甘酸盐结合和物种化在水-甲基石界面:与红外光谱学和MO/DFT相一致的表面复合模型
Bram Geysels1, Tjisse Hiemstra2, Jan E Groenenberg2
1Soil Chemistry and Chemical Soil Quality Group, Wageningen University & Research, PO BOX 47, Wageningen 6700 AA, the Netherlands; INVITE GmbH, Otto-Bayer-Straße 32, D-51061 Cologne, Germany.
Water research
|December 31, 2024
概括
甘酸盐 (PMG) 与石结合涉及单酸盐和双酸盐复合体,这对于了解其环境命运和优化废水排放至关重要. 这项研究量化了PMG在金属氧化物上的吸附机制.
科学领域:
- 环境化学环境化学
- 表面科学是一门学科.
- 计算化学计算化学
背景情况:
- 草甘 (PMG) 与金属 (水氧化物) 的结合影响了其在环境中的可用性和流动性.
- 了解PMG吸附机制对于预测其在水上和陆地系统中的命运以及废水处理至关重要.
- 目前缺乏对金属氧化物PMG吸附和表面物种化的定量描述.
研究的目的:
- 提供关于草甘 (PMG) 吸附和围 (FeOOH) 表面物种化的机制和定量见解.
- 开发一个由MO/DFT计算支持的高级表面复杂化模型.
- 改善PMG命运和运输的预测,并优化其通过金属 (水氧化物) 的去除.
主要方法:
- 在广泛的pH值,溶液度和表面负荷范围内进行了吸附实验.
- 使用电荷分布方法使用先进的表面复杂化建模.
- 分子轨道/密度功能理论 (MO/DFT) 的计算用于确定复杂的几何,热化学和红外光谱.
主要成果:
- 机械建模揭示了单牙和双牙PMG复合体的形成,每个复合体都有两个质子状态.
- 吸附主要 (>60%) 由双酸复合体驱动,质子化/脱质子化取决于pH值和负荷.
- 单酸复合物不那么普遍,酸组在低pH和高负荷下产生质子.
结论:
- 这项研究提供了对PMG与石结合的新机制和定量理解.
- 开发的模型准确地预测了PMG溶液度及其pH依赖性.
- 这些发现使PMG命运和运输的预测得到了改进,并为优化使用金属 (水氧化物) 的去除提供了一个框架.
相关概念视频
Complexometric Titration: Ligands
897
Different monodentate and polydentate ligands are used as complexing agents in complexometric titration reactions. The formation of complexes by mono- and bidentate ligands involves two or more intermediate steps, limiting their use as complexing agents. In comparison, polydentate ligands can form complexes with metal ions in a single-step process, facilitating sharper end points. This means polydentate ligands, such as amino carboxylic acid derivatives, are most commonly employed in...
897
Complexation Equilibria: The Chelate Effect
435
In complexation reactions, metal atoms or cations interact with ligands to form donor-acceptor adducts called metal complexes. Ligands that bind through one donor site are monodentate, ligands with two donor sites are bidentate, and those with more than two donor sites are polydentate ligands. For example, ethylene diamine is a bidentate ligand that binds through two nitrogen donor atoms, forming a five-membered ring. EDTA is a polydentate ligand that binds through four oxygen and two nitrogen...
435
Factors Affecting Solubility
33.0K
Compared with pure water, the solubility of an ionic compound is less in aqueous solutions containing a common ion (one also produced by dissolution of the ionic compound). This is an example of a phenomenon known as the common ion effect, which is a consequence of the law of mass action that may be explained using Le Chȃtelier’s principle. Consider the dissolution of silver iodide:
33.0K
Ligand Binding and Linkage
4.8K
Allosteric proteins have more than one ligand binding site; the binding of a ligand to any of these sites influences the binding of ligands to the other sites. When a protein is allosteric, its binding sites are called coupled or linked. In the case of enzymes, the site that binds to the substrate is known as the active site and the other site is known as the regulatory site. When a ligand binds to the regulatory site, this leads to conformational changes in the protein that can influence...
4.8K
Extraction: Advanced Methods
409
Metal ions can be separated from one another by complexation with organic ligands–the chelating agent– to form uncharged chelates. Here, the chelating agent must contain hydrophobic groups and behave as a weak acid, losing a proton to bind with the metal. Since most organic ligands used in this process are insoluble or undergo oxidation in the aqueous phase, the chelating agent is initially added to the organic phase and extracted into the aqueous phase. The metal-ligand complex is...
409
Complexation Equilibria: Overview
614
Complexation reactions take place when dative or coordinate covalent bonds form between metal ions and ligands. The compounds formed in these reactions are called coordination compounds. The number of bonds formed between the metal ion and the ligands is called its coordination number. Generally, most metal ions in an aqueous solution are solvated by water molecules and thus exist as aqua complexes.
The equilibrium constant of the complexation reaction is represented as the formation constant...
The equilibrium constant of the complexation reaction is represented as the formation constant...
614


