EAGER: Electrochemical Reactor for Spontaneous Power Generation and CO2 Capture

EAGER：用于自发发电和二氧化碳捕获的电化学反应器

• 批准号: 1005303
• 负责人: William Mustain
• 金额: $ 9.77万
• 依托单位: University of Connecticut
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2010
• 资助国家: 美国
• 起止时间: 2010-02-15 至 2011-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1005303&HistoricalAwards=false
• 关键词: EAGER; Electrochemical; Reactor; Spontaneous; Power

1005303Mustain The objective of this project is to test the hypotheses that: i) alkali earth oxides with the pyrochlore structure can selectively reduce O2 and atmospheric CO2 to CO3-2 in an alkaline electrochemical reactor; ii) operating the reactor with carbonate anions reduces the degradation of stateof- the-art anion exchange membranes compared with operation on the hydroxide cycle; and iii) H2 and methanol can be electrochemically oxidized on Pt surfaces with carbonate anions. These fundamental discoveries will allow for the development of a room temperature electrochemical reactor operating on the carbonate anionic cycle with reduced cost and increased durability compared to both the proton and hydroxide exchange membrane fuel cells. In addition to producing energy, this cell also acts as a CO2 ?pump? and purification device. The anode effluent CO2 and water can be separated and either utilized in chemical processing or sequestered.In this work, three pyrochlore structured (A2B2O7) oxygen reduction electrocatalysts will be tested: Ca2Pt2O7, Ca2Ru2O7 and Ca2W2O7. A calcium-based oxide was selected due to the known surface basicity of its root oxide, CaO, which will allow for the preferential adsorption of CO2 over H2O on the catalyst surface. The pyrochlore structured oxide avoids common pitfalls of alkali earth oxides, including low electronic conductivity and the formation of surface passivating species. Pt, Ru and W ?B? metals will be investigated because of their ability to activate molecular oxygen in alkaline media. The resulting catalysts will be fully characterized by SEM/EDS, XRD, BET and XPS. Pt electrocatalysts will be investigated at the anode, where two common fuels, H2 and CH3OH, will be oxidized and their kinetics examined. All electrochemical measurements will be conducted in a custom-built three electrode cell. Finally, the chemical stability and ionic conductivity of six commercially available anion exchange membranes will be investigated in the presence of both concentrated KOH and HCO3-/CO3-2.The results will yield information regarding surface adsorption and electron transfer behavior of the cathode oxides, information regarding electrochemical reactor design, specifically the construction, maintenance and stabilization of the electrochemical interface. Also, the PI will use the individual components to construct a laboratory scale, 5 cm2 electrochemical reactor operating on the carbonate cycle and demonstrate its performance under various operating conditions.Broader ImpactsThe educational objective is to establish a teaching and learning chain related to electrochemical science and engineering within the PI?s group at the University of Connecticut. This will: i) involve an undergraduate student in the research activities; ii) train a graduate student; iii) permit hands-on research in the PI?s laboratory for a Hartford Public School secondary school teacher through the NSF-sponsored Joules-Fellows program at the University of Connecticut; and iv) disseminate the scientific advances in archival journals.The research and educational activities will enhance discovery and understanding while promoting teaching, training and learning across multiple levels. Also, the results could have far reaching impact on many important systems including: fuel cells, batteries, heterogeneous transesterfication of oils for biodiesel, electrochemically assisted carbon sequestration, reduction of nitrous oxides in automotive pollution prevention and water treatment and electrolysis. Success in this regard could catalyze a transformative shift in philosophy regarding electrochemical energy generation devices, renew public, private and legislative support for alternative energy technologies and yield a cost-effective, environmentally green energy source with the potential for a net negative CO2 footprint for the 21st century and beyond.

1005303Mustain该项目的目的是测试以下假设：i）具有pyrochlore结构的碱氧化物可以选择性地将O2和大气CO2选择性地降低至碱性电化学反应器中的CO3-2； ii）用碳酸盐阴离子操作反应堆，与氢氧化物周期的运行相比，降低了ART阴离子交换膜的降解； iii）H2和甲醇可以用碳酸盐阴离子的PT表面进行电化学氧化。与质子和氢氧化物交换膜燃料电池相比，这些基本发现将允许在碳酸盐阴离子循环上运行的室温电化学反应器，其成本降​​低和耐用性提高。除了产生能量外，该细胞还充当二氧化碳？和纯化设备。阳极流出的二氧化碳和水可以分离并用于化学加工或隔离。在这项工作中，将测试三个pyrochlore结构化的（A2B2O7）氧还原电催化剂：Ca2PT2O7，Ca2PT2O7，Ca2RU2O7和CA2W2O7。由于其根氧化物CAO的已知表面碱度，选择了基于钙的氧化物，这将允许在催化剂表面上比H2O优先吸附CO2。 pyrochlore结构化的氧化物避免了碱土氧化物的常见陷阱，包括低电子电导率和表面钝化物种的形成。 pt，ru和w？b？由于金属在碱性培养基中激活分子氧的能力，将研究金属。所得的催化剂将充分以SEM/EDS，XRD，BET和XPS为特征。 PT电催化剂将在阳极进行研究，其中两种常见的H2和CH3OH将被氧化并检查其动力学。所有电化学测量将在定制的三个电极电池中进行。最后，将在浓缩的KOH和HCO3-/CO3-2的情况下研究六个商业上可用阴离子交换膜的化学稳定性和离子电导率。结果将产生有关氧化物氧化物的表面吸附和电子传递行为的信息，有关电化学反应器设计的信息，具有电化学反应器设计的信息，具体是构造，维护和稳定性的，构造和稳定性的，稳定性。此外，PI将使用各个组件来构建实验室规模，在碳酸盐周期运行的5 cm2电化学反应器，并在各种操作条件下证明其性能。BROADER的影响，教育目标是建立与康涅狄格大学PI组中与电化学科学和工程相关的教学链。这将是：i）让一名本科生参与研究活动； ii）培训研究生； iii）允许通过康涅狄格大学的NSF赞助的Joules-Fellows计划在PI的实验室进行实践研究； iv）传播档案期刊的科学进步。研究和教育活动将增强发现和理解，同时促进跨多个层次的教学，培训和学习。此外，结果可能会对许多重要系统产生巨大影响，包括：燃料电池，电池，生物柴油油的异质式三层，电化学辅助碳固执，减少一二氮氧化物在预防自动污染和水处理和水处理和电解和电解中。在这方面的成功可能会促进有关电化学能源生成设备，续签公共，私人和立法支持的哲学转变，并对替代能源技术进行支持，并产生具有成本效益的环境绿色能源，并有可能为21世纪及以后带来净负CO2足迹。