Development of Pd Alloy Membranes for Ultrapure Hydrogen Production

用于超纯氢气生产的钯合金膜的开发

• 批准号: 1033804
• 负责人: James Miller
• 金额: $ 30万
• 依托单位: Carnegie-Mellon University
• 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: 2010-09-01 至 2013-12-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1033804&HistoricalAwards=false
• 关键词: Development; Pd; Alloy; Membranes; Ultrapure

Multicomponent alloy materials are used in a variety of applications in which surface properties are critical. For Pd-based alloys used as dense metal membranes in hydrogen purification processes, critical surface properties include the ability of the alloy surface to dissociate H2 and its ability to resist contamination. A fundamental alloy characteristic that can influence both of these properties is surface segregation, the propensity of the alloy's surface composition to differ from its bulk composition. The proposed effort will develop and apply a novel, high-throughput methodology for fundamental study of these surface properties in Pd100-x-yAgxRuy and Pd100-x-yAgxCuy alloys. This approach will enable measurement of segregation, H2 dissociation kinetics, and sulfur poisoning across continuous regions of alloy composition space, providing an unprecedented and comprehensive understanding of how these surface properties depend on composition. One of the challenges inherent in the study of multicomponent materials is that of understanding their properties over a wide range of composition space without the need to prepare and characterize a prohibitively large set of discrete, fixed-composition samples. For efficient study of alloy surfaces, the PIs have recently developed two unique tools that will serve as the basis for the proposed investigation. The first is a deposition source for preparation of Composition Spread Alloy Films (CSAFs), such as Pd100-x-yAgxRuy, with lateral gradients in composition across their surfaces, thus exposing all possible alloy compositions on a single compact (~1 cm2) substrate. The second tool is a 10x10 multichannel microreactor for spatially resolved measurement of reaction kinetics on CSAF surfaces. In the proposed research, these tools will be combined with spatially resolved surface analysis techniques to deliver a fundamental understanding of the composition dependence of a number of alloy surface properties that are critical to the performance of dense metal hydrogen separation membranes. The tools and methods for preparation and characterization of CSAFs that are developed and refined during the proposed research program will be applied broadly to the study of alloy properties far beyond those relevant to hydrogen purification membranes. Highthroughput study of alloy hardness, corrosion resistance, catalytic activity for fuels conversion reactions, etc., will generate comprehensive data sets across all possible compositions for a nearlimitless number of binary, ternary and even higher order alloys. The proposed work will train students in the application of high-throughput approaches to a wide variety of problems in alloy materials science. Collaborations with Universidad Nacional del Litoral in Santa Fe, Argentina and the Department of Energy's National Energy Technology Laboratory will give students opportunities to work with world-class scientists outside Carnegie Mellon; we plan to pursue separate funding that would support student travel to work in Argentina. Students from Argentina will also benefit from their exposure to this research and their interactions with Carnegie Mellon researchers. The results of the proposed work will be disseminated to the scientific community through publications and presentations at national meetings. Beyond the research impact of the proposed work, the PIs are very active in the research community; they serve several professional organizations in various capacities, including organization of research symposia on topics related to high-throughput catalysis and surface science. They are also active in service to professional student organizations.

多组分合金材料用于各种表面性能至关重要的应用中。对于在氢气净化过程中用作致密金属膜的pd基合金，关键的表面性能包括合金表面解离H2的能力和抗污染的能力。影响这两种性能的合金的一个基本特性是表面偏析，即合金的表面成分与其本体成分不同的倾向。提出的努力将开发和应用一种新的、高通量的方法来研究Pd100-x-yAgxRuy和Pd100-x-yAgxCuy合金的这些表面特性。这种方法将能够测量合金成分空间连续区域的偏析、H2解离动力学和硫中毒，为这些表面特性如何依赖于成分提供前所未有的全面理解。多组分材料研究中固有的挑战之一是，在不需要制备和表征大量离散的固定组分样品的情况下，在广泛的组成空间中理解它们的性质。为了有效地研究合金表面，pi最近开发了两种独特的工具，将作为拟议研究的基础。第一种是用于制备成分扩散合金薄膜（csas）的沉积源，例如Pd100-x-yAgxRuy，其表面的成分具有横向梯度，从而在单个致密（~1 cm2）衬底上暴露所有可能的合金成分。第二个工具是一个10x10的多通道微反应器，用于CSAF表面上的反应动力学的空间分辨测量。在拟议的研究中，这些工具将与空间分辨表面分析技术相结合，以提供对许多合金表面特性的组成依赖性的基本理解，这些特性对致密金属氢分离膜的性能至关重要。在本研究项目中开发和完善的csaf制备和表征工具和方法将广泛应用于合金性能的研究，远远超出与氢净化膜相关的研究。对合金硬度、耐腐蚀性、燃料转化反应的催化活性等的高通量研究，将为几乎无限数量的二元、三元甚至更高阶合金生成所有可能成分的综合数据集。建议的工作将训练学生应用高通量方法来解决合金材料科学中的各种问题。与阿根廷圣达菲国家沿海大学和能源部国家能源技术实验室的合作将使学生有机会与卡内基梅隆大学以外的世界级科学家一起工作；我们计划寻求单独的资金支持学生去阿根廷工作。来自阿根廷的学生也将受益于他们对这项研究的接触以及他们与卡内基梅隆大学研究人员的互动。拟议工作的结果将通过出版物和在国家会议上的介绍向科学界传播。除了拟议工作的研究影响之外，pi在研究界非常活跃；他们以不同的身份为几个专业组织服务，包括组织有关高通量催化和表面科学的研究专题讨论会。他们还积极为专业学生组织服务。