The Preparation and Characterization of Well-Dispersed Copper/Carbon Systems for Use as Selective Hydrogenation and Nitrous-Oxide Decomposition Catalyst

用作选择性加氢和一氧化二氮分解催化剂的分散良好的铜/碳体系的制备和表征

• 批准号: 9415335
• 负责人: M. Albert Vannice
• 金额: $ 51.58万
• 依托单位: Pennsylvania State Univ University Park
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 1994
• 资助国家: 美国
• 起止时间: 1994-08-15 至 1999-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=9415335&HistoricalAwards=false
• 关键词: Preparation; Characterization; Well; Dispersed; Copper

ABSTRACT CTS-9415335 M. Albert Vannice Copper crystallites dispersed on three allotropic forms of carbon are prepared, characterized, and examined as catalysts for selective hydrogenation of conjugated systems and decomposition of nitrous oxide. Both very small and large copper particles are placed on high-surface-area graphitized carbon fibers, diamond films, and activated amorphous carbon. The influence of pretreatment on the size, morphology, and chemical state of the copper particles is investigated. Characterization is accomplished using controlled-atmosphere electron microscopy (CAEM), high-resolution transmission electron microscopy, chemisorption, X-ray diffraction, diffuse-reflectance Fourier-transform infrared spectroscopy (DRIFTS), electron spin resonance (ESR), and copper-63 solid-state nuclear magnetic resonance. Microwave techniques to measure the electron ability and conductivity of carbon are used to guage the effect of pretreatment on the electrical properties of the three forms of carbon and the influence of small adsorbed molecules. Test reactions include hydrogenation of furfural to furfurol, hydrogenation of crontonaldehyde to crotyl alcohol, and decomposition of nitrous oxide. A commercial copper-chromite catalyst is studied for comparison. The effects of copper crystallite size and type of carbon support on specific activity are determined. These new copper/carbon catalyst have three potentially significant industrial applications: replacement of commercial copper-chromite catalyst because spent chromite catalysts are a hazardous waste and hen e a disposal problem; development of new copper catalysts to reduce unwanted byproducts from selective hydrogenations; and decomposition of nitrous oxide, a greenhouse gas, produced as a byproduct in certain industrial processes such as production of adipic acid, a precursor of nylon. This award is part of the Environmentally Benign Chemical Synthesis and Processing Initiative. ***

摘要CTS-9415335 M.阿尔伯特·万尼斯 铜微晶分散在三个同素异形体形式的碳的制备，其特征在于，并检查作为催化剂的共轭系统的选择性氢化和分解一氧化二氮。 非常小和大的铜颗粒都被放置在高表面积的石墨化碳纤维、金刚石膜和活性无定形碳上。 研究了预处理对铜颗粒尺寸、形貌和化学状态的影响。 使用可控气氛电子显微镜（CAEM），高分辨率透射电子显微镜，化学吸附，X射线衍射，漫反射傅里叶变换红外光谱（DRIFTS），电子自旋共振（ESR），和铜-63固态核磁共振表征完成。 利用微波技术测量了碳的电子能力和电导率，以衡量预处理对三种形态碳的电性能的影响以及吸附小分子的影响。 试验反应包括糠醛加氢生成糠醛，巴豆醛加氢生成巴豆醇，以及一氧化二氮的分解。 研究了一种工业铜-亚铬酸盐催化剂以作比较。 测定了铜晶粒尺寸和碳载体类型对比活度的影响。 这些新的铜/碳催化剂具有三个潜在的重要工业应用：替代商业铜-铬铁矿催化剂，因为废铬铁矿催化剂是危险废物并且因此存在处置问题;开发新的铜催化剂以减少来自选择性氢化的不需要的副产物;以及分解一氧化二氮，一种温室气体，在某些工业过程中作为副产品产生，例如己二酸的生产，尼龙的前身。 该奖项是环境友好化学合成和加工倡议的一部分。 ***