Tinnacher Ruth M, Honeyman Bruce D
Environmental Science and Engineering Division, Colorado School of Mines, Golden, Colorado 80401, USA.
Environ Sci Technol. 2007 Oct 1;41(19):6776-82. doi: 10.1021/es070563b.
In this paper, we describe a new method for labeling NOM with the radioisotope tritium (3H) using fulvic acid (FA) as the target NOM fraction. During labeling, FA ketone groups are chemically reduced with tritiated sodium borohydride (NaBH4), while the chemical functionality of the carboxyl and phenol groups is preserved. The labeling procedure was optimized in efficiency experiments that determined the excess concentration of tritiated NaBH4 required for optimum reduction conditions. The chemical characterization of the labeled FA product using FTIR and 1H NMR spectral analysis confirms the proposed reaction mechanism and rules out any significant amounts of impurities or undesirable side reactions. Results from size exclusion chromatography indicate thatthe tritium label is distributed uniformly over the whole molecular size range of FA and that it is stable over time and under various pH conditions. Potential differences in FA sorption behavior onto mineral surfaces due to labeling were excluded based on experimental data. This method produces NOM of high specific activity (e.g., 1.9 mCi mg(-1) FA); this permits the tracing of FA at a detection limit of 0.3 microg L(-1) FA.
在本文中,我们描述了一种以富里酸(FA)作为目标天然有机物组分,用放射性同位素氚(³H)标记天然有机物的新方法。在标记过程中,富里酸的酮基用氚化硼氢化钠(NaBH₄)进行化学还原,而羧基和酚基的化学官能团得以保留。在效率实验中对标记程序进行了优化,该实验确定了最佳还原条件所需的氚化硼氢化钠的过量浓度。使用傅里叶变换红外光谱(FTIR)和¹H核磁共振光谱分析对标记的富里酸产物进行化学表征,证实了所提出的反应机理,并排除了任何大量杂质或不良副反应。尺寸排阻色谱法的结果表明,氚标记均匀分布在富里酸的整个分子大小范围内,并且在不同时间和各种pH条件下都很稳定。基于实验数据排除了由于标记导致的富里酸在矿物表面吸附行为的潜在差异。该方法产生高比活度的天然有机物(例如,1.9 mCi mg⁻¹ FA);这使得能够在0.3 μg L⁻¹ FA的检测限下追踪富里酸。