纳微尺度溶液体系的精确计算

Accurate modeling of aqueous chemistry at the nano-/micro-scale

在纳微尺度上,分子性质、传质过程、化学反应等均与在宏观尺度表现不同.因此,近年来在生命科学、材料科学等领域对于纳微尺度下的液滴和溶液体系的研究蓬勃发展.采用计算模拟手段对相关体系的准确表征有助于揭示其在微观层面的分子机制,并为解开生命的奥秘、促进新材料的研发提供新的见解.本综述回顾了使用模拟方法,包括分子力场、量子化学方法以及结合机器学习等,研究此类体系的最新进展,重点关注纳微尺度下气液界面(包括空气/水、空气/溶液,以及大气/水)的溶液体系.此外,我们还对适用于纳微尺度溶液化学的计算模拟手段未来的发展进行了展望.

At the nano-/micro-scale,the properties of molecules,material transfer,chemical reactions,and other processes exhibit distinct characteristics from those observed at the macroscopic scale.In recent years,the research on droplet and aqueous chemistry at the nano/micro scale in areas such as life sciences,materials science,and other fields has flourished.Accurate calculations and characterization of such systems help to reveal the molecular mechanisms that give rise to their unique properties at the microscopic level,and provide new insights for unraveling the mysteries of life and facilitating the research and development of new materials.This paper provides a review of recent scientific advances in studying such systems using simulation methods,including molecular force fields,quantum chemical methods,and the combination of machine learning algorithms,with a focus on aqueous systems at the gas–liquid interfaces at the nano-/micro-scales(including air/water,air/solution,and atmosphere/water),with bulk-phase liquids serving as a reference.In addition,we also provide an outlook on the future development of computational techniques for characterizing such systems.