论文标题
微流体细胞中点击反应的静电催化
Electrostatic Catalysis of a Click Reaction in a Microfluidic Cell
论文作者
论文摘要
电场在大自然的酶促机械中被强调为智能试剂,因为它们可以直接触发或加速氧化还原和/或具有立体特异性的氧化还原和/或非还原化学工艺。在自然催化中,限制空间中化学物种的受控质量转运也是促进反应物进入活性反应部位的关键。尽管上述机会为开发策略开发用于利用定向电场的新的,干净的静电催化,但该领域的研究主要仅限于单分子或小分子集合水平的理论和实验研究,在这种研究中,无法测试对质量运输的控制和对量表的控制。在这里,我们量化了大面积电极表面中典型的Huisgen Cycloadition的静电催化,并将其性能与传统的Cu(I)催化方法进行了比较。在定制的微流体细胞中实现了质量扩散控制,该细胞增强了试剂向电动反应性界面的转运,同时避免了湍流条件和对流质量转运的不良控制。这个前所未有的静电连续流微流体反应器是电场驱动平台的一个示例,在该平台中可以有效地实施和调节干净的大规模静电催化过程。
Electric fields have been highlighted as a smart reagent in nature's enzymatic machinery, as they can directly trigger or accelerate redox and/or non-redox chemical processes with stereo- and regio-specificity. In natural catalysis, controlled mass transport of chemical species in confined spaces is also key in facilitating the transport of reactants into the active reaction site. Despite the opportunities the above offers in developing strategies for a new, clean electrostatic catalysis exploiting oriented electric fields, research in this area has been mostly limited to theoretical and experimental studies at the level of single molecules or small molecular ensembles, where both the control over mass transport and scalability cannot be tested. Here, we quantify the electrostatic catalysis of a prototypical Huisgen cycloaddition in a large-area electrode surface and directly compare its performance to the traditional Cu(I)-catalyzed method of the same reaction. Mass diffusion control is achieved in a custom-built microfluidic cell, which enhances reagent transport towards the electrified reactive interface while avoiding both turbulent flow conditions and poor control of the convective mass transport. This unprecedented electrostatic continuous-flow microfluidic reactor is an example of an electric-field driven platform where clean large-scale electrostatic catalytic processes can be efficiently implemented and regulated.