NSF/DOE Advanced Combustion Engines: Collaborative Research: GOALI: Understanding NOx SCR Mechanism and Activity on Cu/Chabazite Structures throughout the Catalyst Life Cycle

NSF/DOE 先进内燃机：合作研究：GOALI：了解 NOx SCR 机制以及整个催化剂生命周期中铜/菱沸石结构的活性

• 批准号: 1258715
• 负责人: Fabio Ribeiro
• 金额: $ 84.38万
• 依托单位: Purdue University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2013
• 资助国家: 美国
• 起止时间: 2013-09-15 至 2016-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1258715&HistoricalAwards=false
• 关键词: NSF; DOE; Advanced; Combustion; Engines

ABSTRACT#1258715 - Fabio Ribeiro#1258690 - William Schneider#1258717 - Jean-Sabin McEwenThe lack of a practical and cost-effective lean NOx aftertreatment is the major obstacle to the widespread adoption of fuel-efficient diesel and lean-burn gasoline engines for transportation. Increasingly stringent NOx emissions standards demand that NOx conversion to N2 reach or exceed 90% averaged over standard drive cycles, and even higher instantaneous conversions to compensate for cold startup and transient operation. These high conversions are very difficult to achieve under lean conditions, in which NOx must compete with an overwhelming excess of O2 for a limited amount of reductant. Lean NOx traps can achieve the necessary NOx conversion efficiencies, but have many operational and cost issues in their current forms. NOx selective catalytic reduction (SCR) provides a much more satisfactory solution to lean NOx aftertreatment. In this approach the usual converter catalyst is replaced with a catalyst that promotes reaction of NOx with a reductant, such as urea, NH3, or hydrocarbons, to produce N2 selectively over the competing reactions of reductant with O2.The selective catalytic reduction with ammonia on Cu-exchanged chabazite zeolites is the state-of-the-art for lean NOx reduction and enables access to the fuel efficiency of lean burn engines. Although these materials are used commercially in a small segment of the transportation market, their structure and catalytic behavior changes in unpredictable ways as they respond to varying SCR conditions and in particular as they accumulate deactivating sulfur species. Real-world application of these catalysts at Cummins reveals that their performance at low temperatures is diminished in ways not explained by previously published aging mechanisms. The primary obstacle to the rational improvement and effective application of NOx SCR catalysts is the lack of a firm fundamental understanding of the underlying catalyst structure and catalytic chemistry.An approach to filling this knowledge gap to lead to maximum SCR catalyst performance has been proposed in response to the joint National Science Foundation and Department of Energy solicitation on Advanced Combustion Engines. The joint Agency award is made through the NSF Chemical, Bioengineering, Environmental and Transport Systems Division and its Catalysis & Biocatalysis Program to a multi-disciplined team made up of Professors Fabio H. Ribeiro, W. Nicholas Delgass, and Rajamani Gounder at Purdue University; Prof. Jean-Sabin McEwen at Washington State University; and Prof. William F. Schneider at University of Notre Dame; Dr. Jeffrey T. Miller, Argonne National Laboratory; Dr. Charles H. F. Peden, Pacific Northwest National Laboratory; and Dr. Aleksey Yezerets, Cummins Inc.NSF GOALI support is also provided to this team that has many years of combined industrial, National Laboratory and academic experience in NOx catalysis and catalysis science and a proven record of successful collaboration.To dramatically improve the present catalyst materials, to optimize engine efficiency within emission constraints, and to circumvent deactivation, an atomic and molecularly detailed model of catalyst performance under all operating conditions and throughout the life cycle is essential. This team brings world-class excellence in the variety of experimental and theoretical disciplines that must be combined to reach the atomic-level understanding of the dynamic chemical and catalytic properties of this reaction system, which will form the basis of a predictive model for this SCR catalyst system and for further catalyst system improvements. Though the students working on this project will specialize in particular aspects of the research, frequent teleconferences with the entire team and groups traveling to the National Labs to do specialized experiments will provide broad experience and direct exposure to the importance of the interplay between various experiments and molecular theory at the frontier of catalysis research. Thus, this multi-institutional and diverse team will prepare graduate students and postdocs to operate at the highest levels in application of catalysis to the solution of energy efficiency and environmental problems. It will also provide career-defining educational opportunities to high school and undergraduate students. For high school students and educators, Purdue has already developed a hands-on presentation to interest students in science and engineering. The PIs intend to add the molecular view of this work to that presentation and deliver lectures to high schools across Indiana and to bring this view to the many science and engineering camps that run at Purdue and Notre Dame during the summer. Undergraduates working in the university research groups and in industrial internships at Cummins will also benefit from the breadth of scientific exposure and the unique approach that connects detailed fundamental understanding to the solution of important practical problems.

