PubMed · 11013714
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Y Tong, E Oldfield, A Wieckowski. 1998-08-01. Exploring electrochemical interfaces with solid-state NMR.. https://doi.org/10.1021/ac981932c
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The contamination of water resources by uranyl (UO22+) ions poses significant environmental and health risks, requiring the development of efficient and sustainable remediation strategies. Adsorption-based techniques have emerged as promising approaches in the field of UO22+ removal, but the design of cost-effective, high-capacity, and environmentally friendly adsorbents remains challenging. In this study, a three-dimensional porous nano-hydroxyapatite@gelatin (nHAP@Ge) composite was synthesized through glutaraldehyde cross-linking, combining the structural stability of Ge with the high uranium affinity of nHAP. The optimized nHAP@Ge, with a nHAP:Ge mass ratio of 1:0.5, exhibited exceptional UO22+ removal efficiency (97 %), along with high adsorption capacity (364.03 mg/g). Systematic characterizations using scanning electron microscopy (SEM), thermogravimetric analysis (TGA), Fourier transform infrared (FT-IR) spectroscopy, and X-ray photoelectron spectroscopy (XPS) methods revealed that the porous structure and surface functional groups (-OH, Ca2+, and PO43-) of the material synergistically contributed to binding UO22+ species. Furthermore, the incorporation of nHAP into the Ge framework resulted in enhanced thermal stability while significantly improving the UO22+ adsorption performance. This work presents a scalable, eco-friendly, and recyclable strategy for the effective treatment of uranium-contaminated water, with potential applications in nuclear wastewater treatment and environmental remediation.
A kinetic framework is developed to describe enzyme activity and stability in two-phase liquid-liquid systems. In particular, the model is applied to the enzymatic production of benzaldehyde from mandelonitrile by Prunus amygdalus hydroxynitrile lyase (pa-Hnl) adsorbed at the diisopropyl ether (DIPE)/aqueous buffer interface (pH = 5.5). We quantitatively describe our previously obtained experimental kinetic results (Hickel et al., 1999; 2001), and we successfully account for the aqueous-phase enzyme concentration dependence of product formation rates and the observed reaction rates at early times. Multilayer growth explains the early time reversibility of enzyme adsorption at the DIPE/buffer interface observed by both enzyme-activity and dynamic-interfacial-tension washout experiments that replace the aqueous enzyme solution with a buffer solution. The postulated explanation for the unusual stability of pa-Hnl adsorbed at the DIPE/buffer interface is attributed to a two-layer adsorption mechanism. In the first layer, slow conformational change from the native state leads to irreversible attachment and partial loss of catalytic activity. In the second layer, pa-Hnl is reversibly adsorbed without loss in catalytic activity. The measured catalytic activity is the combined effect of the deactivation kinetics of the first layer and of the adsorption kinetics of each layer. For the specific case of pa-Hnl adsorbed at the DIPE/buffer interface, this combined effect is nearly constant for several hours resulting in no apparent loss of catalytic activity. Our proposed kinetic model can be extended to other interfacially active enzymes and other organic solvents. Finally, we indicate how interfacial-tension lag times provide a powerful tool for rational solvent selection and enzyme engineering.
During the many years of paraquat usage, wide ranges of investigations of its environmental impact have been conducted. Much of this information has been published, but key, long-term field studies have not previously been presented and assessed. The purpose of this review is to bring together and appraise this information. Due to the nature of paraquat residues in soils, the major part (some 99.99%) of a paraquat application that reaches the soil within the typical Good Agricultural Practice (GAP) is strongly adsorbed to soils of a wide variety of textures. This is in equilibrium with an extremely low concentration in soil solution. However, the paraquat in soil solution is intrinsically biodegradable, being rapidly and completely mineralized by soil microorganisms. The deactivation of the biological activity of paraquat in soils, due to sorption, has been investigated thoroughly and systematically. It is recognized that the determination of total soil residues by severe extraction procedures provides no insight into the amount of paraquat biologically available in soil. Consequently, the key assay developed for this purpose, namely, the strong adsorption capacity-wheat bioassay (SAC-WB) method, has proved to be valuable for determination of the adsorption capacity relevant to paraquat for any particular soil. This method has been validated in the field with a series of long-term (>10 years) trials in different regions of the world. These trials have also shown that, following repeated applications of very high levels of paraquat in the field, residues not only reach a plateau but also subsequently decline. This demonstrates that the known biodegradation of paraquat in soil pore water plays an important role in field dissipation. The biological effects of paraquat in the field have been assessed under unrealistically high treatment regimes. These trials have demonstrated that the continued use of paraquat under GAP conditions will have no detrimental effects on either crops or soil-dwelling flora and fauna. Any such effects can occur only under extreme use conditions (above the SAC-WB), which do not arise in normal agricultural practice.