溶解有机质对铁(II)的配合作用和氧化还原缓冲作用。

Complexation and Redox Buffering of Iron(II) by Dissolved Organic Matter.

机构信息

Department of Chemistry, Colorado State University , 1170 Campus Delivery, Fort Collins, Colorado 80523, United States.

Energy Geoscience Division, Lawrence Berkeley National Laboratory , Berkeley, California 94720, United States.

出版信息

Environ Sci Technol. 2017 Oct 3;51(19):11096-11104. doi: 10.1021/acs.est.7b03152. Epub 2017 Sep 18.

Abstract

Iron (Fe) bioavailability depends upon its solubility and oxidation state, which are strongly influenced by complexation with natural organic matter (NOM). Despite observations of Fe(II)-NOM associations under conditions favorable for Fe oxidation, the molecular mechanisms by which NOM influences Fe(II) oxidation remain poorly understood. In this study, we used X-ray absorption spectroscopy to determine the coordination environment of Fe(II) associated with NOM (as-received and chemically reduced) at pH 7, and investigated the effect of NOM complexation on Fe(II) redox stability. Linear combination fitting of extended X-ray absorption fine structure (EXAFS) data using reference organic ligands demonstrated that Fe(II) was complexed primarily by carboxyl functional groups in reduced NOM. Functional groups more likely to preserve Fe(II) represent much smaller fractions of NOM-bound Fe(II). Fe(II) added to anoxic solutions of as-received NOM oxidized to Fe(III) and remained organically complexed. Iron oxidation experiments revealed that the presence of reduced NOM limited Fe(II) oxidation, with over 50% of initial Fe(II) remaining after 4 h. These results suggest reduced NOM may preserve Fe(II) by functioning both as redox buffer and complexant, which may help explain the presence of Fe(II) in oxic circumneutral waters.

摘要

铁(Fe)的生物利用度取决于其溶解度和氧化态,而这两者又强烈受到与天然有机物(NOM)络合的影响。尽管在有利于 Fe 氧化的条件下观察到 Fe(II)-NOM 结合,但 NOM 影响 Fe(II)氧化的分子机制仍知之甚少。在这项研究中,我们使用 X 射线吸收光谱在 pH 7 下确定与 NOM(原样和化学还原)结合的 Fe(II)的配位环境,并研究了 NOM 络合对 Fe(II)氧化还原稳定性的影响。使用参考有机配体对扩展 X 射线吸收精细结构(EXAFS)数据进行线性组合拟合表明,Fe(II)主要与还原 NOM 中的羧基官能团络合。更有可能保留 Fe(II)的官能团代表 NOM 结合的 Fe(II)的更小分数。Fe(II)添加到原样 NOM 的缺氧溶液中被氧化为 Fe(III)并仍然与有机物络合。铁氧化实验表明,还原 NOM 的存在限制了 Fe(II)的氧化,4 小时后仍有超过 50%的初始 Fe(II)存在。这些结果表明,还原 NOM 可以通过充当氧化还原缓冲剂和络合剂来保存 Fe(II),这可能有助于解释氧化中性水中存在 Fe(II)的原因。

文献AI研究员

20分钟写一篇综述,助力文献阅读效率提升50倍

立即体验

用中文搜PubMed

大模型驱动的PubMed中文搜索引擎

马上搜索