Green Chemical Engineering最新文献

The development of green route for preparing propylene oxide (PO) with molecular oxygen is of significance both in academic and industrial. In this work, propylene epoxidation coupled with furfural oxidation catalyzed by platinum meso-tetraphenylporphyrin (Pt (II)TPP) has been developed. Propylene conversion and PO selectivity reached up to 56% and 83%, respectively. Meanwhile, furfural was almost completely converted to furoic acid. Based on operando characterizations and electron paramagnetic resonance (EPR) tests, a mechanism involved high-valent Pt species was proposed. This work is expected to provide a potential application prospects for producing PO and furoic acid simultaneously in chemical industry.

To overcome the limitations of geography, climate, and ore characteristics on the ore beneficiation process, bio-oxidation studies on low-grade arsenic-bearing refractory gold ore by pool leaching were carried out, as well as process fitting analysis. The gold particles are encapsulated by pyrite and arsenopyrite. After 60 days of bio-oxidation, the oxidation rates of arsenic, sulfur, and gold were 39%∼69%, 24%∼41%, and 49%∼83%, respectively. The inoculated Acidithiobacillus ferrooxidans, Ferroplasma acidiphilum, and Leptospirillum ferrodiazotrophum could all mediate the initial pyrite/arsenopyrite oxidation and the Fe²⁺ oxidation reaction, but only the former could mediate the subsequent sulfur compound oxidation. When compared to daily bacterial circulation and bacterial replacement every ten days, aeration improved the gold leaching rate by 14%∼22%. The Boltzmann model could fit both the arsenic and sulfur bio-oxidation, with model fit variances greater than 0.98. Based on the experimental and fitting results, the bio-oxidation cycle was determined to be 60 days, and the bio-oxidation mechanisms are summarized. This study has significant practical implications for the rational utilization of gold resources and provides theoretical and practical guidance for similar gold ores.

The separation of He/H₂ using membrane technology has gained significant interest in the field of He extraction from natural gas. One of the greatest challenges associated with this process is the extremely close kinetic diameters of the two gas molecules, resulting in low membrane selectivity. In this study, we investigated the structure-performance relationship of metal-organic framework (MOF) membranes for He/H₂ separation through molecular simulations and machine learning approaches. By conducting molecular simulations, we identified the potential MOF membranes with high separation performance from the Computation-Ready Experimental (CoRE) MOF database, and the diffusion-dominated mechanism was further elucidated. Moreover, random forest (RF)-based machine learning models were established to identify the crucial factors influencing the He/H₂ separation performance of MOF membranes. The pore limiting diameter (PLD) and void fraction (φ), are revealed as the most important physical features for determining the membrane selectivity and He permeability, respectively. Additionally, density functional theory (DFT) calculations were carried out to validate the molecular simulation results and suggested that the electronegative atoms on the pore surfaces can enhance the diffusion-based separation of He/H₂, which is critical for improving the membrane selectivities of He/H₂. This study offers useful insights for designing and developing novel MOF membranes for the separation of He/H₂ at the molecular level.

Organic dye pollutants present in wastewater pose a significant global challenge. Among pollutants, the synthetic dye Rhodamine B (RB) stands out due to its non-biodegradable nature and associated neurotoxic, carcinogenic, and respiratory irritant properties. Extensive research has been conducted on the efficacy of adsorption and photodegradation techniques for the removal of RB from wastewater. While adsorption and advanced oxidation processes (AOPs) have gained considerable attention for their effectiveness in recent years, the underlying behaviors and mechanisms of these technologies remain incompletely understood. Therefore, a comprehensive summary of recent research progress in this domain is imperative to clarify the basics and present the up-to-date achievements.

