Controlling olefin selectivity in electrocatalytically-assisted alkane dehydrogenation

来自俄亥俄州立大学的Umit S.Ozkan教授和合作者Pi Anne Co将在化学催化计划的这一奖项下，在跨学科的背景下，研究控制低碳烷烃电催化辅助脱氢的烯烃选择性的因素。烷烃脱氢的主要挑战是选择性控制。拟议的研究将结合两种不同的战略来解决这个问题。(1)使用电催化反应器方案可以防止碳氢化合物和氧气在气相中接触，从而限制烯烃分子的进一步氧化。同时，电压控制将为阳极提供稳定的氧离子通量，解除了控制非氧化脱水反应的热力学限制。此外，控制氧化物离子向阳极表面的转移可以限制任何以焦炭形式沉积在阳极表面的碳质物质。(2)通过重点研究阳极电催化剂的表面性质，可以调整其活性以促进烷烃的活化，但抑制C-C键的断裂和烯烃的完全氧化。了解结构/功能关系将指导这一调整。为了实现这一目标，联合PIs将结合他们在两个不同领域的专业知识，即多相催化和电化学。这些区域的界面将提供一种独特的方法来解决烷烃脱氢所固有的问题。该工作计划将在迭代过程中结合材料合成、详细表征和电催化活性测量。烷烃活化和脱氢是化学工业中非常重要的反应。烷烃选择性转化为烯烃可能会产生重大的经济影响。这项研究将获得的基本认识可以扩展到其他催化氧化反应，如从低碳烷烃生产醛、酮和醇。该项目的许多成果将被用来加强由共同国际组织开发的一门新的电化学课程的内容。PI与当地两所高中建立了良好的合作伙伴关系，为高中生提供研究实习经验。其中一所学校，哥伦布女子学校，是一所大学预科学校，致力于女孩从婴儿期到十二年级的智力和社交成长。其他侧重于人力资源开发的项目将包括为工程系女生提供的大学暑期迎新活动，以及为九年级女生举办的“能源与环境日”，作为俄亥俄州“Cheme&Amp；You@OSU”夏令营的一部分。PI和共同PI都有让本科生参与研究的现有记录，导致研究出版物的联合作者。

With this award from the Chemical Catalysis Program, Prof. Umit S. Ozkan from the Ohio State Uinversity and co-PI Anne Co will investigate, in an interdisciplinary setting, the factors that control olefin selectivity from the electrocatalytically-assisted dehydrogenation of lower alkanes. The primary challenge in alkane dehydrogenation is selectivity control. The proposed research will combine two different strategies to tackle this problem. (1) Using an electrocatalytic reactor scheme will prevent hydrocarbons and oxygen coming in contact in the gas phase, hence limiting further oxidation of olefin molecules. At the same time, voltage control will provide a steady-flux of oxide ions to the anode, lifting the thermodynamic limitation, which governs non-oxidative dehydration reactions. Also, controlling the transfer of oxide ions to the anode surface could limit any carbonaceous species depositing on the surface in the form of coke. (2) By focusing on the surface properties of the anode electrocatalysts, it will be possible to tailor its activity to promote alkane activation, but inhibit C-C bond cleavage and complete oxidation of olefins. Understanding the structure/function relationship will guide this tailoring. To achieve this goal, the co-PIs will combine their expertise from two different fields, namely heterogeneous catalysis and electrochemistry. The interface of these areas will provide a unique approach to tackle the problems inherent in alkane dehydrogenation. The work plan will combine materials synthesis, detailed characterization and electrocatalytic activity measurements in an iterative process.Alkane activation and dehydrogenation are reactions of great importance to the chemical industry. Selective conversion of alkanes to olefins may have significant economic impact. The fundamental understanding which will be acquired in this study can be extended to other catalytic oxidation reactions such as production of aldehydes, ketones and alcohols from lower alkanes. Many of the results from this project will be used to enhance the contents of a new course on electrochemistry, developed by the co-PI. The PI has well-established partnerships with two local high schools to provide research internship experience to senior high school students. One of the schools, Columbus School for Girls, is a college preparatory school dedicated to girls' intellectual and social growth from infancy to the twelfth grade. Other programs that focus on human resource development will include College of Engineering Summer Orientation for Female Engineering Freshmen and "Energy and Environment Day" for ninth grade girls as part of a "CheME & YOU @OSU" summer camp at Ohio. Both PI and co-PI have an existing track record of involving undergraduate students in hands on research, leading to co-authorship in research publications.