Yang Zhengpeng, Chang Yatao, Wang Yifan, Qin Tongtong, Liu Dapeng, Zhang Yuanyuan, Bao Xuejiao, Cao Yufang, Zhang Chunjing
School of Materials Science and Engineering, Henan Polytechnic University, Jiaozuo, 454003, PR China.
Key Laboratory of Multifunctional Nanomaterials and Smart Systems, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou, 215123, PR China.
Anal Bioanal Chem. 2025 Jun 4. doi: 10.1007/s00216-025-05938-5.
Channel-aligned modulation of a molecule-recognized photoelectrode to generate superior light-absorbing yet high-level analyte-adsorbing is pivotal but challenging for implementing highly sensitive and selective photoelectrochemical sensing. Herein, we demonstrated an innovative expansion-flow-modulated direct ink writing (DIW) 3D printing coupled with molecular imprinting technology for controllably building a microlattice-shaped photoelectrochemical sensor, with multiscale well-interconnected aligned channels created by vertically aligned arrangement of molecule-recognized photoactive graphene (G) nanosheets within printed filaments and regularly orthogonal layer-by-layer assembly of filaments. The unique architectural merit enabled rapid analyte diffusion and ready light spreading to photoactive and specific recognition sites located at all channel walls, thus endowing the sensor with a combined feature of prominent light absorption and analyte trapping. As a result, the 3D-printed (3DP) vertically aligned photoelectrochemical sensor with specific recognition sites displayed its remarkable capability for urea assay, with rapid response, low detection limit (10 nM), wide linear range (0.03-1100 µM), excellent selectivity, and working stability. This work has shed light on new strategies for processing advanced photoelectrochemical sensing architectures toward highly sensitive and selective assay.
对分子识别光电极进行通道对齐调制以产生优异的光吸收能力和高水平的分析物吸附能力，对于实现高灵敏度和选择性的光电化学传感至关重要，但也具有挑战性。在此，我们展示了一种创新的扩展流调制直接墨水书写（DIW）3D打印技术与分子印迹技术相结合的方法，用于可控地构建微晶格形状的光电化学传感器，通过在打印细丝内垂直排列分子识别的光活性石墨烯（G）纳米片以及细丝的规则正交逐层组装，形成多尺度良好互连的对齐通道。这种独特的结构优点使得分析物能够快速扩散，光能够顺利传播到位于所有通道壁上的光活性和特异性识别位点，从而赋予传感器突出的光吸收和分析物捕获的综合特性。结果，具有特异性识别位点的3D打印（3DP）垂直排列光电化学传感器在尿素检测中显示出卓越的能力，具有快速响应、低检测限（10 nM）、宽线性范围（0.03 - 1100 µM）、优异的选择性和工作稳定性。这项工作为处理先进的光电化学传感架构以实现高灵敏度和选择性检测提供了新策略。
