Collaborative Research: SusChEM: Mechanistic origins of synergetic effects in plasma catalysis

合作研究：SusChEM：等离子体催化协同效应的机制起源

• 批准号: 1703439
• 负责人: Peter Bruggeman
• 金额: $ 20万
• 依托单位: University of Minnesota-Twin Cities
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2017
• 资助国家: 美国
• 起止时间: 2017-08-01 至 2022-05-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1703439&HistoricalAwards=false
• 关键词: Collaborative; Research; SusChEM; Mechanistic; origins

1703211 / 1703439PI: Oehrlein, Gottlieb S. / Bruggeman, Peter J. Institution: University of Maryland College Park / University of Minnesota-Twin CitiesThe proposed 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 proposed 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.

1703211 / 1703439PI：Oehrlein, Gottlieb S. / Bruggeman, Peter J. 机构：马里兰大学学院公园分校/明尼苏达大学双城分校拟议的合作研究项目旨在使用特征良好的大气压等离子体源来实现良好的控制等离子体与地球上丰富的催化剂的相互作用。使用等离子体活化催化剂对于提高催化系统的效率具有广阔的前景，并在化学和材料合成、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研究等离子体与催化剂产生协同效应的潜在机制。该计划是将等离子体催化协同效应的大小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联系起来。对不同催化剂进行仔细的系统比较可以阐明协同效应的微观起源，并探索热惰性催化剂的潜在等离子体活化作用。该项目可能会导致更好地了解等离子体条件和催化剂的要求，以充分利用等离子体催化剂系统的协同潜力。提出了一项机制研究，旨在提供原子学见解，以揭示负责协同效应的关键机制（ s) 在等离子体-催化剂相互作用期间。本研究将采用铁、镍、钴和铜负载型催化剂（在氧化铝和二氧化硅载体上）。由于不同的电子结构和表面催化机制，这些催化剂的热催化活性差异很大。该研究将重点研究当等离子体-表面相互作用条件发生变化时，氧气/甲烷模型系统催化剂的原子表面修饰。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光度法、紫外线和 X 射线诱导光电子能谱与热解吸相结合，以及傅里叶变换红外光谱。 所提出的方法有可能通过实现最适合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做出革命性的改变。除了培训研究生和本科生外，研究人员还计划为中学生开发等离子体催化课程材料和互动讲座。

项目成果

Tuning plasma parameters to control reactive species fluxes to substrates in the context of plasma catalysis

调整等离子体参数以控制等离子体催化背景下的活性物质通量

• DOI: 10.1088/1361-6463/abe89a
• 发表时间: 2021-05-27
• 期刊: Journal of Physics D: Applied Physics
• 作者: Jingkai Jiang;P. Bruggeman
• 通讯作者: P. Bruggeman

The 2022 Plasma Roadmap: low temperature plasma science and technology

• DOI: 10.1088/1361-6463/ac5e1c
• 发表时间: 2022-07-05
• 期刊: Journal of Physics D: Applied Physics
• 作者: I. Adamovich;S. Agarwal;E. Ahedo;L. Alves;S. Baalrud;N. Babaeva;A. Bogaerts;A. Bourdon;P. Bruggeman;C. Canal;E. H. Choi;S. Coulombe;Z. Donkó;D. Graves;S. Hamaguchi;D. Hegemann;M. Hori;H. Kim;G. Kroesen;M. Kushner;A. Laricchiuta;X. Li;T. Magin;S. Mededovic Thagard;V. Miller;A. Murphy;G. Oehrlein;N. Puač;R. M. Sankaran;S. Samukawa;M. Shiratani;M. Šimek;N. Tarasenko;K. Terashima;E. Thomas Jr;J. Trieschmann;S. Tsikata;M. Turner;I. J. Van der Walt;M. V. D. van de S;en;en;T. von Woedtke
• 通讯作者: T. von Woedtke

Absolute spatially and time‐resolved O, O 3 , and air densities in the effluent of a modulated RF‐driven atmospheric pressure plasma jet obtained by molecular beam mass spectrometry

通过分子束质谱法获得调制 RF 驱动的大气压等离子体射流流出物中的绝对空间和时间分辨 O、O 3 和空气密度

• DOI: 10.1002/ppap.201900163
• 发表时间: 2019-12
• 期刊: Plasma Processes and Polymers
• 影响因子: 3.5
• 作者: Jiang, Jingkai;Luo, Yuchen;Moldgy, Ankit;Aranda Gonzalvo, Yolanda;Bruggeman, Peter J.
• 通讯作者: Bruggeman, Peter J.

Investigation of the Mechanisms Underpinning Plasma-Catalyst Interaction for the Conversion of Methane to Oxygenates

研究甲烷转化为含氧化合物的等离子体-催化剂相互作用的机制

• DOI: 10.1007/s11090-022-10251-5
• 发表时间: 2022-07
• 期刊: Plasma Chemistry and Plasma Processing
• 影响因子: 3.6
• 作者: Jiang, Jingkai;Bruggeman, Peter J.
• 通讯作者: Bruggeman, Peter J.

Characterization of plasma catalytic decomposition of methane: role of atomic O and reaction mechanism

甲烷等离子体催化分解表征：原子O的作用及反应机理

• DOI: 10.1088/1361-6463/ac4728
• 发表时间: 2022-01
• 期刊: Journal of Physics D: Applied Physics
• 作者: Li, Yudong;Jiang, Jingkai;Hinshelwood, Michael;Zhang, Shiqiang;Bruggeman, Peter J;Oehrlein, Gottlieb S
• 通讯作者: Oehrlein, Gottlieb S