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1.
J Environ Manage ; 366: 121878, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-39018845

RESUMO

Traditional activators such as sodium hydroxide and sodium silicate are commonly used in the preparation of alkali-activated materials; however, their significant environmental impact, high cost, and operational risks limit their sustainable use in treating solid waste. This study explores the innovative use of carbide slag (CS) and sodium metasilicate (NS) as alternative activators in the production of sewage sludge ash-based alkali-activated materials (SSAM) with the aim of reducing the carbon footprint of the preparation process. The results demonstrate that CS effectively activates the sewage sludge ash, enhancing the compressive strength of the SSAM to 40 MPa after curing for 28 d. When used in conjunction with NS, it synergistically improves the mechanical properties. Furthermore, the microstructure and phase composition of the SSAM are characterized. Increasing the quantities of CS and NS accelerates the dissolution of the precursor materials, promoting the formation of a higher quantity of hydration products. This significantly reduces the number of voids and defects within the samples, further enhancing the densification of the microstructure. Environmental assessments reveal that CS and NS offer substantial sustainability benefits, confirming the feasibility of activating SSAM using these materials. This approach provides a less energy-intensive and more environmentally friendly alternative to conventional activation methods and presents an effective strategy for managing large volumes of sewage sludge ash and CS.


Assuntos
Esgotos , Silicatos , Silicatos/química , Esgotos/química , Álcalis/química , Resíduos Sólidos
2.
Sci Rep ; 14(1): 14861, 2024 Jun 27.
Artigo em Inglês | MEDLINE | ID: mdl-38937515

RESUMO

The combustion of hydrogen and carbon-monoxide mixtures, so-called syngas, plays an increasingly important role in the safety context of non-fossil energy generation, more specifically in the risk management of incidents in process engineering plants for ammonia synthesis and in nuclear power plants. In order to characterize and simulate syngas/air combustion on industrially relevant scales, subgrid modelling is required, which is often based on a reaction progress variable. To understand the influence of different fuel compositions, turbulence intensities and flame topologies on different possible definitions of reaction progress variable, detailed chemistry direct numerical simulations data of premixed, lean hydrogen/air and syngas/air flames has been considered. A reaction progress variable based on normalized molecular oxygen mass fraction has been found not to capture the augmentation of the normalized burning rate per unit flame surface area in comparison to the corresponding 1D unstretched premixed flame due to preferential diffusion effects. By contrast, reaction progress variables based on other individual species, such as hydrogen, can capture the augmentation of the rate of burning well, but exhibit a pronounced sensitivity to preferential diffusion effects, especially in response to flame curvatures. However, a reaction progress variable based on the linear combination of the main products can accurately represent the temperature evolution of the flame for different mixtures, turbulence intensities and varying local flame topology, while effectively capturing the augmentation of burning rate due to preferential diffusion effects. However, its tendency to assume values larger than 1.0 in the regions of super-adiabatic temperatures poses challenges for future modeling approaches, whereas the reaction progress variable based on hydrogen mass fraction remains bound between 0.0 and 1.0 despite showing deviations in comparison to corresponding variations obtained from the unstretched laminar flame depending on flame curvature variations.

3.
BMC Chem ; 17(1): 118, 2023 Sep 20.
Artigo em Inglês | MEDLINE | ID: mdl-37730608

RESUMO

Biofuels are renewable alternatives to fossil fuels. Levopimaric acid‒base biofuels have attracted increasing attention. However, their stability remains a critical issue in practice. Thus, there is a strong impetus to evaluate the thermal stability of levopimaric acid. Through thermogravimetry (TG) and a custom-designed mini closed pressure vessel test (MCPVT) operating under isothermal and stepped temperature conditions, we investigated thermal oxidation characteristics of levopimaric acid under oxygen atmosphere. Thin-layer chromatography (TLC) and iodimetry were used to measure the hydrogen peroxides generated by levopimaric acid oxidation. A high pressure differential scanning calorimeter (HPDSC) was used to assess hydroperoxide thermal decomposition characteristics. Gas chromatography-mass spectrometry (GC-MS) was used to characterize the oxidation products. The thermal decomposition kinetics of levopimaric acid were thus elucidated, and a high peroxide value was detected in the levopimaric acid. The decomposition heat (QDSC) and exothermic onset temperature (Tonset) of hydroperoxides were 338.75 J g-1 and 375.37 K, respectively. Finally, levopimaric acid underwent a second-stage oxidation process at its melt point (423.15 K), resulting in complex oxidation products. Thermal oxidation of levopimaric acid could yield potential thermal hazards, indicating that antioxidants must be added during levopimaric acid application to protect against such hazardous effects.

4.
ACS Catal ; 12(10): 5961-5969, 2022 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-37727697

RESUMO

The mechanism of asymmetric hydrogenation of 2-pyridyl alkenes catalyzed by chiral Rh-phosphine complexes at ambient temperature is examined using kinetic, spectroscopic, and computational tools. The reaction proceeds with reversible substrate binding followed by rate-determining addition of hydrogen. Substrate binding occurs only through the pyridine nitrogen in contrast to other substrate classes exhibiting stronger substrate direction. The lack of influence of hydrogen pressure on the product enantiomeric excess suggests that a pre-equilibrium in substrate binding is maintained across the pressure range investigated. An off-cycle Rh-hydride species is implicated in the mild catalyst deactivation observed. In contrast to Ru-phosphine-catalyzed reactions of the same substrate class, the stereochemical outcome in this system correlates generally with the relative stability of the E and Z rotamers of the substrate.

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