Understanding and Exploiting the Favorable Role of Non-Stoichiometric Oxygen in Bulk Metal Oxide Catalyzed Partial Oxidation of Light Alkanes

了解和利用非化学计量氧在块体金属氧化物催化轻质烷烃部分氧化中的有利作用

基本信息

批准号：
2128846
负责人：
Praveen Bollini
金额：
$ 49.98万
依托单位：
University of Houston
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2022
资助国家：
美国
起止时间：
2022-02-01 至 2025-01-31
项目状态：
未结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=2128846&HistoricalAwards=false
关键词：
Understanding Exploiting Favorable Role Non

项目摘要

Our Nation’s transition to clean energy requires more efficient utilization of fossil fuels combined with a transition to sustainable or biorenewable fuels generated through alternative energy sources such electricity produced from solar or wind energy. The current chemical market relies heavily on ethene – produced from the steam cracking of ethane (from natural gas) - to manufacture a wide range of commodity chemicals. Steam cracking is an energy-intensive process. The project explores an alternative, less energy-intensive, process for ethene manufacture via the oxidative dehydrogenation of ethane (ODHE). Controlled introduction of oxygen – in ways that promote ethene production without deeper oxidation to waste products such as carbon monoxide (CO) and carbon dioxide (CO2) – has been a major impediment to the commercial introduction of ODHE technology. The project addresses this technology gap by exploring a novel catalytic approach for enhancing ethene production while decreasing energy consumption. New catalyst synthesis techniques will be combined with reaction engineering concepts to achieve optimal supply of oxygen. In addition to facilitating the clean energy transition, the project includes educational and outreach efforts that raise awareness of the need for clean energy as related to carbon emissions and climate impact, while also training future scientists and engineers. Introduction of excess, non-stoichiometric oxygen in light-alkane ODH, while favorable for producing exothermicity and lowering the reaction temperature, has traditionally been avoided due to lower olefin selectivity associated with production of CO and CO2. The project seeks a paradigm shift in the study and design of bulk metal oxide catalysts by evidencing and exploiting a potentially favorable role of oxygen present in excess of that stipulated by metal oxide catalyst stoichiometry. Novel methods for assessing active site requirements on oxide surfaces, involving a range of kinetic, isotopic, and spectroscopic tools to assess the mechanistic function of non-stoichiometric oxygen, will be combined with advanced synthetic strategies for manipulating the catalytic function of surface oxygen moieties through control over dopant distribution and crystal habit. This synergistic approach - combining mechanistic investigations and advanced crystallization techniques such as molten salt syntheses - although applied specifically to nickel oxide catalyzed ODHE, may prove broadly applicable to high temperature catalytic partial oxidation reactions of industrial importance. Catalysts developed as part of the proposed work could form the basis for an inexpensive, energy-efficient route to producing ethene due to significantly lower operation temperatures compared to conventional processes. The investigators will use the findings of these studies in graduate-level courses at their institution, while continuing on-going STEM outreach activities in the Houston area including UH Energy Day and Chevron Girls Engineering the Future Day, providing high school students with hands-on research experience (Project ACS SEED), and mentoring undergraduate researchers.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

我们国家向清洁能源的过渡需要更有效地利用化石燃料，并结合通过通过太阳能或风能产生的替代能源产生的替代能源产生的可持续或生物生物燃料的过渡。当前的化学市场在很大程度上依赖于乙烯（由Samene的蒸汽破裂（从天然气）生产）来生产广泛的商品化学品。蒸汽破裂是一个能源密集型过程。该项目通过相同（ODHE）的氧化物脱氢作用探索了乙烯生产的替代性，能源密集型的过程。氧的受控引入 - 以促进乙烯生产而没有对废物产物（例如一氧化碳（CO）和二氧化碳（CO2））进行更深入的氧化的方式，一直是ODHE技术商业引入的主要障碍。该项目通过探索一种增强乙烯生产的新型催化方法，同时减少能源消耗，以解决这一技术差距。新的催化剂合成技术将与反应工程概念相结合，以实现最佳的氧气供应。除了支持清洁能源过渡外，该项目还包括教育和外展工作，这些工作提高了人们对与碳排放和气候影响有关的清洁能源的认识，同时还培训未来的科学家和工程师。由于与CO和CO2的产生相关的较低的烯烃选择性，传统上避免了引入轻质烷烃ODH中过量的非化学计量氧，但有利于产生放热和降低反应温度。该项目通过探测和利用超过金属氧化物催化剂化学测定法所定义的氧气的潜在有利作用来寻求散装金属氧化物催化剂的研究和设计范式转移。评估氧化物表面上有效位点需求的新方法，涉及一系列的动力学，同位素和光谱工具评估非化学计量氧的机械功能，将与先进的合成策略相结合，以操纵通过对照组分和结晶的习惯，可以通过对照组分进行对照组合的表面氧气的催化功能来操纵表面氧气的催化功能。这种协同方法 - 将机械研究和晚期结晶技术（例如熔融盐合成）结合使用 - 尽管专门用于氧化镍催化的ODHE，但可能广泛适用于工业重要性的高温催化部分氧化反应。作为拟议工作的一部分而开发的催化剂可能是与常规过程相比，由于操作温度明显较低，因此生产乙烯的廉价，产生乙烯的途径可能是基础。调查人员将在其机构的研究生水平课程中使用这些研究结果，同时继续在休斯敦地区进行的持续的STEM外展活动，包括UH Energy Day和Chevron Girls在未来的一天中工程，为高中生提供动手的研究经验（Project Acs Acs Seed）（项目ACS种子），并通过Infornally Inforthartifient of Internitional的宣言，并以此为基础。更广泛的影响审查标准。