Collaborative Research: SusChEM: Mechanistic origins of synergistic effects in plasma-catalysis

1703211 /1703439 PI：Oehrlein，Gottlieb S. 作者：Peter J. 该合作研究项目旨在使用一种特征良好的大气压等离子体源，使等离子体与地球上丰富的催化剂之间的相互作用得到良好的控制。使用等离子体的催化剂的活化对于提高催化系统的效率具有很大的希望，其在广泛的工业中具有潜在的应用，包括化学和材料合成、环境修复和能源产生。该项目的首要目标是研究等离子体与催化剂协同效应的潜在机制。计划是将等离子体催化协同效应的大小与入射反应性物质通量、沿着催化剂表面性质和表面电子结构的变化相关联。仔细系统的比较不同的催化剂可以阐明的协同效应的微观起源，并探讨潜在的热惰性催化剂的等离子体活化。该项目将有助于更好地理解等离子体条件和催化剂的要求，以充分发挥等离子体-催化剂系统的协同潜力。铁，镍，钴，铜负载催化剂（氧化铝和二氧化硅载体）将在这项研究中。这些催化剂由于电子结构和表面催化机理的不同，其热催化活性有很大差异。调查将集中在研究原子表面改性的催化剂的氧气/甲烷模型系统的等离子体-表面相互作用条件的变化。这将包括这些表面变化对形成的产品及其形成速率的影响。气相表征将通过分子束质谱和双光子激光诱导荧光来实现。表面表征将包括椭圆偏振法、紫外线和X射线诱导的光电子能谱与热脱附相结合，以及傅里叶变换红外光谱。 所提出的方法有可能通过实现理想地适合于等离子体-催化剂协同作用的催化剂的机械知情设计来对当前最先进的技术进行变革性改变。除了培训研究生和本科生，研究人员计划开发等离子体催化课程材料和中学生互动讲座。

1703211 / 1703439PI: Oehrlein, Gottlieb S. / Bruggeman, Peter J. The collaborative research project aims at using a well-characterized atmospheric-pressure plasma source to enable well-controlled interactions of the plasma with earth-abundant catalysts. The activations of catalysts using plasmas holds great promise for increasing the efficiency of catalytic systems with potential applications in a broad spectrum industries, including chemical and materials synthesis, environmental remediation, and energy generation. The overriding goal of the project is to investigate the underlying mechanisms that are responsible for the synergistic effects of plasma with catalysts. The plan is to correlate the magnitude of the plasma catalytic synergistic effect(s) with incident reactive species fluxes, along with changes in catalyst surface properties, and surface electronic structure. A careful systematic comparison of the different catalysts may elucidate the microscopic origins of the synergistic effect and explore potential plasma activation of thermally inactive catalysts. The project may lead to better understanding of the requirements for plasma conditions and catalysts to fully exploit the synergistic potential of plasma-catalyst systems.A mechanistic study is proposed that is aimed at providing atomistic insights to unravel the key mechanisms responsible for the synergistic effect(s) during plasma-catalyst interactions. Iron, nickel, cobalt, and copper supported catalysts (on alumina and silica supports) will be employed in this study. These catalysts vary strongly in thermal catalytic activities due to different electronic structure and surface-catalytic mechanisms. The investigation will be focused on studying atomistic surface modifications of the catalysts for the oxygen/methane model system as the plasma-surface interaction conditions are changed. This will include the impact of these surface changes on the products formed and their formation rates. Gas phase characterization will be achieved by molecular beam mass spectrometry and two-photon laser induced fluorescence. Surface characterization will include ellipsometry, ultra-violet and x-ray induced photoemission spectroscopy coupled with thermal desorption, and Fourier transform infrared spectroscopy. The proposed approach has the potential to make transformative changes to the current state-of-the-art by enabling a mechanistically informed design of catalysts ideally suited for plasma-catalyst synergies. In addition to training graduate and undergraduate students, the investigators plan to develop course material on plasma-catalysis and an interactive lecture for middle school students.