摘要＃1258715-Fabio Ribeiro＃1258690-William Schneider＃1258717-Jean-Sabin McEwenthe缺乏实用且具有成本效益的精益NOX后处理后的主要障碍，这是燃油效率高效柴油和精益燃气机进行运输的广泛采用。越来越严格的NOX排放标准要求NOX转换为N2或超过90％的标准驱动周期，甚至更高的瞬时转换以补偿冷启动和瞬态操作。在精益条件下，这些高转化率很难实现，在这种条件下，NOX必须与少量的还原量与压倒性的O2竞争。精益NOX陷阱可以达到必要的NOX转换效率，但在当前形式中具有许多运营和成本问题。 NOx选择性催化减少（SCR）为精益NOX后处理提供了更令人满意的解决方案。 In this approach the usual converter catalyst is replaced with a catalyst that promotes reaction of NOx with a reductant, such as urea, NH3, or hydrocarbons, to produce N2 selectively over the competing reactions of reductant with O2.The selective catalytic reduction with ammonia on Cu-exchanged chabazite zeolites is the state-of-the-art for lean NOx reduction and enables access to the fuel efficiency of瘦发动机。尽管这些材料在运输市场的一小部分中商业使用，但它们的结构和催化行为在反应不同的SCR条件时，以不可预测的方式变化，尤其是在积累失活的硫种类时。这些催化剂在康明斯的现实应用表明，它们在低温下的性能以先前发表的老化机制无法解释的方式降低。 NOX SCR催化剂的合理改进和有效应用的主要障碍是缺乏对基础催化剂结构和催化化学的坚定理解。填补这一知识差距以响应最高的SCR催化剂性能，以响应国民科学基金会和高级燃烧机构的能源局部，提出了最大的SCR催化剂表现。联合机构奖是通过NSF化学，生物工程，环境和运输系统部及其催化与生物催化计划的，由由Fabio H. Ribeiro教授，W。NicholasDelgass和Rajamani Gounder At Purdue University组成的多学科团队；华盛顿州立大学Jean-Sabin McEwen教授；巴黎圣母院的威廉·施耐德（William F. Schneider）教授； Argonne国家实验室的Jeffrey T. Miller博士；太平洋西北国家实验室的查尔斯·H·F·佩登博士；以及Aleksey Yezerets博士，康明斯Inc.NSF攻击支持，该团队在NOX催化和催化学科学方面拥有多年的工业，国家实验室和学术经验多年，并获得了成功的协作记录，以极大地改善目前的催化剂材料，以优化发动机在发动机效率上，并在发动机上进行融合，并构成了型号的型号，并构建了型号的型号，并构成了型号的DEACTIVENTIVS，并构成了型号的型号。在所有操作条件下以及整个生命周期下的表现至关重要。该团队在必须合并的实验和理论学科中带来了世界一流的卓越，以达到对该反应系统动态化学和催化特性的原子级别的理解，这将构成该SCR催化剂系统的预测模型的基础，以及进一步的催化剂系统的改进。尽管从事该项目的学生将专门研究研究的特定方面，但与整个团队和前往国家实验室进行专业实验的小组的频繁电视会议将提供广泛的经验，并直接暴露于催化研究领域的各种实验与分子理论之间相互作用的重要性。因此，这个多机构和多样化的团队将为研究生和博士后做好准备，以最高水平的催化解决能源效率和环境问题的解决方案。它还将为高中和本科生提供职业定义的教育机会。 对于高中生和教育者来说，普渡大学已经开发了动手演讲，以使科学和工程学的学生感兴趣。 PIS打算将这项工作的分子观点添加到该演讲中，并向印第安纳州的高中提供演讲，并将这种观点带入夏季在Purdue和Notre Dame上经营的许多科学和工程营。 在大学研究小组和康明斯的工业实习工作的大学生也将受益于科学曝光的广度以及将详细的基本理解与解决重要实际问题解决的独特方法。