To understand the emergence of function in complex reaction networks is a primary goal of systems chemistry and origin-of-life studies. Especially challenging is the establishment of systems that simultaneously exhibit several functionality parameters that can be independently tuned. In this work, a multifunctional complex reaction network of nucleophilic small molecule catalysts for the Morita-Baylis-Hillman (MBH) reaction is demonstrated. The dynamic system exhibited triggered self-resolution, preferentially amplifying a specific catalyst/product set out of a many potential alternatives. By utilizing selective reversibility of the products of the reaction set, systemic thermodynamically driven error-correction could also be introduced. To achieve this, a dynamic covalent MBH reaction based on adducts with internal H-transfer capabilities was developed, displaying rate accelerations of retro-MBH reactions up to 104 times. This study demonstrates how efficient self-sorting of catalytic systems can be achieved through an interplay of several complex emergent functionalities.

中文翻译：

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催化反应网络中的活化的自解析和纠错

理解复杂反应网络中功能的出现是系统化学和生命起源研究的主要目标。尤其具有挑战性的是建立同时显示可以独立调整的几个功能参数的系统。在这项工作中，展示了用于森田-贝利斯-希尔曼（MBH）反应的亲核小分子催化剂的多功能复杂反应网络。该动态系统表现出触发的自我分辨率，可从许多潜在替代方案中优先扩增特定的催化剂/产物。通过利用反应组产物的选择性可逆性，还可以引入系统热力学驱动的误差校正。为了达成这个，开发了基于具有内部H转移能力的加合物的动态共价MBH反应，显示逆向MBH反应的速率加速高达104倍。这项研究表明如何通过几个复杂的紧急功能的相互作用来实现催化系统的高效自选。