Department of Chemistry, Technical University of Munich, Lichtenbergstrasse 4, 85748, Garching, Germany.
Catalysis Research Centre, Technical University of Munich, Lichtenbergstrasse 4, 85748, Garching, Germany.
Nat Commun. 2022 May 20;13(1):2816. doi: 10.1038/s41467-022-30424-2.
The ability to store information in chemical reaction networks is essential for the complex behavior we associate with life. In biology, cellular memory is regulated through transcriptional states that are bistable, i.e., a state that can either be on or off and can be flipped from one to another through a transient signal. Such memory circuits have been realized synthetically through the rewiring of genetic systems in vivo or through the rational design of reaction networks based on DNA and highly evolved enzymes in vitro. Completely bottom-up analogs based on small molecules are rare and hard to design and thus represent a challenge for systems chemistry. In this work, we show that bistability can be designed from a simple non-equilibrium reaction cycle that is coupled to crystallization. The crystals exert the necessary feedback on the reaction cycle required for the bistability resulting in an on-state with assemblies and an off-state without. Each state represents volatile memory that can be stored in continuously stirred tank reactors indefinitely even though molecules are turned over on a minute-timescale. We showcase the system's abilities by creating a matrix display that can store images and by creating an OR-gate by coupling several switches together.
信息在化学反应网络中的存储能力对于我们所认为的生命的复杂行为至关重要。在生物学中,细胞记忆是通过转录状态来调节的,这些状态是双稳态的,即一种状态要么是开启的,要么是关闭的,可以通过短暂的信号从一种状态翻转到另一种状态。这种记忆电路已经通过在体内重新布线遗传系统或通过基于 DNA 和高度进化的酶在体外合理设计反应网络来实现。完全基于小分子的自下而上的类似物很少见,也很难设计,因此对系统化学来说是一个挑战。在这项工作中,我们表明,双稳性可以从一个简单的非平衡反应循环设计,该循环与结晶相耦合。晶体对双稳性所需的反应循环施加必要的反馈,导致有组装的开启状态和无组装的关闭状态。每个状态都代表着易失性记忆,可以在连续搅拌罐反应器中无限期地存储,即使分子在分钟尺度上被替换。我们通过创建一个可以存储图像的矩阵显示器,并通过将几个开关耦合在一起创建一个或门,展示了该系统的能力。