Poly(acrylic acid) Hydrogel Microspheres for a Metal-Ion Sensor,ACS Sensors

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Poly(acrylic acid) Hydrogel Microspheres for a Metal-Ion Sensor
ACS Sensors ( IF 8.2 ) Pub Date : 2021-01-17 , DOI: 10.1021/acssensors.0c02269
Hao Tan ₁ , Soo-Young Park ₁

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Monodispersed cross-linked poly(acrylic acid) (PAA) droplets (PAA X-droplets), prepared using the microfluidic method with in situ ultraviolet curing, were used as small spherical sensors to simultaneously detect both Ca²⁺ and Mg²⁺ in human saliva and serum. The PAA X-droplet treated with KOH (PAA_KOH X-droplet) was used as a reference droplet because of its highly swollen state. The PAA_KOH X-droplets shrunk in response to the presence of divalent metal ions (Ms) by forming a bridged structure of COO–M–OOC. The sizes of the PAA_KOH X-droplets were precisely and dynamically monitored in the poly(dimethylsiloxane) (PDMS) channel with passing time when the aqueous metal-ion solutions were flowing at a controlled flow rate. The sizes of the PAA_KOH X-droplets continuously decreased to the saturated constant size. The saturated size of the PAA_KOH X-droplet did not change; however, the speed of size reduction increased with an increase in the concentration of the divalent metal ion. The saturated size was studied using the saturated diameter ratio (R_sat-dia) with respect to the initial diameter of the PAA_KOH X-droplet before the metal-ion treatment, and the speed of the size reduction was investigated using the inverse time to reach half the saturated diameter reduction (T_1/2^–1). Ca²⁺ and Mg²⁺ exhibited R_sat-dia values of 75.9 and 83.6%, respectively, when the flow rate was 5 μL min^–1, regardless of the metal concentration. The T_1/2^–1s for the Ca²⁺ and Mg²⁺ linearly increased with an increase in their concentrations. The R_sat-dia of the aqueous Ca²⁺/Mg²⁺ mixture solution had a linear relationship with φ [= C_Ca/(C_Ca + C_Mg), where C_Ca and C_Mg are the molar concentrations of Ca²⁺ and Mg²⁺, respectively]. The T_1/2^–1 of the aqueous Ca²⁺, Mg²⁺ mixture solution was calculated by adding the individual T_1/2^–1s of pure aqueous Ca²⁺ and Mg²⁺ solutions. Using the R_sat-dia and T_1/2^–1 of the Ca²⁺/Mg²⁺ mixture aqueous solution, the individual C_Ca and C_Mg in the mixture solution were successfully calculated. This method was applied to the human saliva and serum in which the major metal ions are Ca²⁺ and Mg²⁺, and other metal ions existed in undetectable amounts by the PAA_KOH X-droplets. This method is simple, cost-effective, and highly accurate and solves the hurdles of separating the interference effect of a Mg²⁺ ion when a Ca²⁺ ion is measured in biofluids.

中文翻译：

用于金属离子传感器的聚丙烯酸水凝胶微球

使用微流体方法和原位紫外线固化制备的单分散交联聚丙烯酸（PAA）液滴（PAA X液滴）用作小型球形传感器，以同时检测人体中的Ca ²⁺和Mg ²⁺唾液和血清。用KOH处理过的PAA X-液滴（PAA _KOH X-液滴）由于其高度溶胀状态而被用作参考液滴。通过形成COO–M–OOC的桥联结构，PAA _KOH X液滴响应二价金属离子（Ms）的存在而收缩。PAA _KOH的大小当金属离子水溶液以受控的流速流动时，随着时间的流逝，在聚二甲基硅氧烷（PDMS）通道中精确动态地监测X滴。PAA _KOH X液滴的大小连续减小到饱和的恒定大小。PAA _KOH X液滴的饱和大小没有变化；然而，随着二价金属离子浓度的增加，尺寸减小的速度增加。使用相对于PAA _KOH初始直径的饱和直径比（R _sat-dia）研究饱和尺寸使用倒数时间达到饱和直径减小的一半（T _1/2^–1）的时间来研究金属离子处理之前的X液滴和尺寸减小的速度。的Ca ²⁺和Mg ²⁺显示出ř _SAT-直径分别75.9和83.6％，值，当流率为5μL分钟^-1，而不管该金属的浓度。Ca ²⁺和Mg ²⁺的T _1/2^–1 s随着浓度的增加而线性增加。Ca ²⁺ / Mg ²⁺的R_饱和度混合溶液与φ[= C _Ca /（C _Ca + C _Mg）具有线性关系，其中C _Ca和C _Mg分别是Ca ²⁺和Mg ²⁺的摩尔浓度]。所述Ť _1/2^-1钙水溶液²⁺，镁²⁺混合物溶液通过将各个计算的Ť _1/2^-1 S的纯水溶液的Ca ²⁺和Mg ²⁺的解决方案。使用R_饱和直径和T _1/2成功计算了^–1的Ca ²⁺ / Mg ²⁺混合物水溶液中的各个C _Ca和C _Mg。此方法适用于主要金属离子为Ca ²⁺和Mg ²⁺的人唾液和血清，而PAA _KOH X-droplets无法检测到其他金属离子。该方法简单，经济，准确度高，解决了在生物流体中测量Ca ²⁺离子时分离Mg ²⁺离子的干扰效应的障碍。

更新日期：2021-03-26

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