Probing catalyst-support interactions via experiment and theory

通过实验和理论探讨催化剂-载体相互作用

• 批准号: 1800585
• 负责人: Svitlana Pylypenko
• 金额: $ 43.52万
• 依托单位: Colorado School of Mines
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-09-01 至 2022-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1800585&HistoricalAwards=false
• 关键词: Probing; catalyst; support; interactions; via

Industrial catalysts often use precious metal nanoparticles on supporting surfaces to speed up a wide range of chemical reactions that are important in the chemical industry. Carbon-based materials that contains small amounts of nitrogen represent a class of materials for catalyst supports that offer an opportunity to improve the performance of current nanoparticle catalysts. Scientists do not yet understand the fundamental interactions between the nanoparticle catalysts and these nitrogen-doped carbon supports. In this project, the research groups of Dr. Svitlana Pylypenko and Dr. Shubham Vyas of the Colorado School of Mines are using both targeted experiments and chemical computations to improve the interaction between nanoparticle catalysts and these nitrogen-doped carbon supports. Their results may produce less expensive and more earth-abundant catalysts while improving the yield of the desired product (no by-products). Drs. Pylypenko and Vyas are engaged in a multi-level outreach and educational program that involves K-12 students and teachers, as well as undergraduate and graduate researchers. Their recent developments blending experimental and computational approaches are discussed during a distinctive summer field session at the Colorado School of Mines. The insights gained by this research may advance the improve the performance of a wide range of catalytic applications that are vital to the chemical industry and domestic economy.With funding from the Chemical Catalysis Program of the Chemistry Division, Drs. Pylypenko and Vyas are developing a fundamental understanding of catalyst-support interactions by investigating nanoparticle catalysts supported on nitrogen-doped carbons. Despite abundant reports of the advantageous impact of nitrogen functional groups on catalyst nucleation, stability, and, in some instances, catalytic activity, the underlying phenomena associated with catalyst-support interactions for these systems has not yet been elucidated - mainly due to the overall complexity of the system. The team is using a synergistic approach that includes electronic structure calculations, controlled synthesis with targeted composition and morphology, and advanced ex situ and in situ characterization to decrease the cost of metal catalysts, reduce national dependence on precious metals, and lower the environmental impact associated with mining and processing.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.

工业催化剂经常使用贵金属纳米颗粒来支撑表面，以加快化学工业中重要的化学反应。含有少量氮的碳基材料代表了一类催化剂材料支持，这些材料提供了改善当前纳米颗粒催化剂性能的机会。科学家尚不了解纳米颗粒催化剂与这些氮掺杂的碳载体之间的基本相互作用。在这个项目中，科罗拉多州矿业学院的Svitlana Pylypenko博士和Shubham Vyas博士的研究小组都使用有针对性的实验和化学计算来改善纳米粒子催化剂和这些氮气掺杂碳的相互作用。他们的结果可能会产生较便宜的土壤丰富的催化剂，同时提高所需产品的产量（无副产品）。博士。 Pylypenko和Vyas参加了一项多层外展和教育计划，涉及K-12学生和老师，以及本科和研究生研究人员。在科罗拉多州矿业学院的一次独特的夏季野外课程中，讨论了他们最近的发展结合实验和计算方法的发展。这项研究获得的见解可能会提高对化学工业和国内经济至关重要的广泛催化应用的性能。从化学催化计划的资金中，化学催化计划的资金。 Pylypenko和Vyas正在通过研究支持氮掺杂的碳的纳米颗粒催化剂，从而对催化剂 - 支持的相互作用产生基本了解。尽管报道了氮官能团对催化剂成核，稳定性以及在某些情况下的催化活性的有利影响，但与这些系统的催化剂 - 支持相互作用相关的潜在现象尚未阐明 - 主要是由于系统的整体复杂性。 The team is using a synergistic approach that includes electronic structure calculations, controlled synthesis with targeted composition and morphology, and advanced ex situ and in situ characterization to decrease the cost of metal catalysts, reduce national dependence on precious metals, and lower the environmental impact associated with mining and processing.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审查标准。

项目成果

3D Atomic Understanding of Functionalized Carbon Nanostructures for Energy Applications

• DOI: 10.1021/acsanm.9b02360
• 发表时间: 2020-01
• 作者: C. Ngo;Margaret A. Fitzgerald;Michael J. Dzara;Matthew B Strand;D. Diercks;S. Pylypenko

Improved durability and activity of Pt/C catalysts through atomic layer deposition of tungsten nitride and subsequent thermal treatment

• DOI: 10.1016/j.apcatb.2019.05.036
• 发表时间: 2019-10
• 期刊: Applied Catalysis B: Environmental
• 作者: W. McNeary;S. Zaccarine;Annika Lai;Audrey E. Linico;S. Pylypenko;A. Weimer

Characterizing Complex Gas–Solid Interfaces with in Situ Spectroscopy: Oxygen Adsorption Behavior on Fe–N–C Catalysts

• DOI: 10.1021/acs.jpcc.0c05244
• 发表时间: 2020-07
• 期刊: The Journal of Physical Chemistry C
• 作者: Michael J. Dzara;K. Artyushkova;M. Sougrati;C. Ngo;Margaret A. Fitzgerald;A. Serov;B. Zulevi;P. Atanassov;Frédéric Jaouen;S. Pylypenko

X-ray photoelectron spectroscopy and rotating disk electrode measurements of smooth sputtered Fe-N-C films

• DOI: 10.1016/j.apsusc.2020.146012
• 发表时间: 2020-06
• 期刊: Applied Surface Science
• 影响因子: 6.7
• 作者: Yun Xu;Michael J. Dzara;Sadia Kabir;S. Pylypenko;K. Neyerlin;A. Zakutayev

Effects of Graphitic and Pyridinic Nitrogen Defects on Transition Metal Nucleation and Nanoparticle Formation on N-Doped Carbon Supports: Implications for Catalysis

• DOI: 10.1021/acsanm.2c03186
• 发表时间: 2022-09
• 期刊: ACS Applied Nano Materials
• 影响因子: 5.9
• 作者: Vu T. Nguyen;Margaret A. Fitzgerald;Denali Ibbotson;Jayson G. Foster;Michael J. Dzara;S. Zaccarine;Shubham Vyas;S. Pylypenko