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[Display omitted] • Proposed a strategy for developing a low-temperature oil-in-water demulsifier. • Increasing the aromaticity and polarity could enhance the effectiveness and rate of demulsifiers. • The role of structure and interfacial activity in demulsifiers has been discussed. • Poly (amino acids) demulsifier performs well in terms of efficiency and rate at room temperatures. To improve the universality and efficiency of polymer demulsifiers at low temperatures, a unique type of biodegradable poly (ε-carbobenzyloxy-L-lysine) - block -poly (L-phenylalanine) (PZLL- b -PPA) demulsifier with stronger polarity and higher aromaticity was developed. The molecular structure and weight of PZLL- b -PPA were determined using Fourier transform infrared (FT-IR) spectroscopy, 1H nuclear magnetic resonance hydrogen spectra (NMR) and gel permeation chromatography (GPC). A bottle test was used to evaluate the demulsification performance of PZLL- b -PPA with different block ratios, structure and interfacial activity. Numerous critical variables, such as demulsifier structure and dosage, pH levels, emulsion salinity, oil content and oil type, were carefully examined. The demulsification results showed that PZLL 5 - b -PPA 25 has excellent low-temperature demulsification capability and can effectively separate oil from water emulsions with different pH values (4.0 ∼ 11.0) and oil contents ranging from 1.0 ∼ 20.0 wt% within 2 min at room temperature. The best demulsification efficiency reached 99.98 %, with only 6.0 mg/L of residual oil in the separated water. The analysis of interfacial self-assembly behavior revealed that PZLL- b -PPA has a strong affinity for aromatic molecules and exhibits high interfacial activity. The quantum chemical calculation indicated that the main chain polyamide skeleton of PZLL- b -PPA has a stronger interaction for asphaltene, resin and naphthenic acid molecules than conventional oxygen-containing skeleton polymers. Furthermore, the microscopy analysis indicated that PZLL- b -PPA has excellent capacity for flocculation and coalescence of oil droplets in an O/W emulsion. As a result, when PZLL- b -PPA is added to the emulsion, it can quickly migrate to the oil-water interface and interact with and displace the emulsion's stabilizers (asphaltenes and resins), promoting oil droplet coalescence and separation from water at low temperature. [ABSTRACT FROM AUTHOR]

• Co-, Ni-, and Ru-based catalysts show good primary amine selectivity. • The competitive adsorption of FAM and H 2 suppresses its excessive hydrogenation. • The adsorption energies of FAM on Co, Ni, and Ru surfaces are calculated. • The activation energy is not the key factor in determining the FAM hydrogenation. In addition to the main reaction, understanding the structure-activity relationship in the side reactions is another important goal for catalysis science. In this work, the catalytic activities and selectivities of various active metals were studied in the reductive amination of furfural (FAL). Compared with Co- and Ni-based catalysts, the excessive hydrogen of furfurylamine (FAM) was found over Ru-based catalysts at much higher reaction temperature (130 vs. 50 °C). Moreover, the evaluation of FAM hydrogenation undoubtedly substantiated the intimate relationship between H 2 reaction pressure and catalytic activity. Combining the theoretical and experimental results, it is clearly verified that the active metal determines the excessive hydrogen of FAM by affecting the competitive adsorption of FAM and H on the active sites. [Display omitted] [ABSTRACT FROM AUTHOR]

Graphene oxide (GO) nanosheets have been experimentally proved to be a highly efficiency, rapid and universal demulsifier to break up the crude oil-in-water emulsion and/or the emulsified oily waste water in our previous study. To recycle the GO nanosheets and avoid the possible contamination of GO for crude oil, in this work, the magnetic graphene oxide (M-GO) was successfully synthesized and used for separating oil/water emulsions. Demulsification tests indicated that M-GO could separate the oil/water emulsions within a few minutes and recycle 6–7 times without losing its demulsification capability. The residual oil content in the separated water was as low as ∼10 mg/L, corresponding to a demulsification efficiency of 99.98% at an optimal dosage. Quantum chemical calculation results indicated that the π-π/σ-π interactions between GO materials and asphaltene molecules are the major driven forces for the high demulsification performance of M-GO nanosheets. This work not only provides a promising demulsifies to demulsify the crude oil-in-water emulsion or the oily wastewater but also give a deep understanding on the intrinsic interaction between demulsifiers and asphaltenes. [ABSTRACT FROM AUTHOR]

