气候变化领域集成服务门户(CCPortal): Computational discovery of chemically patterned surfaces that effect unique hydration water dynamics

CCPortal

DOI	10.1073/pnas.1807208115
	Computational discovery of chemically patterned surfaces that effect unique hydration water dynamics
	Monroe J.I.; Scott Shell M.
发表日期	2018
ISSN	0027-8424
起始页码	8093
结束页码	8098
卷号	115 期号:32
英文摘要	The interactions of water with solid surfaces govern their apparent hydrophobicity/hydrophilicity, influenced at the molecular scale by surface coverage of chemical groups of varied nonpolar/polar character. Recently, it has become clear that the precise patterning of surface groups, and not simply average surface coverage, has a significant impact on the structure and thermodynamics of hydration layer water, and, in turn, on macroscopic interfacial properties. Here we show that patterning also controls the dynamics of hydration water, a behavior frequently thought to be leveraged by biomole-cules to influence functional dynamics, but yet to be generalized. To uncover the role of surface heterogeneities, we couple a genetic algorithm to iterative molecular dynamics simulations to design the patterning of surface functional groups, at fixed coverage, to either minimize or maximize proximal water diffusivity. Optimized surface configurations reveal that clustering of hydrophilic groups increases hydration water mobility, while dispersing them decreases it, but only if hydrophilic moieties interact with water through directional, hydrogen-bonding interactions. Remarkably, we find that, across different surfaces, coverages, and patterns, both the chemical potential for inserting a methane-sized hydrophobe near the interface and, in particular, the hydration water orientational entropy serve as strong predictors for hydration water diffusivity, suggesting that these simple thermodynamic quantities encode the way surfaces control water dynamics. These results suggest a deep and intriguing connection between hydration water thermodynamics and dynamics, demonstrating that subnanometer chemical surface patterning is an important design parameter for engineering solid−water interfaces with applications spanning separations to catalysis. © 2018 National Academy of Sciences. All rights reserved.
英文关键词	computational inverse design; hydration dynamics; interfaces; Molecular dynamics simulations; water
语种	英语
scopus关键词	methane; water; algorithm; Article; catalysis; chemically patterned surface; computer analysis; controlled study; diffusion; entropy; hydration; hydrogen bond; hydrophilicity; molecular dynamics; priority journal; solid; surface property; thermodynamics
来源期刊	Proceedings of the National Academy of Sciences of the United States of America
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/160485
作者单位	Monroe, J.I., Department of Chemical Engineering, University of California, Santa Barbara, CA 93106; Scott Shell, M., Department of Chemical Engineering, University of California, Santa Barbara, CA 93106
推荐引用方式 GB/T 7714	Monroe J.I.,Scott Shell M.. Computational discovery of chemically patterned surfaces that effect unique hydration water dynamics[J],2018,115(32).
APA	Monroe J.I.,&Scott Shell M..(2018).Computational discovery of chemically patterned surfaces that effect unique hydration water dynamics.Proceedings of the National Academy of Sciences of the United States of America,115(32).
MLA	Monroe J.I.,et al."Computational discovery of chemically patterned surfaces that effect unique hydration water dynamics".Proceedings of the National Academy of Sciences of the United States of America 115.32(2018).