Su Yi-Ting, Chiu Hsiao-Chu, Su Cheng-Kuan
Department of Chemistry, National Chung Hsing University, Taichung City, 402202, Taiwan, ROC.
Department of Chemistry, National Chung Hsing University, Taichung City, 402202, Taiwan, ROC.
Talanta. 2025 Jan 1;282:126998. doi: 10.1016/j.talanta.2024.126998. Epub 2024 Oct 4.
Four-dimensional printing (4DP) technologies are revolutionizing the fabrication, functionality, and applicability of stimuli-responsive analytical devices. More practically, 4DP technologies are effective in fabricating devices with complex geometric designs and functions, and the degree of shape programming of 4D-printed stimuli-responsive devices can be optimized to become a reliable analytical strategy. Although shape-programming modes play a critical role in determining the analytical characteristics of 4D-printed stimuli-responsive sensing devices, the effect of shape-programming modes on the analytical performance of 4D-printed stimuli-responsive devices remains an unexplored subject. We employed digital light processing three-dimensional printing (3DP) with acrylate-based photocurable resins and 2-carboxyethyl acrylate (CEA)-incorporated photocurable resins for 4DP of the bending, helixing, and twisting needles. Upon immersion in samples with pH values above the pK of CEA, the electrostatic repulsion among the dissociated carboxyl groups of polyCEA caused swelling of the CEA-incorporated part and [H]-dependent shape programming. When coupling with the derivatization reaction of the urease-mediated hydrolysis of urea, the decline in [H] induced shape programming of the needles, offering reliable determination of urea based on the shape-programming angles. After optimizing the experimental conditions, the helixing needles provided the best analytical performance, with the method's detection limit of 0.9 μM. The reliability of this analytical method was validated by determining urea in samples of human urine and sweat, fetal bovine serum, and rat plasma with spike analyses and comparing these results with those obtained from a commercial assay kit. Our demonstration and analytical results suggest the importance of optimizing the shape-programming modes to improve the analytical performance of 4D-printed stimuli-responsive shape-programming sensing devices and emphasize the benefits and applicability of 4DP technologies in advancing the development and fabrication of stimuli-responsive sensing devices for chemical sensing and quantitative chemical analyses.
四维打印（4DP）技术正在彻底改变刺激响应型分析装置的制造、功能和适用性。更实际地说，4DP技术在制造具有复杂几何设计和功能的装置方面很有效，并且可以优化4D打印刺激响应型装置的形状编程程度，使其成为一种可靠的分析策略。尽管形状编程模式在决定4D打印刺激响应型传感装置的分析特性方面起着关键作用，但形状编程模式对4D打印刺激响应型装置分析性能的影响仍是一个未被探索的课题。我们采用基于丙烯酸酯的光固化树脂和含2-羧乙基丙烯酸酯（CEA）的光固化树脂进行数字光处理三维打印（3DP），以实现弯曲、螺旋和扭转针的4DP。将其浸入pH值高于CEA的pK的样品中时，聚CEA解离羧基之间的静电排斥导致含CEA部分膨胀以及与[H]相关的形状编程。当与脲酶介导的尿素水解的衍生化反应相结合时，[H]的下降引发针的形状编程，基于形状编程角度提供可靠的尿素测定。优化实验条件后，螺旋针提供了最佳分析性能，该方法的检测限为0.9 μM。通过对人尿液和汗液、胎牛血清及大鼠血浆样品中的尿素进行加标分析，并将结果与商业检测试剂盒所得结果进行比较，验证了该分析方法的可靠性。我们的论证和分析结果表明，优化形状编程模式对于提高4D打印刺激响应型形状编程传感装置的分析性能很重要，并强调了4DP技术在推进用于化学传感和定量化学分析的刺激响应型传感装置的开发和制造方面的益处及适用性。
