 at. % of C and 15.02 at. % of N (wear rate 8.02 × 10-7 mm3/Nm, average CoF 0.166). The balance between the effect of lubricating phase and mechanical performance strengthen by C/N dopants were achieved in these two films. The passivation of reactive sites in MoS2 leads to the improvement of corrosion resistance, while excessive dopants induce more pathways for corrosive medium, which leads to the corrosion failure of films.

Distribution and dynamics of antibiotic resistance genes in sludge under discharge plasma oxidation

Antibiotic resistance genes (ARGs), emerging environmental contaminants, have been largely accumulated in sludge during wastewater treatment. Discharge plasma oxidation, an advanced oxidation technology, has been demonstrated as an effective strategy in sludge pretreatment. However, the effect of plasma oxidation on the distribution and dynamics of ARGs in sludge is unknown. Herein, the variations of four typical ARGs (tetC, tetW, blaTEM-1, aac(3)-Ⅱ) and one integron (intI-1) in sludge during discharge plasma treatment were investigated. The results showed that under low discharge voltage or short treatment time, weak plasma oxidation enriched the contents of ARGs and intI-1 in sludge (with 1.14 log unit maximum increment) via proliferating biomass or promoting horizontal gene transfer. Further increasing discharge voltage or prolonging treatment time, strong plasma oxidation eliminated target genes due to the destroyed bacteria or inhibited horizontal transfer of ARGs. Especially, the homogeneous condition greatly promoted the reduction of ARGs in liquid phase (up to 1.52 log unit reduction). Furthermore, the correlation analysis between intI-1 and ARGs implied that tetC and tetW abundances might be significantly affected by intI-1 through horizontal transfer. At the same time, the microbial communities in sludge were investigated to help understand the effect of plasma oxidation on ARGs variation. Notably, the most predominant phylum Proteobacteria and genus Acinetobacter resisted the oxidative infringement from plasma to maintain high relative abundances (52.05 % in solid phase and 84.10 % in liquid phase for Proteobacteria, 13.82 % in solid phase and 78.00 % in liquid phase for Acinetobacter at 20 kV). Meanwhile, the co-occurrence analysis between genes and dominant genera further showed that Romboutsia sp. might be a potential host bacteria of ARGs and intI-1 in solid phase, and Acidovorax sp., Parachlamydia sp., and Armatimonadetes_gp5 sp. might be the potential hosts of tetW, tetC, and intI-1 in liquid phase.

Oxygen vacancy-driven strong metal-support interactions on AuPd/TiO2 catalysts for high-efficient air-oxidation of 5-hydroxymethylfurfural

The regulation ofstrong metal-support interactions (SMSI) has emerged as a powerful strategy in boosting catalytic activity and controlling product selectivity. However, directly tuning the metal-supportinteractions in oxide supported metal nanocatalysts remains challenging. Herein, citric acid (CA)‑assisted synthesized TiO2 layer on halloysite nanotubes (HNTs) with varied oxygen vacancies (Ov) concentrations was designed for loading AuPd nanoparticles. SMSI between the AuPd nanoparticles and the TiO2-xCA@HNTs support was successfully induced by adjustable Ov concentrations. The synthesized catalyst was employed for air-oxidation of bio-based 5-hydroxymethylfurfural (HMF) to bioplastic monomer 2,5-furandicarboxylic acid (FDCA) in water. A satisfactory FDCA yield of 98.4 %, accompany with an outstanding FDCA formation rate of 900.9 mmol·g−1·h−1 and an excellent TOF value at 441.2 h−1 was afforded. Based on catalysts characterizations and experimental studies, the catalytic performance was significantly affected by Ov concentrations. The kinetic study showed that the supported gold nanoparticles in alkaline environment had strong aldehyde oxidation activity but weak alcohol oxidation ability. On the contrary, supported palladium nanoparticles were more conducive to alcohol oxidation. This imbalance was overcome by the loading of AuPd nanoparticles, which enhanced the activity for air-oxidation of HMF. Mechanistic studies demonstrated that the stronginteractions between noble metal nanocatalysts and supports were regulated by Ov, which not only increased the adsorption capacity of the substrate and crucial intermediate, but also facilitated the adsorption and activation of molecular oxygen to generate oxygen active species of superoxide radicals. The possible catalytic mechanism for air-oxidation of HMF over Ov-driven SMSI on the obtained catalysts was proposed. This work sheds lights on the design of supported metal catalysts with SMSI for the catalytic upgrading of biomass-derived platform chemicals.

