权益分类	功能权益	普通用户	{{item.name}}会员
{{category.name}}	{{benefitItem.name}}

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.

我国向清洁能源的过渡需要更有效地利用化石燃料，同时过渡到通过太阳能或风能等替代能源产生的可持续或生物可再生燃料。目前的化工市场严重依赖乙烯——由乙烷（来自天然气）的蒸汽裂解产生——来制造各种各样的商品化学品。蒸汽裂解是一个能源密集型的过程。该项目探索了通过乙烷氧化脱氢（ODHE）生产乙烯的替代能源密集型工艺。有控制地引入氧气——以促进乙烯生产而不进一步氧化产生诸如一氧化碳和二氧化碳等废物的方式——一直是ODHE技术商业化引入的主要障碍。该项目通过探索一种新的催化方法来提高乙烯产量，同时降低能源消耗，从而解决了这一技术差距。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。除了促进清洁能源转型外，该项目还包括教育和推广工作，以提高人们对清洁能源的必要性的认识，以减少碳排放和气候影响，同时培训未来的科学家和工程师。在轻烷烃ODH中引入过量的非化学计量氧，虽然有利于产生放热性和降低反应温度，但由于与CO和CO2产生相关的烯烃选择性较低，传统上是避免的。该项目旨在通过证明和利用超过金属氧化物催化剂化学计量学规定的氧气存在的潜在有利作用，从而在散装金属氧化物催化剂的研究和设计中实现范式转变。评估氧化物表面活性位点需求的新方法，包括一系列动力学、同位素和光谱工具来评估非化学计量氧的机制功能，将与先进的合成策略相结合，通过控制掺杂剂分布和晶体习性来操纵表面氧部分的催化功能。这种结合机理研究和熔盐合成等先进结晶技术的协同方法，虽然专门应用于氧化镍催化的ODHE，但可能广泛适用于具有工业重要性的高温催化部分氧化反应。与传统工艺相比，由于操作温度显著降低，作为提议工作的一部分开发的催化剂可以形成廉价、节能的乙烯生产路线的基础。研究人员将把这些研究结果用于他们所在机构的研究生课程，同时继续在休斯敦地区进行STEM外展活动，包括休斯敦大学能源日和雪佛龙女孩工程未来日，为高中生提供实践研究经验（ACS SEED项目），并指导本科生研究人员。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。