Amphiphilic aromatic poly (amino acids) polymers were designed as biodegradability demulsifiers with higher aromaticity, stronger polarity, and side chain-like combs. The effects of demulsifier dosage, structural characteristics and emulsion properties such as pH, salinity, and oil content on the demulsification efficiency were investigated. The results show that the poly (L-glutamic-benzyl ester)-block-poly (L-phenylalanine) (PBLG 15 - b -PPA 15) as the demulsifier can remove more than 99.97% of the oil in a 5.0 wt% oil-in-water (O/W) emulsion at room temperature within 2 min. The poly (L-tyrosine)-block-poly (L-phenylalanine) (PTyr 15 - b -PPA 15) with environmental durability demonstrates high effectiveness, universality, and demulsification speed. It achieves a remarkable demulsification efficiency of up to 99.99% for a 20.0 wt% O/W emulsion at room temperature. The demulsification mechanism indicates that demulsifiers have sufficient interfacial activity can quickly migrate to the oil-water interface after being added to the emulsions. Additionally, when demulsifiers are present in a continuous phase in the molecular form, their "teeth" side chains are beneficial for increasing coalescence and flocculation capacities. Furthermore, according to the Density Functional Theory (DFT) calculations, enhancing the intermolecular interactions between demulsifiers and the primary native surfactants that form an oil-water interfacial film is a more efficient approach to reducing demulsification temperature and improving demulsification efficiency and rate. [Display omitted] • Proposed a strategy for developing a low-temperature oil-in-water demulsifier. • Improving the polarity and aromaticity of demulsifiers enhances their performance. • Aromatic poly (amino acids) demulsifiers perform well at low temperatures. • The intermolecular interactions determine the deoiling temperature and efficiency. [ABSTRACT FROM AUTHOR]

The integrated synergistic effect of the ligand and the strong metal-support interaction (SMSI) effectively improves the selectivity and stability of heterogeneous Pd-based catalysts for acetylene dicarbonylation under high-pressure CO conditions. [Display omitted] • Stabilizing the catalytic active site Pdδ+ for acetylene dialkoxycarbonylation. • Oxygen-containing functional groups of AC provide anchoring sites for stabilize active Pd2+ ions. • The coordination of I- not only accelerates the reaction but also stabilizes the catalyst. The support and ligand play a crucial role in regulating the catalytic performance, selectivity, and stability of heterogeneous catalysis. Herein, activated carbon (AC) supported palladium (Pd) catalysts (2.0 wt%) were prepared by impregnation for acetylene dicarbonylation. The oxygen-containing groups on the surface of the AC support were modulated by nitric acid (HNO 3) to investigate metal–support interactions on the catalytic performance and stability of the Pd/AC. The characterization of the chemical composition and structure of the supports and catalysts demonstrates that high concentrations of oxygen-containing groups on the surface of the carbon support lead to the fine dispersion of Pd nanoparticles. Notably, the finely dispersed Pd/AC 70 catalyst exhibited good activity and stability for acetylene dicarbonylation under high-pressure CO conditions after several rounds of regeneration. Furthermore, operational parameters including the type of support, co-catalyst (KI), and reaction time and temperature were identified for their impact on the reaction. It was found that I- anions serve as a co-catalyst and can ligate with Pd species, thereby preventing the leaching of Pd and improving reaction selectivity. This study presents a straightforward and sustainable modulation strategy to improve the dispersion of active metals, as well as to prevent the leaching and sintering of these metals during high-pressure CO reactions. [ABSTRACT FROM AUTHOR]