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溶液 P 核磁共振研究无定形氧化铝水合物-水界面上的肌醇六磷酸表面络合物。

Solution P NMR Investigation of Inositol Hexakisphosphate Surface Complexes at the Amorphous Aluminum Oxyhydroxide-Water Interface.

机构信息

Department of Natural Resources and Environmental Sciences, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States.

出版信息

Environ Sci Technol. 2021 Nov 2;55(21):14628-14638. doi: 10.1021/acs.est.1c04421. Epub 2021 Oct 11.

DOI:10.1021/acs.est.1c04421
PMID:34633799
Abstract

Phytate (-inositol hexakisphosphate, -IHP) is one of the most common organic phosphorus (P) species in soils and sediments which can be mineralized to increase the concentration of dissolved phosphate in pore water. Because of its six phosphate functional groups, functional group-specific adsorption mechanisms in reactive soil minerals become important in predicting solubility. In this study, solution P NMR was used to elucidate the functional group-specific adsorption mechanisms of -IHP at the amorphous Al hydroxide (AAH)-water interface at pH 6.5 in conjunction with batch adsorption experiments and Zetasizer measurements. The adsorption maximum of -IHP with AAH was ∼312.50 mmol kg, and the charge reversal effects in IHP-reacted AAH particles suggested the presence of inner-sphere surface species. The upfield shifts of various phosphate groups in the NMR spectra further supported the formation of inner-sphere IHP complexes at the AAH-water interface. When the initial -IHP/AAH (mol kg) was decreased from 2.5 to 1.25-1.67, P1,3 and P4,6 functional groups were coordinated in addition to P2; P5 became reactive with the ratio being decreased to <0.84, P5. This multifunctional group coordination increased aggregate size. The study showed that the availability of surface sites of adsorbents influenced the functional group-specific -IHP adsorption.

摘要

植酸(-肌醇六磷酸,-IHP)是土壤和沉积物中最常见的有机磷(P)物种之一,它可以矿化以增加孔水中溶解磷酸盐的浓度。由于其具有六个磷酸官能团,因此在预测溶解度时,反应性土壤矿物质中的官能团特异性吸附机制变得很重要。在这项研究中,在 pH 6.5 下,使用溶液 P NMR 结合批吸附实验和 Zetasizer 测量,阐明了 -IHP 在无定形氢氧化铝(AAH)-水界面上的官能团特异性吸附机制。-IHP 与 AAH 的最大吸附量约为 312.50 mmol kg,并且 IHP 反应的 AAH 颗粒中的电荷反转效应表明存在内球表面物种。NMR 光谱中各种磷酸盐基团的向上位移进一步支持了在 AAH-水界面上形成内球 IHP 配合物。当初始 -IHP/AAH(mol kg)从 2.5 降低至 1.25-1.67 时,除 P2 外,P1,3 和 P4,6 官能团也得到了配位;当比例降低至 <0.84 时,P5 变得具有反应性。这种多功能团配位增加了聚集体的尺寸。该研究表明,吸附剂表面位点的可用性影响了官能团特异性 -IHP 吸附。

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引用本文的文献

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Enhancing Phytate Availability in Soils and Phytate-P Acquisition by Plants: A Review.提高土壤中植酸的有效性和植物对植酸的获取:综述。
Environ Sci Technol. 2022 Jul 5;56(13):9196-9219. doi: 10.1021/acs.est.2c00099. Epub 2022 Jun 8.