Improving low-temperature NH3-SCR denitration activity and resistance to H2O and SO2 over Nb-modified NbaSn0.3CeOx catalysts by enhancing acidity to compensate for its weak oxidation ability

In this paper, a series of Nb-modified NbaSn0.3CeOx (a = 0.2, 0.4, 0.5) catalysts for denitrification were prepared using a facile co-precipitation method. In order to explore the various individual properties of the samples, the catalysts were characterized by XRD, Raman, N2 adsorption and desorption, TEM, NH3-TPD, H2-TPR, XPS and in-situ DRIFTS tests to understand the influences of the Nb introduction on the NH3-SCR reaction. Among these catalysts, the Nb0.4Sn0.3CeOx catalyst exhibit excellent NH3-SCR performance in the temperature range of 155–450 °C with more than 90 % NO conversion, 100 % N2 selectivity, and possess good resistance to H2O and SO2. Compared with the Sn0.3CeOx catalyst, we believe that the improvement of the low-temperature NH3-SCR performance of the Nb0.4Sn0.3CeOx catalysts is mainly due to the change in the amount of acid, special for the increase in B acid content, which compensates for the effect of the weaken oxidizing ability on the low-temperature activity. Beyond that, the good H2O and SO2 resistance at low temperature after the introduction of Nb into Nb0.4Sn0.3CeOx catalysts was analyzed by using in-situ DRIFTS characterization in detail, and the results indicate that the incorporation of Nb can inhibit the oxidation of SO2 to form sulfate on the catalysts, and prevent the competing adsorption of H2O and NOx, but the adsorption of NH3 is not affected. This work proves that the acidity regulation can improve low-temperature SCR activity by the synergistic effect between oxidation capacity and acidity.

Aging effects on residential biomass burning emissions under quasi-real atmospheric conditions

Emissions from biomass burning (BB) vastly contribute to the atmospheric trace gases and particles, which affect air quality and human health. After emission, the chemical evolution changes the mass and composition of organic aerosol (OA) in the diluted and aged plume. In this study, we used a quasi-real atmospheric smog chamber system to conduct aging experiments and investigated the multiphase oxidation of primary organic aerosol (POA) and the formation of secondary organic aerosols (SOA) in residential biomass burning plumes. We found that the emissions in the gas and particle phases were interlinked during the plume evolution. During photochemical aging, more oxidized OA was produced, and SOA formation increased by a factor of 2 due to functionalization reactions of gaseous precursors such as furans, phenols, and carbonyls. On the other hand, dark aging resulted in a lower OA mass enhancement by a factor of 1.2, with weaker oxidation from gaseous reactions. Dark aging experiments resulted in the generation of substantial quantities of nitrogen-containing organic compounds in both gas and particulate phases, while photochemical aging led to a notable increase in the concentration of gaseous carboxylic acids. Our observations show that the properties of SOA are influenced by exposure to sunlight radiation and oxidants such as OH or NO3 radicals. These results reflect the aging process of BB plumes in real-world atmospheric conditions and highlight the importance of considering various aging mechanisms.

Enhanced corrosion resistance of ammonium heptamolybdate (AHM) sealed Li[sbnd]Al LDHs conversion coating on aluminum alloy

In this study, we prepared a hierarchical structured coating via a versatile two-step approach for the protection of 6N01 aluminum alloy. On the basis of as-prepared secondary alkane sulphonate (SAS) modified LiAl LDHs conversion coating (SLDH) by in-situ synthesis method, ammonium heptamolybdate (AHM) was introduced in the post-treatment to fabricate AHM@SLDH with enhanced corrosion resistance. The surface morphology, chemical composition and corrosion performance are characterized by means of scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS), potentiodynamic polarization (PDP) and electrochemical impedance spectroscopy (EIS), etc. The hybrid coating has a persistence corrosion resistance in 3.5 wt% NaCl aqueous solution with protective efficiency of 99.64 %. As a highlight, a self-repairing function is detected in the immersion test, which is attributed to the weak oxidation function of Mo (VI). We believe that AHM@SLDH in-situ grown on aluminum substrate can provide a promising route for its corrosion prevention.