This review provides an in-depth exploration of the fundamentals, advancements, and future trajectories of RB wastewater treatment technologies, mainly encompassing adsorption and photodegradation. This work starts with a general introduction of outlining the sources, toxicity, and diverse applicable removal strategies. Subsequently, it thoroughly examines crucial techniques within non-photochemical, photochemical, and adsorption technologies, such as UV light assisted AOP, catalyst assisted AOP, ozonation, Fenton system, electrochemical AOP, and adsorption technology. The primary objective is to furnish a broad overview of these techniques, elucidating their effectiveness, limitations, and applicability. Following this, the review encapsulates state-of-the-art computational simulations pertaining to RB adsorption and interactions with clays and other adsorbents. Lastly, it delves into column adsorption of RB dye, and elucidates various influencing factors, including bed height, feed concentration, pollutant (RB) feeding or flow rate, and column regeneration. This panoramic review aims to provide valuable insights into suitable techniques, research gaps, and the applicability of non-photochemical, photochemical, and adsorption technologies in the treatment of wastewater containing RB dye.

Antimicrobial materials are a crucial component in eradicating and managing the spread of infectious diseases. They are expected to act on a broad-spectrum of microbes, including emerging pathogens which could cause the next Disease X. Herein, we reassessed a series of antimicrobial imidazolium polymers on our shelves and uncovered extended functionality through dual modes of action. By redesigning their structures, a truly broad-spectrum antimicrobial material with optimized activity against bacteria (G ​+ve, G -ve) and fungi, as well as enveloped and non-enveloped viruses was developed. We demonstrated that the imidazolium polymer exhibits dual modes of function against microbes: targeting the microbial membrane and binding DNA. The latter DNA binding affinity was found to be key against non-enveloped viruses. With this insight, we designed small molecule compounds that exhibited optimum broad-spectrum antimicrobial activity and excellent efficacy against ESKAPE group of pathogens that are responsible for some of the deadliest nosocomial infections worldwide. Our results could also shed light on the design of broad-spectrum antimicrobial compounds against Disease X.

Research on solvent effects is an important and long-standing topic, but there still is some room, especially for the special solvent effect of fluoroalcohols. In this work, we investigated the stability of phenoxyl radical in monohydric alcohol solvents through in-situ electron paramagnetic resonance detections. The decay behavior of phenoxyl radical showed a reasonable relationship with the mesoscopic structure of alcohols, characterized by small- and wide-angle X-ray scattering. Moreover, the distinct solvent effects of fluoroalcohols were emphasized, and the significant influence of van der Waals distance in the solvents was suggested. Overall, the stability of phenoxyl radical in alcohols was quantified and correlated with the solvent structures. We believe that the established method for stability study on radicals will encourage solvent effect studies on various organic reactions, and the proposed solvent effects in fluoroalcohols may inspire the development of green solvents in both industrial conversions and organic synthesis.

Utilizing ionic liquid (IL)-water mixtures as selective extraction solvents for raw materials from natural sources represents an efficacious approach; however, elucidating the underlying mechanisms inherent in various types of IL-aqueous solutions continues to pose a significant challenge. In this study, molecular dynamics simulations and density functional theory calculations are employed to illuminate the influence of the functional anion within ILs and the water content on the solvation mechanism and phase separation phenomena observed during the extraction of camptothecin (CPT) using aqueous IL solutions. The simulation results show that the anions in ILs preferentially dissolve CPT through hydrogen bonding at low water concentrations. As the water concentration increases, the hydrophobic IL binds more tightly to CPT, enabling the water to self-aggregate. The anions in hydrophilic IL form hydrogen bonds with water instead, further enhancing the dissolution of CPT. This work reveals the mechanism of phase separation and solvation of different types of IL aqueous solutions, which is helpful in developing new drug extraction and purification technologies.

Cooling water systems (CWSs) are extensively utilized in various industries to eliminate the excess heat and converse energy. Studies on CWSs mainly concentrated on finding the optimal cooler network structure. In addition, some works also considered the optimal design under varied operation conditions. However, in these works, once the optimal design of the cooler's network is determined, its arrangement remains fixed and cannot be adapted to accommodate diverse operating conditions. In this work, a flexible topology network concept is proposed to make the adjustment of network structure possible under different operation conditions. The CWS with integrated air cooler and flexible topology network has better overall performance, represented by a mixed integer nonlinear programming (MINLP) model that require advanced tools such as GAMS software. Case studies revealed that the proposed methodology can realize better energy-saving performance, and improve the economic performance under varied operation conditions. The impact of critical flexible nodes on system configuration and economy is achieved by sensitivity analysis.