Adsorption kinetics of platinum group elements onto macromolecular organic matter in seawater
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摘要: 研究了代表性大分子有机化合物(MOCs)以及不同分子量的天然有机质(NDOM)对海水中Pt、Pd、Rh(PGEs)的吸附动力学。所选用的大分子有机质包括腐殖酸、卡拉胶、牛血清白蛋白,其分子量均>10 kDa;海水中天然有机质通过切向超滤方法获得,分为分子量 >1 kDa组分与 > 3 kDa组分两种。在实验时间内,除了>1 kDa的NDOM组分对Pt、腐殖酸对Pd的吸附达到平衡外,其余的吸附都没有达到平衡。对于MOCs,其对PGEs的吸附分为两个阶段:前8 h的快速吸附阶段和8 h后的解吸阶段。PGEs离子在MOCs中的分配系数(log10Kd)随实验时间的变化与其动力学的变化趋势一致。但在NDOM对PGEs的吸附中,其log10Kd变化与动力学变化之间存在明显差异。这表明海水中PGEs离子与NDOM的分配行为可能受到多种有机组分的综合控制。PGEs在>1 kDa的NDOM组分中的吸附量及log10Kd都大于>3 kDa的NDOM组分,表明1-3 kDa的NDOM组分可能对PGEs离子和NDOM之间的相互作用有重要影响。现有的动力学模型都不能很好地模拟PGEs与受试有机质之间的吸附过程,表明海水中MOCs或NDOM的胶体结构和形态可能不均匀,PGEs离子与海水中溶解有机物之间的相互作用是一个复杂的过程。Abstract: Adsorption kinetics of the interaction between Pt, Pd and Rh (defined here as platinum group elements, PGEs) ions and macromolecular organic compounds (MOCs, >10 kDa), including humic acid, carrageenan and bovine serum albumin, and different cutoff fractions of natural organic matter (>1 kDa and >3 kDa) obtained from seawater using centrifugal ultrafiltration devices were investigated. For a given element, all the adsorption kinetics did not reach equilibrium except the interaction between Pt and >1 kDa cutoff, and between Pd and humic acid. For all the tested MOCs, the adsorption kinetics could be divided into two stages, a rapid adsorption process in the first 8 h and the desorption stage after the first 8 h until the equilibrium. The change trend of partition coefficient (log10Kd) values with experiment time was consistent with that of the kinetic curves. However, in the interaction between PGE ions and natural dissolved organic matter (NDOM), an obvious difference in the change trends of log10Kd and kinetic curves was observed. It indicated that the partition behavior of PGE ions interacting with NDOM in seawater was a combined effect of different organic constituents. The adsorption and log10Kd of PGEs in the >1 kDa NDOM fraction were higher and more stable than those in the >3 kDa NDOM fraction. The results also indicated that the 1–3 kDa NDOM may dominate the interaction between PGEs ions and NDOM. Moreover, no kinetic model could perfectly simulate the adsorption process. It indicated that the colloidal struction and morphology of MOCs or NDOM in seawater might be inhomogeneous. Hence, the interaction between PGE ions and organic matter in seawater was a complicated process and needs further research.
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Key words:
- adsorption /
- kinetics /
- platinum group elements /
- macromolecular organic compounds /
- natural organic matter /
- seawater
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