发表机构
Future Technology School, Shenzhen Technology University; College of Applied Sciences, Shenzhen University; College of Physical Science and Technology, Bohai University; Department of Electronic Engineering and Materials Science and Technology Research Center, The Chinese University of Hong Kong; School of Energy Science and Engineering, Harbin Institute of Technology; Zhengzhou Advanced Research Institute of Harbin Institute of Technology; Department of Chemical and Materials Engineering, University of Alberta（深圳技术大学未来技术学院; 深圳大学应用科学学院; 渤海大学物理科学与技术学院; 香港理工大学电子工程系及材料科学技术研究中心; 哈尔滨工业大学能源科学与工程学院; 哈尔滨工业大学郑州先进研究院; 阿尔伯塔大学化学与材料工程系）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
HyTopo是一种以笼拓扑为中心的分析框架，通过分层识别与转变网络分析，揭示甲烷水合物生长、成核和分解中路径依赖的笼动力学，连接局部水有序与相变。
AI 中文摘要
解析水合物的形成与分解机制，不仅需要识别类水合物水，还需要识别特定的笼状拓扑结构，无序液态水正是通过这些拓扑结构重组为结晶水合物网络或从中逸出。本文介绍了HyTopo，一种以笼状拓扑为中心的分析框架，它结合了水合物序参量、分层环与笼识别以及笼转变网络分析。基于局部取向关联，HyTopo将水分子分类为液态样、前驱体样、水合物样和冰样环境，并利用这些信息引导对结晶水合物笼和缺陷中间体的高效拓扑搜索。将HyTopo应用于甲烷水合物生长、均相成核和降压诱导分解，结果表明水合物演化受异质且路径依赖的笼动力学控制。在生长过程中，EA-WPU抑制了笼状结构的整体增殖，同时改变了缺陷笼与结晶sI笼之间的平衡。在成核过程中，不完全笼基序主导早期路径，并提供一个结构储备库，其中一小部分稳定的512和51262笼从中形成。水合物分解通过界面塌陷、体相分解和溶解气体析出进行，笼寿命和转变路径强烈依赖于笼拓扑。这些结果表明，HyTopo提供了一条物理可解释且拓扑分辨的途径，将复杂分子模拟中的局部水有序、笼形成、结构缺陷和水合物相变联系起来。
英文摘要
Resolving the formation and dissociation mechanisms of hydrate requires identifying not only hydrate-like water, but also the specific cage topologies by which disordered liquid water reorganizes into, or escapes from, crystalline hydrate networks. Here we introduce HyTopo, a cage-topology-centered analysis framework that combines a hydrate order parameter, hierarchical ring and cage recognition, and cage-transition network analysis. Based on local orientational correlations, HyTopo classifies water molecules into liquid-like, precursor-like, hydrate-like, and ice-like environments, and uses this information to guide efficient topological searches for crystalline hydrate cages and defective intermediates. Applications to methane hydrate growth, homogeneous nucleation, and depressurization-induced dissociation reveal that hydrate evolution is governed by heterogeneous and pathway-dependent cage dynamics. During hydrate growth, EA-WPU suppresses the overall proliferation of cage-like structures while altering the balance between defective cages and crystalline sI cages. During nucleation, incomplete cage motifs dominate the early pathway and provide a structural reservoir from which a small fraction of stable 512 and 51262 cages. Hydrate dissociation proceeds through interfacial collapse, bulk decomposition, and dissolved-gas exsolution, with cage lifetimes and transition pathways strongly dependent on cage topology. These results show that HyTopo provides a physically interpretable and topology-resolved route to connect local water ordering, cage formation, structural defects, and hydrate phase transitions in complex molecular simulations.
