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1.
Org Process Res Dev ; 28(4): 891-923, 2024 Apr 19.
Article in English | MEDLINE | ID: mdl-38660379

ABSTRACT

Separation and purification in organic solvents are indispensable procedures in pharmaceutical manufacturing. However, they still heavily rely on the conventional separation technologies of distillation and chromatography, resulting in high energy and massive solvent consumption. As an alternative, organic solvent nanofiltration (OSN) offers the benefits of low energy consumption, low solid waste generation, and easy scale-up and incorporation into continuous processes. Thus, there is a growing interest in employing membrane technology in the pharmaceutical area to improve process sustainability and energy efficiency. This Review comprehensively summarizes the recent progress (especially the last 10 years) of organic solvent nanofiltration and its applications in the pharmaceutical industry, including the concentration and purification of active pharmaceutical ingredients, homogeneous catalyst recovery, solvent exchange and recovery, and OSN-assisted peptide/oligonucleotide synthesis. Furthermore, the challenges and future perspectives of membrane technology in pharmaceutical applications are discussed in detail.

2.
Langmuir ; 38(42): 12859-12870, 2022 Oct 25.
Article in English | MEDLINE | ID: mdl-36221959

ABSTRACT

A two-step seeded-growth method was refined to synthesize Au@Pd core@shell nanoparticles with thin Pd shells, which were then deposited onto alumina to obtain a supported Au@Pd/Al2O3 catalyst active for prototypical CO oxidation. By the strict control of temperature and Pd/Au molar ratio and the use of l-ascorbic acid for making both Au cores and Pd shells, a 1.5 nm Pd layer is formed around the Au core, as evidenced by transmission electron microscopy and energy-dispersive spectroscopy. The core@shell structure and the Pd shell remain intact upon deposition onto alumina and after being used for CO oxidation, as revealed by additional X-ray diffraction and X-ray photoemission spectroscopy before and after the reaction. The Pd shell surface was characterized with in situ infrared (IR) spectroscopy using CO as a chemical probe during CO adsorption-desorption. The IR bands for CO ad-species on the Pd shell suggest that the shell exposes mostly low-index surfaces, likely Pd(111) as the majority facet. Generally, the IR bands are blue-shifted as compared to conventional Pd/alumina catalysts, which may be due to the different support materials for Pd, Au versus Al2O3, and/or less strain of the Pd shell. Frequencies obtained from density functional calculations suggest the latter to be significant. Further, the catalytic CO oxidation ignition-extinction processes were followed by in situ IR, which shows the common CO poisoning and kinetic behavior associated with competitive adsorption of CO and O2 that is typically observed for noble metal catalysts.

3.
J Hazard Mater ; 432: 128723, 2022 06 15.
Article in English | MEDLINE | ID: mdl-35316632

ABSTRACT

Removing and recovering uranium (U) from U-mining wastewater would be appealing, which simultaneously reduces the adverse environmental impact of U mining activities and mitigates the depletion of conventional U resources. In this study, we demonstrate the application of a constant-voltage electrochemical (CVE) method for the removal and recovery of U from U-mining wastewater, in an ambient atmosphere. The effects of operation conditions were elucidated in synthetic U-bearing water experiments, and the cell voltage and the ionic strength were found to play important roles in both the U extraction kinetics and the operation cost. The mechanistic studies show that, in synthetic U-bearing water, the CVE U extraction proceeds exclusively via a single-step one-electron reduction mechanism, where pentavalent U is the end product. In real U-mining wastewater, the interference of water matrices led to the disproportionation of the pentavalent U, resulting in the formation of tetravalent and hexavalent U in the extraction products. The U extraction efficacy of the CVE method was evaluated in real U-mining wastewater, and results show that the CVE U extraction method can be efficient with operation costs ranging from $0.55/kgU ~ $64.65/kgU, with varying cell voltages from 1.0 V to 4.0 V, implying its feasibility from the economic perspective.


Subject(s)
Uranium , Water Pollutants, Radioactive , Mining , Wastewater , Water , Water Pollutants, Radioactive/analysis
4.
iScience ; 24(11): 103230, 2021 Nov 19.
Article in English | MEDLINE | ID: mdl-34712926

ABSTRACT

Current photocatalytic uranium (U) extraction methods have intrinsic obstacles, such as the recombination of charge carriers, and the deactivation of catalysts by extracted U. Here we show that, by applying a bias potential on the photocatalyst, the photoelectrochemical (PEC) method can address these limitations. We demonstrate that, owing to efficient spatial charge-carriers separation driven by the applied bias, the PEC method enables efficient and durable U extraction. The effects of multiple operation conditions are investigated. The U extraction proceeds via single-step one-electron reduction, resulting in the formation of pentavalent U, which can facilitate future studies on this often-overlooked U species. In real seepage water the PEC method achieves an extraction capacity of 0.67 gU m-3·h-1 without deactivation for 156 h continuous operation, which is 17 times faster than the photocatalytic method. This work provides an alternative tool for U resource recovery and facilitates future studies on U(V) chemistry.

5.
Water Res ; 186: 116327, 2020 Nov 01.
Article in English | MEDLINE | ID: mdl-32846377

ABSTRACT

The presence of contaminants of emerging concern (CECs) in various water bodies and the associated threats to eco-system and human society have raised increasing concerns. To fight against such a problem, TiO2 photocatalysis is considered to be a powerful tool. In recent decades, TiO2 nanotube array (TNA) fabricated by electrochemical anodization emerged as a viable immobilized catalyst and its applications on CECs removal have gained a considerable amount of research interest. We herein present a critical review on the development of TNA and its applications on the removal of aqueous CECs. In this work, the CECs removal in different TNA based processes, the CECs removal mechanisms, the role of TNA properties, the role of operational parameters, and the role of water matrices are discussed. Moreover, perspectives on the current research progress are presented and recommendations on future research are elaborated.


Subject(s)
Nanotubes , Catalysis , Humans , Titanium , Wastewater
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