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首页> 外文期刊>Environmental Science & Technology >Uranyl Adsorption onto Hydrous Ferric Oxide-A Re-Evaluation for the Diffuse Layer Model Database
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Uranyl Adsorption onto Hydrous Ferric Oxide-A Re-Evaluation for the Diffuse Layer Model Database

机译：铀酰在含水三氧化二铁上的吸附-扩散层模型数据库的重新评估

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摘要

The diffuse layer model (DLM) database of Dzombak and Morel was developed to quantify the adsorption of dissolved species onto the hydrous ferric oxide (HFO) surface, and contained numerous surface complexation reactions, including surface complexation reactions for uranyl (UO_2~(+2)) consisting of Hfo_sOUO_2~+ and Hfo_wOUO_2~+. However, these constants were not based upon experimentally obtained data, but rather were derived from linear free energy relationships (LFER) using log K_(MOH) values. When compared to experimental data, the LFER-derived constants for uranyl were shown to overestimate adsorption by a factor of 10 in some cases. At least 14 uranyl HFO data sets have been previously published and were used to re-estimate constants by coupling the geochemical computer code PHREEQC with UCODE_2005, an automated parameter optimization program. Five uranyl-bearing surface complexation reactions were initially evaluated;the constants were optimized by allowing UCODE to incrementally vary selected log K_x~(im) values until the best fit to the experimental data was obtained. Assumptions consistent with the original DLM were retained. Changes to the K_1~(int) and K_2~(int) constants, and addition of uranyl monocarbonate and uranyl dicarbonate surface complexes, will update and correct the uranyl sorption reactions in thiswidely used database.
机译：建立Dzombak和Morel的扩散层模型（DLM）数据库以量化溶解的物质在含水三氧化二铁（HFO）表面上的吸附，并包含许多表面络合反应，包括铀酰（UO_2〜（+2 ））由Hfo_sOUO_2〜+和Hfo_wOUO_2〜+组成。但是，这些常数不是基于实验获得的数据，而是使用log K_（MOH）值从线性自由能关系（LFER）导出的。与实验数据相比，在某些情况下，铀酰的LFER衍生常数被高估了10倍。至少已经发布了14个铀酰HFO数据集，并通过将地球化学计算机代码PHREEQC与自动参数优化程序UCODE_2005耦合来重新估计常数。最初评估了五个带有铀酰的表面络合反应；通过允许UCODE逐步改变所选log K_x〜（im）值来优化常数，直到获得最适合实验数据的值。保留与原始DLM一致的假设。更改K_1〜（int）和K_2〜（int）常数，并添加铀酰单碳酸酯和铀酰二碳酸酯表面配合物，将更新和校正此广泛使用的数据库中的铀酰吸附反应。

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  • 来源
    《Environmental Science & Technology》 |2009年第24期|9260-9266|共7页
  • 作者

    JOHN I. MAHONEY; SONYA A. CABLE; AND RYAN T. JAKUBOWSKI;

  • 作者单位

    Mahoney Geochemical Consulting LLC, Lakewood, Colorado 80226;

    GeoTrans, Inc., Louisville, Colorado 80027;

    MWH Americas, Inc. Steamboat Springs, Colorado 80487;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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  • 正文语种 eng
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