SusChEM: Rational Design of High Temperature Water-Gas Shift Catalysts with Non-Toxic Earth-Abundant Elements

该提案旨在了解并重新设计高温水煤气变换(WGS)催化剂，以避免使用铬(一种具有潜在环境和健康风险的元素)。目前，含铬催化剂几乎只用于这一重要的反应，该反应从一氧化碳和水中产生氢气，从而有助于可持续的氢气能源经济。该项目将利用最先进的催化剂表征和机械工具来了解高温水煤气变换反应条件下发生的详细表面反应，然后根据潜在的低成本替代材料的已知特性提出新的配方。这项研究将考察常规和模型的HT-WGS催化剂在反应条件下的体相和表面化学和物理状态。PI有许多最先进的表征工具可供他使用，这些工具应该可以前所未有地深入了解当前基于铬的催化剂发挥作用的机理。然后，他将尝试通过使用一种新的“控制合成”方法来模拟铬的性质，这种方法将用于各种富含地球的候选催化剂材料。对商用含铬催化剂的基本了解应为与含铬催化剂相匹配所需的结构、组成和氧化还原性能提供指导。除了一套光谱工具外，PI还将使用标准的反应性测试方法和同位素标记物种的研究，以详细了解工作催化剂的组成和WGS反应机理。这项拟议的研究如果在所有方面都获得成功，可以改变HT-WGS的工业流程，同时避免与目前使用铬相关的环境和健康问题。该项目还将有助于实现可持续的氢经济，这将改善美国的能源安全，并有助于确保美国化学工业的竞争力。从教育的角度来看，该项目将培养1名研究生和4-6名本科生。此外，PI将继续长期参与利哈伊谷地区的一系列教育外展项目，包括利哈伊大学选择计划，该计划每年将中学女学生带到校园一天，与从事STEM活动的教职员工和学生互动。

The proposal seeks to understand and re-design high-temperature water-gas shift (WGS) catalysts so as to avoid the use of chromium (an element with potential environmental and health risks). Currently, chromium-containing catalysts are used almost exclusively for this important reaction that generates hydrogen from carbon monoxide and water, thereby contributing to a sustainable hydrogen-based energy economy. The project will utilize state-of-the art catalyst characterization and mechanistic tools to understand the detailed surface reactions that occur under high-temperature water-gas shift reaction conditions, and then propose new formulations based on known properties of potential low-cost substitute materials. The study will examine both conventional and model HT-WGS catalysts for both their bulk and surface chemical and physical states under reaction conditions. The PI has many state-of-the-art characterization tools at his disposal that should allow unprecedented insight into the mechanism by which the current chromium-based catalyst functions. He will then attempt to emulate the properties of chromium by using a novel "controlled synthesis" method that will be employed with various earth-abundant candidate catalyst materials. The fundamental understanding obtained on the commercial chromium-containing catalyst should provide guidance on the structure, composition and redox properties needed to match the chromium-containing catalyst. In additional to a suite of spectroscopic tools, the PI will employ standard reactivity testing methods and studies with isotopically labeled species to gain detailed understanding of both the working catalyst composition and the WGS reaction mechanism. The proposed research, if successful in all aspects, could transform the industrial process for HT-WGS while avoiding environmental and health issues associated with the current use of chromium. The project would also contribute to the realization of a sustainable hydrogen economy, which would improve U.S. energy security and help ensure competitiveness of the U.S. chemical industry. From an educational standpoint, the project will train one graduate student and 4-6 undergraduate students. In addition the PI will continue his longstanding involvement in a number of educational outreach programs in the Lehigh Valley area, including the Lehigh University CHOICES program that annually brings middle-school female students to the campus for a day to interact with faculty and students engaged in STEM activities.