Université de Strasbourg, CNRS, ISIS, 8 allée Gaspard Monge, 67000 Strasbourg, France.
J Am Chem Soc. 2020 Mar 4;142(9):4083-4087. doi: 10.1021/jacs.9b11503. Epub 2020 Feb 21.
Nature uses catalysis as an indispensable tool to control assembly and reaction cycles in vital non-equilibrium supramolecular processes. For instance, enzymatic methionine oxidation regulates actin (dis-)assembly, and catalytic guanosine triphosphate hydrolysis is found in tubulin (dis-)assembly. Here we present a completely artificial reaction cycle which is driven by a chemical fuel that is catalytically obtained from a "pre-fuel". The reaction cycle controls the dis-assembly and re-assembly of a hydrogel, where the rate of pre-fuel turnover dictates the morphology as well as the mechanical properties. By addition of additional fresh aliquots of fuel and removal of waste, the hydrogels can be re-programmed time after time. Overall, we show how catalytic fuel generation can control reaction/assembly kinetics and materials' properties in life-like non-equilibrium systems.
自然界利用催化作用作为一种不可或缺的工具来控制重要的非平衡超分子过程中的组装和反应循环。例如，酶促蛋氨酸氧化调节肌动蛋白（解）组装，催化鸟苷三磷酸水解存在于微管蛋白（解）组装中。在这里，我们提出了一个完全人工的反应循环，该循环由化学燃料驱动，该燃料是从“预燃料”中催化获得的。该反应循环控制水凝胶的解聚和再组装，其中预燃料转化的速率决定了形态以及机械性能。通过添加额外的新鲜燃料和去除废物，水凝胶可以一次又一次地重新编程。总的来说，我们展示了催化燃料的产生如何控制类似生命的非平衡系统中的反应/组装动力学和材料特性。
