Elucidating the impact of carbon nanoparticles and surfaces on gas hydrates and developing machine learning kinetic models

气体或笼形水合物是由水作为许多原子和分子客体（诸如氢、氙、氮、二氧化碳和硫化氢等）的主体形成的非化学计量的结晶包合化合物。天然气水合物在与能源有关的广泛人类活动中引起人们的兴趣，特别是在减轻碳氢化合物生产、加工和运输设施中水合物形成的风险方面。此外，人们对开发新的能源效率技术，如二氧化碳捕获、海水淡化、天然气和氢储存的兴趣越来越大。地球上的甲烷水合物也是一种潜在的正反馈，可以加剧气候变化驱动的现象。拟议研究计划的长期目标是促进我们对天然气水合物的基本认识。了解有利于气体水合物形成的热力学条件和影响动力学的因素，是设计设施和工艺以减轻和管理水合物风险以及开发用于能源、环境和其他应用的气体水合物技术所必需的。此外，我们的目标也是了解如何在可持续的工艺设计框架内将这些知识适当地整合到基于水合物的技术中。 在这个提议中，我们的目标是确定悬浮的碳纳米管，二氧化硅纳米颗粒和纤维素纳米晶体对气体水合物成核和晶体生长的影响。这项工作将在定制的高压搅拌反应器（结晶器）中进行气/液结晶实验以及高压量热法。将采用统计学显著性检验来确定是否存在效应。有必要核对报告，这将通过使用统计显著性检验来完成。此外，我们的目标是探索机制，碳纳米管和纤维素纤维表面影响水合物的形成在分子水平上通过开发一个分子动力学（MD）模拟框架。这项工作建立在我们以前的MD模拟工作，显示了二氧化硅表面如何影响气体水合物的形成和分解。这项工作得到了以前的发现赠款计划的支持。我们还旨在开发基于机器学习的新一代水合物动力学模型。这项工作建立在我们在参数估计和优化方面的工作和专业知识的基础上。新模型将被集成到基于气体水合物的工艺中，以描述工业规模的结晶器。在这种整合之后，我们的目标是开发一种基于热力学的通用方法来评估这些技术的能源效率。还将评估这些技术的技术就绪程度。拟议的研究将由两名博士生和两名硕士生进行。五名本科生也将参与这项研究。

Gas or clathrate hydrates are non-stoichiometric crystalline inclusion compounds formed by water acting as a host to many atomic and molecular guests such as hydrogen, xenon, nitrogen, carbon dioxide, and hydrogen sulfide among others. Gas hydrates are of interest in a broad spectrum of human activities related to energy, especially to mitigate the risk of hydrate formation in hydrocarbon production, processing and transportation facilities. In addition, there is a growing interest for the development of new energy efficient technologies such as carbon dioxide capture, seawater desalination, natural gas and hydrogen storage. The earth's methane hydrates are also of interest as potential positive feedback to intensify climate change driven phenomena. The long-term goal of the proposed research program is to advance our fundamental understanding of gas hydrates. Understanding the thermodynamic conditions that favour the formation of gas hydrates and the factors affecting the kinetics is required for the design of facilities and processes to mitigate and manage the risk of hydrates and to develop gas hydrate technologies for energy, environmental and other applications. Moreover, our goal is also to understand how to properly integrate such knowledge into hydrate-based technologies within a sustainable process design framework.    In this proposal, we aim to determine the impact of suspended carbon nanotubes, silica nanoparticles and cellulose nanocrystals on gas hydrate nucleation and crystal growth. This work will be done with gas/liquid crystallization experiments in custom-made high pressure stirred reactors (crystallizers) as well as with high pressure calorimetry. Statistical tests of significance will be employed to decide whether there is an effect or not. There is a need to reconcile reports and this will be done by using statistical tests of significance. Moreover, we aim to probe the mechanism by which carbon nanotube and cellulosic nanocrystal surfaces influence hydrate formation at the molecular level by developing a molecular dynamics (MD) simulation framework. This effort builds on our previous MD simulation work which showed how silica surfaces influence gas hydrate formation and dissociation. That work was supported by a previous Discovery grants program. We also aim to develop a new generation of hydrate kinetic models based on machine learning. This effort builds on our work and expertise in parameter estimation and optimization. The new models will be integrated into gas hydrate-based processes to describe industrial scale crystallizers. Following this integration, we aim to develop a generalized method based on thermodynamics to assess the energy efficiency of these technologies. The technology readiness level of the technologies will also be assessed. The proposed research will be carried by two Doctoral and two Masters students. Five undergraduate students will also be involved in the research.