Harnessing Peptide Binding to Capture and Reclaim Phosphate
Harnessing Peptide Binding to Capture and Reclaim Phosphate
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DOI：
10.1021/jacs.1c01241
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发表时间：
2021-03-15
影响因子：
15
通讯作者：
Tirrell, Matthew, V
中科院分区：
文献类型：
--
作者：
Fowler, Whitney C.;Deng, Chuting;Tirrell, Matthew, V
随着消费者需求的不断增长，社会正在利用废水作为回收消耗资源的创新来源。最近为此目的探索了新的回收技术，包括一些优化自然生物过程以实现有针对性的回收的技术。然而，这个新兴领域明显缺乏能够捕获、释放和回收特定目标的合成材料技术；在现有的新型材料中，结合生物启发机制的合成平台很少见。我们在这里展示了一个利用肽两亲物的材料平台原型，该材料平台经过分子工程设计，可通过刺激响应 pH 触发器来隔离、释放和回收磷酸盐，利用直接纳入自组装材料网络的蛋白质启发的结合机制。这种材料能够收集并可控地释放磷酸盐以进行多次重复利用，并且它比硝酸盐和亚硝酸盐具有选择性。我们通过模拟确定，在高 pH 条件下，肽的结合构象在致密胶束冠中受到限制，使得磷酸盐在原本会优先结合的情况下被排出。然而，在中性pH下，这种致密结构相反地采用多链结合来进一步稳定磷酸盐，否则磷酸盐将处于未结合状态，从而为将高阶构象结合设计工程化到这种可控堆积的冠中提供了机会。通过这项工作，我们正在开创一个新平台，可以轻松改变以捕获其他有价值的目标，提供一类新型捕获和释放材料，用于在纳米尺度上回收资源。
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.