GOALI: Thermo-catalytic Decomposition of Natural Gas Coupled with Regeneration: Nanostructure Connections and Control

GOALI：天然气热催化分解与再生：纳米结构连接和控制

• 批准号: 2228140
• 负责人: Randy Vander Wal
• 金额: $ 36.89万
• 依托单位: Pennsylvania State Univ University Park
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2022
• 资助国家: 美国
• 起止时间: 2022-10-01 至 2025-09-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2228140&HistoricalAwards=false
• 关键词: GOALI; Thermo; catalytic; Decomposition; Natural

Hydrogen has several present-day uses including fertilizer production, refining, and boosting natural gas combustion for power generation. Presently hydrogen for these uses is generated by steam-methane reforming, an energy intensive process producing considerable carbon dioxide and consuming substantial water. In contrast thermally driven catalytic decomposition of methane can produce clean hydrogen uncontaminated by reforming byproducts. Thermally driven catalytic decomposition produces hydrogen using roughly half the input energy of steam methane reforming. Operating with renewable energy, thermally driven catalytic decomposition could supply hydrogen for power generation and transportation based on hydrogen fuel cells free of carbon dioxide production. Effectively decarbonizing methane by producing solid carbon in addition to clean hydrogen, thermally driven catalytic decomposition can facilitate the transition to the hydrogen economy. This project promotes elementary and high-school engagement in science though summer science camps and after-school demonstrations.Carbon is an ideal catalyst for thermally driven catalytic decomposition given its high temperature stability and resistance to poisoning. Yet its activity declines with reaction time. Surprisingly, deposited carbon nanostructure has not been examined by microscopy nor connected with its initial activity and decline. The project goal is to realize thermally driven catalytic decomposition as a semi-continuous process via coupling thermally driven catalytic decomposition with a regeneration reaction for the carbon serving as catalyst. Thermally driven catalytic decomposition will be conducted using synthetic natural gas representing realistic pipeline mixtures. Regeneration will be conducted by gasification, using carbon dioxide or water, separately or as mixtures. The experimental approach will systematically resolve reaction parameters and their interactions upon thermally driven catalytic decomposition metrics of methane conversion, hydrogen yield and product selectivity and key kinetic metrics: reaction rate, reaction order and activation energy. A similar approach will be applied to regeneration reactions, individually and coupled with thermally driven catalytic decomposition. Reaction rates will be correlated with carbon structure, thereby developing structure-activity relationships specific to both thermally driven catalytic decomposition and regeneration (gasification) reactions. Kinetic models for thermally driven catalytic decomposition and gasification – both resolved by carbon structure, will be developed with experimental input, using an open-source chemical kinetic modeling code. Fundamentally, this study seeks to connect carbon structure and activity as a fundamental metric for thermally driven catalytic decomposition and gasification reactions.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

氢气目前有多种用途，包括化肥生产、精炼和促进天然气燃烧发电。目前，这些用途的氢气是通过蒸汽甲烷重整产生的，这是一种能源密集型过程，会产生大量二氧化碳和大量水。甲烷驱动催化分解可以产生不受重整副产物污染的清洁氢气。热驱动催化分解使用大约蒸汽甲烷重整一半的输入能量。可再生能源，热驱动催化分解可以为基于氢燃料电池的发电和运输提供氢气，不产生二氧化碳。除了清洁氢气之外，热驱动催化分解还可以通过产生固体碳来有效地脱碳甲烷，从而促进向氢气的过渡。该项目通过夏季科学营和课后演示促进中小学生对科学的参与。由于碳具有高温稳定性和耐腐蚀性，因此是热驱动催化分解的理想催化剂。然而，令人惊讶的是，沉积的碳纳米结构并未通过显微镜检查，也没有与其初始活性和下降相关。该项目的目标是通过耦合热驱动来实现热驱动催化分解。催化分解与碳的再生反应将使用代表实际管道混合物的合成天然气进行热驱动催化分解。该实验方法将系统地解决反应参数及其相互作用，包括甲烷转化率、氢气产率和产物选择性的热驱动催化分解指标以及关键动力学指标：反应速率、反应级数和反应速率。类似的方法将单独应用于再生反应，并与热驱动催化分解相结合，反应速率将与碳结构相关，从而开发出针对热驱动催化的结构-活性关系。热驱动催化分解和气化的动力学模型（均由碳结构解决）将使用开源化学动力学建模代码通过实验输入来开发。和活性作为热驱动催化分解和气化反应的基本指标。该奖项反映了 NSF 的法定使命，并通过使用基金会的智力价值和更广泛的影响审查进行评估，被认为值得支持标准。