Energy storage by plasma methane decarbonization for CO2-free synthesis of H2 & carbonaceous nanoparticles

通过等离子体甲烷脱碳储能用于无二氧化碳合成氢气

• 批准号: RGPIN-2019-06330
• 负责人: Kholghy, MohammadReza
• 金额: $ 1.97万
• 依托单位: Carleton University
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2020
• 资助国家: 加拿大
• 起止时间: 2020-01-01 至 2021-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=715358
• 关键词: Energy; storage; plasma; methane; decarbonization

The share of natural gas (methane) in Canadian energy portfolio is rapidly increasing which hinders energy decarbonization. Novel processes are needed to use methane recourses with minimal environmental impact. Plasma decomposition is an emerging technology for breaking C-H bonds without direct CO2 emissions to produce hydrogen and carbonaceous nanoparticles. This technology stores electricity in hydrogen and produces valuable carbonaceous nanoparticles used in batteries with minimal, if not zero environmental footprint. With plasma decarbonization, most of the consumed electricity can be recycled from hydrogen and the elemental carbon can be converted to valuable nanoparticles without combustion emissions. This technique has not been widely used because: 1. There is a fundamental lack of understanding regarding the interaction of methane pyrolysis with plasma chemistry. Combustion kinetic models are developed for methane oxidation where only a handful of reactions dominate. However, plasma synthesis operates without oxygen for which other important reaction pathways are active. Such non-oxidative routes have major implications for process design and open possibilities for novel technologies. 2. Knowledge of gas phase synthesis of carbonaceous nanoparticles is limited to a narrow range of flame temperatures. With plasma, this range is extended beyond thermodynamic limitations of combustion and an array of new valuable functional nanoparticles can be made. The non-oxidizing nature of plasma synthesis results in particles with completely different compositions, surface functionalities and optical properties. It is not currently possible to predict how these parameters change with high temperature particle residence time due to gaps in understanding and lack of a predictive framework. This research addresses many of these issues through a multiscale experimental and modeling approach with a focus on the interaction of plasma chemistry with: a) methane pyrolysis kinetics, b) high temperature aerosol dynamics and c) functional properties of carbonaceous nanoparticles. Specifically, we will couple methane and plasma kinetic models with particle simulations to predict species and aerosol measurements in pyrolysis conditions. Then we benchmark predicted particle optical properties needed for laser diagnostics in process control. Finally, with experiments in a modular reactor, we understand how the functional properties of carbonaceous nanoparticles are controlled. The main goal is to reveal how process conditions such as high temperature particle residence time affect particle functional properties and hydrogen production. This research enables Canada to harness the energy of its vast hydrocarbon resources by converting them to hydrogen and functional nanoparticles, i.e. two essential commodities for carbon free energy conversion and storage. It also contributes to developing novel hydrocarbon reforming technologies to reduce emissions.

天然气（甲烷）在加拿大能源组合中的份额正在迅速增加，这阻碍了能源脱碳。需要新的工艺来使用甲烷资源，同时对环境影响最小。等离子体分解是一种新兴技术，可在不直接排放二氧化碳的情况下打破 C-H 键，从而产生氢气和碳质纳米颗粒。该技术将电力储存在氢气中，并生产用于电池的有价值的碳质纳米颗粒，环境足迹即使不是零，也是最小的。通过等离子体脱碳，大部分消耗的电力可以从氢气中回收，元素碳可以转化为有价值的纳米颗粒，而不会产生燃烧排放。该技术尚未得到广泛应用，因为： 1. 对于甲烷热解与等离子体化学的相互作用，人们根本缺乏了解。燃烧动力学模型是针对甲烷氧化而开发的，其中只有少数反应占主导地位。然而，等离子体合成在没有氧气的情况下进行，而其他重要的反应途径也处于活跃状态。这种非氧化途径对工艺设计具有重大影响，并为新技术提供了可能性。 2. 碳质纳米颗粒气相合成的知识仅限于狭窄的火焰温度范围。通过等离子体，该范围超出了燃烧的热力学限制，并且可以制造一系列新的有价值的功能纳米颗粒。等离子体合成的非氧化性质导致颗粒具有完全不同的成分、表面功能和光学性质。由于理解上的差距和缺乏预测框架，目前无法预测这些参数如何随高温颗粒停留时间而变化。 这项研究通过多尺度实验和建模方法解决了其中许多问题，重点关注等离子体化学与以下因素的相互作用：a）甲烷热解动力学，b）高温气溶胶动力学和c）碳质纳米粒子的功能特性。具体来说，我们将甲烷和等离子体动力学模型与粒子模拟结合起来，以预测热解条件下的物种和气溶胶测量。然后，我们对过程控制中激光诊断所需的预测粒子光学特性进行基准测试。最后，通过模块化反应器中的实验，我们了解了如何控制碳质纳米颗粒的功能特性。主要目标是揭示高温颗粒停留时间等工艺条件如何影响颗粒功能特性和氢气生产。 这项研究使加拿大能够利用其丰富的碳氢化合物资源，将其转化为氢气和功能性纳米颗粒，即无碳能源转换和储存的两种重要商品。它还有助于开发新型碳氢化合物重整技术以减少排放。