Molecular Mechanism of Linear Polyphosphate Adsorption on Iron and Aluminum Oxides,The Journal of Physical Chemistry C

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Molecular Mechanism of Linear Polyphosphate Adsorption on Iron and Aluminum Oxides
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2020-12-16 , DOI: 10.1021/acs.jpcc.0c06127
Biao Wan ₁ , Evert J. Elzinga ₂ , Rixiang Huang ₃ , Yuanzhi Tang ₁

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Polyphosphate is a polymeric P species with environmental and industrial significance. Understanding their interaction with natural minerals is fundamental for predicting their transport and fate in the environment. This study investigates the molecular mechanism of interaction between linear polyphosphates with varied chain length (15P, 60P, and 130P) and Fe/Al oxides using quartz crystal microbalance with dissipation (QCM-D), ³¹P solid-state nuclear magnetic resonance (NMR) spectroscopy, and attenuated total reflection–Fourier transformed infrared (ATR–FTIR) spectroscopy. QCM-D results show that all three polyphosphates irreversibly adsorb on Fe/Al oxides at pH 4–10 with similar mass-based adsorption amounts despite the large difference in chain lengths. ATR–FTIR and NMR spectroscopy results suggest that terminal phosphate groups of the polyphosphate molecules may form bidentate binuclear surface complexes, and a fraction of middle phosphate groups may form monodentate mononuclear surface complexes on Fe/Al oxides. The interaction modes persist for both minerals and all tested pH conditions. A combination of these complementary techniques helps gain a mechanistic understanding of polyphosphate interaction with Fe/Al oxides, and the results fill a knowledge gap on polyphosphate cycling in natural environments.

中文翻译：

线性多磷酸盐在铁和铝氧化物上吸附的分子机理

聚磷酸盐是具有环境和工业意义的聚合P物质。了解它们与天然矿物的相互作用是预测其在环境中的运输和命运的基础。本研究使用耗散的石英晶体微天平（QCM-D）研究了链长可变（15P，60P和130P）的线性多磷酸盐与Fe / Al氧化物之间相互作用的分子机理，[ ^31]P固态核磁共振（NMR）光谱，以及衰减的全反射-傅立叶变换红外（ATR-FTIR）光谱。QCM-D结果表明，尽管链长差异很大，但所有三种聚磷酸盐在pH 4-10时均不可逆地吸附在Fe / Al氧化物上，具有相似的基于质量的吸附量。ATR–FTIR和NMR光谱结果表明，多磷酸盐分子的末端磷酸基团可能形成双齿双核表面配合物，而部分中间磷酸基团可能在Fe / Al氧化物上形成单齿单核表面配合物。对于矿物质和所有测试的pH条件，相互作用模式均保持不变。这些互补技术的结合有助于对多磷酸盐与Fe / Al氧化物的相互作用进行机械理解，

更新日期：2020-12-31

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