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在乙二胺四乙酸(EDTA)存在下重晶石(001)表面的铅吸附与解吸

Lead Adsorption and Desorption at the Barite (001) Surface in the Presence of EDTA.

作者信息

Dorfman Amanda, Wanhala Anna K, Lee Sang Soo, Eng Peter J, Stubbs Joanne E, Kenis Lexi, Bracco Jacquelyn N

机构信息

School of Earth and Environmental Sciences, Queens College, City University of New York, Queens, New York 11367, United States.

Center for Advanced Radiation Sources, University of Chicago, Chicago, Illinois 60439, United States.

出版信息

ACS ES T Water. 2024 Dec 17;5(1):264-273. doi: 10.1021/acsestwater.4c00836. eCollection 2025 Jan 10.

Abstract

Scaling minerals, such as barite, can cause detrimental consequences for oil/gas pipelines and water systems, but their formation can be inhibited by organic chelators such as ethylenediaminetetraacetic acid (EDTA). Here, we resolve how EDTA affects sorption and desorption of Pb at the barite (001) surface using a combination of X-ray scattering and microscopy measurements. In the presence of EDTA, Pb incorporated in the topmost part of the barite surface and adsorbed as inner-sphere complexes on the surface. In barite saturated solutions containing [Pb] ≥ 100 μM, overgrowth films grew along step edges. These films were exclusively monolayer thick, indicating that their growth was a self-limiting process. Approximately half of the Pb was removed after 14.5 h reaction with a Pb-free EDTA solution where most of the desorption occurred to adsorbed Pb rather than incorporated Pb. Dissolution proceeded primarily via step retreat and etch pit formation in EDTA, but in deionized water, the secondary phase was quickly removed within 3 min. Together these results suggest EDTA binds to both the surface and Pb in solution, which limits Pb sorption. However, EDTA binding to the surface also inhibits removal of the secondary phase that formed at higher Pb concentrations.

摘要

重晶石等结垢矿物会给石油/天然气管道和水系统带来不利影响,但其形成可被乙二胺四乙酸(EDTA)等有机螯合剂抑制。在此,我们结合X射线散射和显微镜测量,解析了EDTA如何影响重晶石(001)表面铅的吸附和解吸。在EDTA存在的情况下,铅掺入重晶石表面的最顶层,并以内层配合物的形式吸附在表面。在含铅量≥100 μM的重晶石饱和溶液中,外延生长膜沿台阶边缘生长。这些膜仅为单层厚度,表明其生长是一个自限过程。与无铅EDTA溶液反应14.5小时后,约一半的铅被去除,其中大部分解吸发生在吸附的铅而非掺入的铅上。在EDTA中,溶解主要通过台阶后退和蚀刻坑形成进行,但在去离子水中,次生相在3分钟内迅速被去除。这些结果共同表明,EDTA与溶液中的表面和铅都结合,这限制了铅的吸附。然而,EDTA与表面的结合也抑制了在较高铅浓度下形成的次生相的去除。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/70d8/11731300/1590e779386b/ew4c00836_0001.jpg

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