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

1703211/1703439PI：Oehrlein，Gottlieb S./Bruggeman，Peter J.合作研究项目旨在使用特性良好的大气压等离子体源，使等离子体与富含地球的催化剂能够很好地控制相互作用。利用等离子体活化催化剂在提高催化体系效率方面具有很大的潜力，在化学和材料合成、环境修复和能源生产等广泛行业中具有潜在的应用前景。该项目的首要目标是调查导致等离子体与催化剂协同作用的潜在机制。该计划将等离子体催化协同效应的大小(S)与入射反应物种通量以及催化剂表面性质和表面电子结构的变化相关联。对不同催化剂进行仔细的系统比较，可能会阐明协同效应的微观来源，并探索热失活催化剂的潜在等离子体活化。该项目可能有助于更好地了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。提出了一项旨在提供原子学见解的机理研究，旨在揭示等离子体-催化剂相互作用中协同效应的关键机理(S)。本研究将使用铁、镍、钴和铜负载的催化剂(氧化铝和二氧化硅载体)。由于不同的电子结构和表面催化机理，这些催化剂的热催化活性有很大的差异。本研究将重点研究等离子体-表面相互作用条件改变时，氧/甲烷模型催化剂的原子化表面改性。这将包括这些表面变化对形成的产品及其形成速度的影响。气相的表征将通过分子束质谱仪和双光子激光诱导荧光来实现。表面表征将包括椭偏法、紫外光和x射线诱导的光电子能谱与热脱附，以及傅里叶变换红外光谱。建议的方法有可能对当前最先进的技术进行变革性的改变，使催化剂的机械信息设计成为理想的适合等离子体催化剂协同作用的设计。除了培训研究生和本科生外，研究人员还计划开发有关等离子体催化的课程材料，并为中学生提供互动讲座。

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.