Life-Like Materials and Systems, Department of Chemistry, University of Mainz, Duesbergweg 10-14, 55128 Mainz, Germany.
Chem Commun (Camb). 2023 Jan 26;59(9):1125-1144. doi: 10.1039/d2cc06402b.
pH-responsive systems have gained importance for the development of smart materials and for biomedical applications because they can switch between different states by simple acid/base triggers. However, such equilibrium systems lack the autonomous behaviour that is so ubiquitous in living systems that self-regulate out of equilibrium. As a contribution to the emerging field of autonomous chemical systems, we have developed pH-feedback systems (pH-FS) based on the coupling of acid- and base-producing steps in chemical reaction networks. The resulting autonomous nonlinear pH curves can be coupled with a variety of pH-sensitive building blocks to program the lifecycles of the associated transient state at the level of self-assemblies and material systems. In this article, we discuss the different generations of such pH-feedback systems, the principles of their coupling to self-assemblies with lifecycles and highlight emerging concepts for the design of autonomous functional materials. The specificity, robustness, and flexible operation of such pH-FS can also be used to realize chemo-structural and chemo-mechanical feedbacks that extend the behaviour of such materials systems toward complex and functional life-like systems.
pH 响应系统在智能材料和生物医学应用方面的重要性日益增加，因为它们可以通过简单的酸碱触发在不同状态之间切换。然而，这样的平衡系统缺乏自主性，而自主性在生命系统中无处不在，生命系统可以在不平衡的情况下自我调节。作为对自主化学系统这一新兴领域的贡献，我们已经开发了基于化学反应网络中酸和碱产生步骤耦合的 pH 反馈系统（pH-FS）。由此产生的自主非线性 pH 曲线可以与各种 pH 敏感构建块耦合，以在自组装和材料系统的水平上对相关瞬态的生命周期进行编程。在本文中，我们讨论了这种 pH 反馈系统的不同代，它们与具有生命周期的自组装耦合的原理，并强调了用于设计自主功能材料的新兴概念。这种 pH-FS 的特异性、鲁棒性和灵活的操作也可用于实现化学结构和化学机械反馈，从而使这些材料系统的行为向复杂的、功能类似生命的系统扩展。
