{Ba2+}:{SO42–} 对水溶液中 BaSO4 晶体成核和生长的不对称依赖性：动态光散射研究,ACS Omega

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{Ba2+}:{SO42–} 对水溶液中 BaSO4 晶体成核和生长的不对称依赖性：动态光散射研究
ACS Omega ( IF 3.7 ) Pub Date : 2023-01-30 , DOI: 10.1021/acsomega.2c07418
Sergěj Y M H Seepma ₁ , Bonny W M Kuipers ₂ , Mariette Wolthers ₁

Affiliation

使用动态光散射 (DLS) 研究了溶液化学计量在 0.02 M NaCl 悬浮液中形成 BaSO ₄晶体后对粒径发展的影响。根据组分离子活度乘积 {Ba ²⁺ }{SO ₄^2– } 与溶解度乘积K _sp (Ω_重晶石= {Ba ²⁺ } {SO ₄^2– }/ K _sp = 100、500 或 1000–11,000，步长为 1000），以及离子活度溶液化学计量（r _aq = {Ba ²⁺}:{SO ₄^2– } = 0.01, 0.1, 1, 10 和 100)，在环中性 pH 值 5.5–6.0 以及环境温度和压力下。DLS 表明，对于批量实验，在 1000 的初始 Ω_重晶石和使用前向检测角时，可以最好地研究具有不同r _aq的晶体形成。在这个 Ω_重晶石和一组raq下，所有悬浮液中存在的最大群体的平均表观流体动力学粒径在 10-15 分钟内从 ~200 增加到 ~700 nm，并通过透射电子显微镜 (TEM) 成像独立证实_。在相同流动条件下进行的额外 DLS 测量证实 BaSO ₄对于我们特别选择的条件，形成动力学非常快。DLS 流量测量监测 BaSO _{4形成的第一分钟，显示出强烈的预成核簇聚集迹象，形成每个}r _aq大小在 200–300 nm 范围内的颗粒。从批量 DLS 结果估计的初始整体生长速率表明，BaSO ₄晶体在接近化学计量的条件下形成最快，而在非化学计量条件下形成得更慢。此外，在极端 SO ₄-限制条件，与 Ba 限制条件相比，重晶石形成速度较慢。我们的结果表明，DLS 可用于在精心选择的实验和分析条件下研究成核和生长。DLS 和 TEM 的组合结果表明 BaSO ₄的形成受溶液化学计量的影响，可能有助于优化阻垢剂效率并调节 BaSO ₄（水垢）形成过程。

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Asymmetrical Dependence of {Ba2+}:{SO42–} on BaSO4 Crystal Nucleation and Growth in Aqueous Solutions: A Dynamic Light Scattering Study

The impact of solution stoichiometry, upon formation of BaSO₄ crystals in 0.02 M NaCl suspensions, on the development of particle size was investigated using dynamic light scattering (DLS). Measurements were performed on a set of suspensions prepared with predefined initial supersaturation, based on the quotient of the constituent ion activity product {Ba²⁺}{SO₄^2–} over the solubility product K_sp (Ω_barite = {Ba²⁺}{SO₄^2–}/K_sp = 100, 500, or 1000–11,000 in steps of 1000), and ion activity solution stoichiometries (r_aq = {Ba²⁺}:{SO₄^2–} = 0.01, 0.1, 1, 10 and 100), at circumneutral pH of 5.5–6.0, and ambient temperature and pressure. DLS showed that for batch experiments, crystal formation with varying r_aq was best investigated at an initial Ω_barite of 1000 and using the forward detection angle. At this Ω_barite and set of r_aq, the average apparent hydrodynamic particle size of the largest population present in all suspensions increased from ∼200 to ∼700 nm within 10–15 min and was independently confirmed by transmission electron microscopy (TEM) imaging. Additional DLS measurements conducted at the same conditions in flow confirmed that the BaSO₄ formation kinetics were very fast for our specifically chosen conditions. The DLS flow measurements, monitoring the first minute of BaSO₄ formation, showed strong signs of aggregation of prenucleation clusters forming particles with a size in the range of 200–300 nm for every r_aq. The estimated initial bulk growth rates from batch DLS results show that BaSO₄ crystals formed fastest at near-stoichiometric conditions and more slowly at nonstoichiometric conditions. Moreover, at extreme SO₄-limiting conditions, barite formation was slower compared to Ba-limiting conditions. Our results show that DLS can be used to investigate nucleation and growth at carefully selected experimental and analytical conditions. The combined DLS and TEM results imply that BaSO₄ formation is influenced by solution stoichiometry and may aid to optimize antiscalant efficiency and regulate BaSO₄ (scale) formation processes.

更新日期：2023-01-30

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