Pritzker School of Molecular Engineering, University of Chicago, Chicago, Illinois 60637, United States.
Chemical Engineering Department, Ben-Gurion University, Beer Sheva 841050, Israel.
J Am Chem Soc. 2021 Mar 24;143(11):4440-4450. doi: 10.1021/jacs.1c01241. Epub 2021 Mar 15.
With rising consumer demands, society is tapping into wastewater as an innovative source to recycle depleting resources. Novel reclamation technologies have been recently explored for this purpose, including several that optimize natural biological processes for targeted reclamation. However, this emerging field has a noticeable dearth of synthetic material technologies that are programmed to capture, release, and recycle specified targets; and of the novel materials that do exist, synthetic platforms incorporating biologically inspired mechanisms are rare. We present here a prototype of a materials platform utilizing peptide amphiphiles that has been molecularly engineered to sequester, release, and reclaim phosphate through a stimuli-responsive pH trigger, exploiting a protein-inspired binding mechanism that is incorporated directly into the self-assembled material network. This material is able to harvest and controllably release phosphate for multiple cycles of reuse, and it is selective over nitrate and nitrite. We have determined by simulations that the binding conformation of the peptide becomes constrained in the dense micelle corona at high pH such that phosphate is expelled when it otherwise would be preferentially bound. However, at neutral pH, this dense structure conversely employs multichain binding to further stabilize phosphate when it would otherwise be unbound, opening opportunities for higher-order conformational binding design to be engineered into this controllably packed corona. With this work, we are pioneering a new platform to be readily altered to capture other valuable targets, presenting a new class of capture and release materials for recycling resources on the nanoscale.
随着消费者需求的增长，社会正在利用废水作为一种创新的资源回收方式来回收日益减少的资源。最近，人们已经探索了一些新型的回收技术来实现这一目标，包括几种优化自然生物过程以实现目标回收的技术。然而，这个新兴领域明显缺乏经过编程以捕获、释放和回收特定目标的合成材料技术；而且，现有的新型材料中，很少有包含受生物启发机制的合成平台。我们在这里提出了一个利用肽两亲分子的材料平台原型，该平台经过分子工程设计，可以通过响应 pH 值的触发来隔离、释放和回收磷酸盐，利用直接纳入自组装材料网络中的受蛋白质启发的结合机制。这种材料能够进行多次循环再利用，以可控的方式回收和释放磷酸盐，并且对硝酸盐和亚硝酸盐具有选择性。我们通过模拟确定，在高 pH 值下，肽的结合构象在密集的胶束冠层中受到限制，从而在磷酸盐本来会优先结合的情况下将其排出。然而，在中性 pH 值下，这种密集的结构反而采用多链结合，在磷酸盐本来会未结合的情况下进一步稳定它，为在这种可控制的密集冠层中设计更高阶的构象结合提供了机会。通过这项工作，我们开创了一个新的平台，以方便地捕获其他有价值的目标，为纳米尺度上的资源回收提供了一类新的捕获和释放材料。
