title: Unraveling Mixed Hydrate Formation: Microscopic Insights into Early Stage Behavior.
abstract: The molecular-level details of mixed hydrate nucleation remain unclear despite the broad implications of this process for a variety of scientific domains. Through analysis of mixed hydrate nucleation in a prototypical CH4/H2S/H2O system, we demonstrate that high-level kinetic similarities between mixed hydrate systems and corresponding pure hydrate systems are not a reliable basis for estimating the composition of early stage mixed hydrate nuclei. Moreover, we show that solution compositions prior to and during nucleation are not necessarily effective proxies for the composition of early stage mixed hydrate nuclei. Rather, microscopic details, (e.g., guest-host interactions and previously neglected cage types) apparently play key roles in determining early stage behavior of mixed hydrates. This work thus provides key foundational concepts and insights for understanding mixed hydrate nucleation.
authors.affiliation: Department of Chemistry, University of Calgary , 2500 University Drive NW, Calgary, T2N 1N4 Alberta, Canada.
authors.forename: Kyle Wm
authors.initials: KW
authors.lastname: Hall
authors.affiliation: Key Laboratory of Earth and Planetary Physics, Institute of Geology and Geophysics, Chinese Academy of Sciences , Beijing 100029, China.
authors.forename: Zhengcai
authors.initials: Z
authors.lastname: Zhang
authors.affiliation: Department of Chemistry, University of Calgary , 2500 University Drive NW, Calgary, T2N 1N4 Alberta, Canada.
authors.forename: Peter G
authors.identifier: 0000-0001-6270-663X
authors.initials: PG
authors.lastname: Kusalik