CAREER: Nanoparticle Non-Noble Metal Intermetallic Compounds as Tunable Catalysts for Selective Hydrogenation Reactions

职业：纳米颗粒非贵金属金属间化合物作为选择性加氢反应的可调催化剂

• 批准号: 1752063
• 负责人: Siris Laursen
• 金额: $ 50.01万
• 依托单位: University of Tennessee Knoxville
• 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: 2018-03-15 至 2023-02-28
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1752063&HistoricalAwards=false
• 关键词: CAREER; Nanoparticle; Non; Noble; Metal

The project will investigate new, low-cost materials for catalyzing important chemical reactions associated with the refining of petroleum and bio-based materials to produce fuels and a wide range of chemical products. In addition, the project will explore the potential for improving the effectiveness of the catalytic materials by synthesizing them as nanoparticles rather than traditional micron-sized particles. The new materials can be formed through combinations of many different elements, and the study will also develop methods for predicting the best combinations of elements for specific chemical reactions, thereby streamlining the catalyst discovery process and promoting U.S. competitiveness in the fuels and chemicals manufacturing sectors. The project will be linked to educational and outreach efforts that will train the next generation of engineers, and increase public awareness of new energy-efficient technologies such as fuel cells and batteries.Preliminary efforts in the investigator's laboratory have established a working understanding of how supported nanoparticle intermetallic compounds (IMCs) may be synthesized with well-defined bulk and surface compositions. The project will utilize those findings to enable a systematic study of IMC surface chemistry as a function of constituent elements in the selective hydrogenation of unsaturated aldehyde and nitro compounds. Experimental and computational methods will be used to examine the selectivity of C=C, C=O, and N-O activation, dissociation, and hydrogenation as a function of IMC bulk and surface composition and electronic structure information. Synthesis of oxide-supported non-noble metal nanoparticle IMCs will focus on developing clear understanding of the physical phenomena that dictate their bulk and surface composition as a function of element selection, oxide choice, and preparation environment. Formation of the bulk crystal structure of the nanoparticles will be investigated by ex- and in-situ x-ray diffraction and neutron scattering. Complementary high-resolution energy-dispersive x-ray spectroscopy will verify bulk composition and quantify elements not incorporated into the IMC nanoparticles. Surface composition of the IMCs will be analyzed using low energy ion scattering. Diffusion of constituent elements, particle growth, and bulk crystal structure will be analyzed as a function of synthesis variables to produce a complete picture of how well-defined nanoparticle IMCs may be produced. Results of these studies will allow for a general procedure to be developed for the synthesis, characterization, reactivity evaluation, and stability analysis of the IMC catalysts. Beyond the targeted reactions, the project will enable atomic- and electronic-level understanding of how nanoparticle IMC catalysis can be controlled and widely utilized in chemical transformations important to the field of heterogeneous catalysis. The educational component of the proposed program will serve to develop a surface and materials chemistry education program at the University of Tennessee, Knoxville. In addition, a YouTube video series, focused on materials, surface, and catalytic science, will be developed in a format accessible to the general population to promote a greater understanding of the impact these sciences have on everyday life.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.

