Department of Chemical Sciences|, University of Padova, Via Marzolo 1, 35131, Padova, Italy.
Angew Chem Int Ed Engl. 2021 Sep 6;60(37):20120-20143. doi: 10.1002/anie.202100274. Epub 2021 Apr 7.
Life is a non-equilibrium state of matter maintained at the expense of energy. Nature uses predominantly chemical energy stored in thermodynamically activated, but kinetically stable, molecules. These high-energy molecules are exploited for the synthesis of other biomolecules, for the activation of biological machinery such as pumps and motors, and for the maintenance of structural order. Knowledge of how chemical energy is transferred to biochemical processes is essential for the development of artificial systems with life-like processes. Here, we discuss how chemical energy can be used to control the structural organization of organic molecules. Four different strategies have been identified according to a distinguishable physical-organic basis. For each class, one example from biology and one from chemistry are discussed in detail to illustrate the practical implementation of each concept and the distinct opportunities they offer. Specific attention is paid to the discussion of chemically fueled non-equilibrium self-assembly. We discuss the meaning of non-equilibrium self-assembly, its kinetic origin, and strategies to develop synthetic non-equilibrium systems.
生命是以消耗能量为代价维持的一种非平衡态物质。自然界主要利用储存在热力学激活但动力学稳定的分子中的化学能量。这些高能分子被用于合成其他生物分子、激活泵和马达等生物机器,以及维持结构有序性。了解化学能如何传递到生化过程对于开发具有类似生命过程的人工系统至关重要。在这里,我们讨论了如何利用化学能来控制有机分子的结构组织。根据可区分的物理有机基础,确定了四种不同的策略。对于每一类,我们从生物学和化学中各讨论一个实例,详细说明每个概念的实际实现以及它们提供的独特机会。特别关注讨论化学燃料驱动的非平衡自组装。我们讨论了非平衡自组装的含义、其动力学起源以及开发合成非平衡系统的策略。