Study on the role of solution treatment on corrosion behavior of duplex lightweight steel in different environments

Diverse microstructure and complex application environments increases the uncertainty of the corrosion resistance of lightweight steels. The effect of solution treatment on the corrosion behavior of Fe–16Mn–10Al–1.5C–0.1Ti lightweight steel in Cl−, HSO3− and Cl−–HSO3− environments was investigated using electrochemical measurement, scanning electron microscope (SEM) and X–ray photoelectron spectroscopy (XPS). The lightweight steels are dominated by austenite and contain a small amount of ferrite. The increase in solution treatment temperature leads to more ferrite formation, but it has less effect on grain size. The decrease in austenite content results in more corrosion microcells and a porous oxide film; therefore, the corrosion resistance of the steel deteriorates with increasing temperature. In addition, in the Cl−–HSO3− environment, the synergistic effect of Cl− and HSO3− leads to the formation of a weak protective oxide film, resulting in a significant increase in corrosion rate compared to the Cl−and HSO3− environment.

Fe-Ni bimetallic adsorbent for efficient As2O3 removal from coal-fired flue gas under a wide temperature range: Experimental and DFT study

Adding metal oxides in the furnace can effectively control the emission of heavy metal arsenic in the coal-fired flue gas, and α-Fe2O3 has excellent adsorption performance. However, single metal oxides still have defects such as easy sintering or weak oxidation ability during use, which significantly impact the adsorption effect of arsenic. In this work, a new Fe-Ni bimetallic adsorbent was prepared by hydrothermal calcination, and its mechanism of As2O3 adsorption was investigated in depth through the combination of experiment and theory. The experimental results show that the FN8 (Ni-doped molar percentage is 8%) adsorbent exhibits excellent performance, and its arsenic adsorption capacity reaches 405.60 mg/kg, which is more than twice the adsorption capacity of α-Fe2O3. Ni doping can not only regulate the electron transfer between the α-Fe2O3 interface and As, but also promote the conversion of lattice oxygen to chemisorbed oxygen in the system. In the temperature range of 500 °C–900 °C, the prepared FN8 adsorbent can maintain a good microsphere structure, avoid sintering and provide more adsorption sites, and its arsenic capture capacity is stronger than α-Fe2O3. The density functional theory further reveals the microscopic mechanism of improving the oxidation performance of Fe-Ni adsorbent. The results show that Fe-Ni adsorbent has lower adsorption energy than α-Fe2O3. This is due to the synergism of Ni and O, which leads to the redistribution of electrons on the α-Fe2O3 (001) surface, and the Ni atom provides more free electrons for O atoms, which ultimately promotes the oxidation ability of Fe-Ni adsorbent and forms an As-O covalent bond. The Fe-Ni bimetallic composite adsorbent proposed in this work provides a new idea of bimetallic adsorbent for the effective adsorption of arsenic in the flue gas.

Suzuki-Miyaura Type Regioselective C-H Arylation of Aromatic Aldehydes by a Transient Directing Strategy.

Herein, we disclose a common approach for palladium-catalyzed direct coupling of the ortho-C-H bond of aromatic aldehydes with various organoboronic reagents by a transient directing strategy. In contrast to widely used cross-coupling reactions of C-H bonds with aryl halides, which generally need silver salt as a halide removal reagent, the method which used BQ/TFA as weak oxidation system for the PdII/Pd0 redox cycle is cost-effective, ecofriendly, and more aligned with green catalysis. This broadly applicable method opens up a new and efficient Suzuki-Miyaura coupling route for the direct formation of carbon-carbon bonds by C-H bond activation.

Influence of adding Nb on oxidation resistance of hypoeutectic high-chromium cast iron

This experiment investigates the effect of Nb on the oxidation resistance of high-chromium cast iron by adding different contents of Nb to high-chromium cast iron. The experimental results show that the oxidation resistance of high-chromium cast iron with the addition of 1 wt% Nb is increased by 43% compared with high-chromium cast iron without the addition of Nb, which may be related to the formation of a large area of weak oxidation area on the surface of high-chromium cast iron. When more than 2.5 wt% Nb is added to high-chromium cast iron, the oxidation resistance of high-chromium cast iron deteriorates significantly due to a large amount of Fe oxide formed around the Nb2O5. However, as the subsequent Nb content continues to increase to 5 wt%, the oxidation resistance of high-chromium cast iron is improved compared to 2.5 wt% Nb because the dispersion of NbC in the matrix decreases.