该项目将研究新型低成本材料，用于催化与石油和生物基材料精炼相关的重要化学反应，以生产燃料和各种化学产品。 此外，该项目还将探索通过将催化材料合成为纳米颗粒而不是传统的微米级颗粒来提高催化材料的有效性的潜力。 新材料可以通过许多不同元素的组合形成，该研究还将开发预测特定化学反应的最佳元素组合的方法，从而简化催化剂发现过程并提高美国在燃料和化学品制造领域的竞争力。 该项目将与教育和外展工作联系起来，培训下一代工程师，并提高公众对燃料电池和蓄电池等新节能技术的认识。研究人员实验室的初步工作已经对如何支持纳米颗粒金属间化合物（IMC）可以用明确的本体和表面成分来合成。 该项目将利用这些发现对 IMC 表面化学作为不饱和醛和硝基化合物选择性氢化中组成元素的函数进行系统研究。将使用实验和计算方法来检查 C=C、C=O 和 N-O 活化、解离和氢化的选择性作为 IMC 本体和表面组成以及电子结构信息的函数。 氧化物负载的非贵金属纳米粒子IMC的合成将侧重于对物理现象的清晰理解，这些物理现象决定其体积和表面组成作为元素选择、氧化物选择和制备环境的函数。纳米粒子块状晶体结构的形成将通过原位和原位 X 射线衍射和中子散射进行研究。补充的高分辨率能量色散 X 射线光谱将验证整体成分并量化未纳入 IMC 纳米粒子的元素。 IMC 的表面成分将使用低能离子散射进行分析。组成元素的扩散、颗粒生长和块状晶体结构将作为合成变量的函数进行分析，以全面了解如何生产明确的纳米颗粒 IMC。这些研究的结果将为 IMC 催化剂的合成、表征、反应性评估和稳定性分析开发通用程序。 除了目标反应之外，该项目还将在原子和电子水平上理解如何控制纳米粒子 IMC 催化并广泛应用于对多相催化领域重要的化学转化。拟议计划的教育部分将用于在诺克斯维尔田纳西大学开发表面和材料化学教育计划。 此外，YouTube 视频系列将重点关注材料、表面和催化科学，将以普通大众易于理解的形式制作，以促进人们更好地了解这些科学对日常生活的影响。该奖项反映了 NSF 的法定使命通过使用基金会的智力优点和更广泛的影响审查标准进行评估，并被认为值得支持。

项目成果

Fundamental understanding of the synthesis of well-defined supported non-noble metal intermetallic compound nanoparticles

对明确负载型非贵金属金属间化合物纳米颗粒的合成的基本了解

• DOI: 10.1039/d2cy00183g
• 发表时间: 2022-06
• 期刊: Catalysis Science & Technology
• 影响因子: 5
• 作者: Song, Yuanjun;He, Yang;Laursen, Siris
• 通讯作者: Laursen, Siris

Selective and Stable Non-Noble-Metal Intermetallic Compound Catalyst for the Direct Dehydrogenation of Propane to Propylene

用于丙烷直接脱氢制丙烯的选择性稳定非贵金属金属间化合物催化剂

• DOI: 10.1021/jacs.8b05060
• 发表时间: 2018-10
• 期刊: Journal of the American Chemical Society
• 影响因子: 15
• 作者: He, Yang;Song, Yuanjun;Cullen, David A.;Laursen, Siris
• 通讯作者: Laursen, Siris

The Origin of the Special Surface and Catalytic Chemistry of Ga-Rich Ni 3 Ga in the Direct Dehydrogenation of Ethane

富Ga Ni 3 Ga的特殊表面及催化乙烷直接脱氢化学的起源

• DOI: 10.1021/acscatal.9b03402
• 发表时间: 2019-09
• 期刊: ACS Catalysis
• 影响因子: 12.9
• 作者: He, Yang;Song, Yuanjun;Laursen, Siris
• 通讯作者: Laursen, Siris

Controlling Selectivity and Stability in the Hydrocarbon Wet-Reforming Reaction Using Well-Defined Ni + Ga Intermetallic Compound Catalysts

使用明确的 Ni Ga 金属间化合物催化剂控制烃湿重整反应的选择性和稳定性

• DOI: 10.1021/acscatal.0c01261
• 发表时间: 2020-07-17
• 期刊: ACS Catalysis
• 影响因子: 12.9
• 作者: Yuanjun Song;Yang He;Siris Laursen
• 通讯作者: Siris Laursen

Control of surface reactivity towards unsaturated C C bonds and H over Ni-based intermetallic compounds in semi-hydrogenation of acetylene

• DOI: 10.1016/j.jcat.2019.02.018
• 发表时间: 2019-04-01
• 期刊: Journal of Catalysis
• 影响因子: 7.3
• 作者: Yuanjun Song;Siris Laursen
• 通讯作者: Siris Laursen