Calixarene-functionalized MoS2 nanoparticles as catalysts for HDS reactions

杯芳烃功能化的 MoS2 纳米颗粒作为 HDS 反应的催化剂

• 批准号: 325483629
• 负责人: Dr. Christian Schöttle
• 金额: --
• 依托单位: Department of Chemical & Biomolecular Engineering
• 依托单位国家: 德国
• 项目类别: Research Fellowships
• 财政年份: 2016
• 资助国家: 德国
• 起止时间: 2015-12-31 至 2017-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/325483629?language=en
• 关键词: Calixarene; functionalized; MoS2; nanoparticles; catalysts

Legislative regulations and decreasing quality of global oil feedstocks require all the more active catalysts for the desulfurization of petroleum products. Materials for hydrodesulfurization (HDS) based on molybdenum disulfide (MoS2) represent a rapidly growing area of industrial application and academic research for HDS catalysis. A crucial aspect is to obtain a high surface area to facilitate catalytic activity, and to stabilize small particle sizes during catalysis under high temperature reducing conditions. Based on the synthesis of small, high quality MoS2 nanoparticles that I have synthesized during my PhD thesis, I aim to incorporate these building blocks to synthesize catalytically active and robust structures that retain their high activity and selectivity under working catalysis conditions. My goal is to create catalytic structure-function understanding that will serve as a foundation for developing my academic career. I seek to perform postdoctoral studies in the research group of Professor Katz at University of California, Berkeley because this group is a world leader in the surface functionalization of clusters and nanoparticles with calixarene ligands, which act as sterically bulky ligands that prevent agglomeration and create free coordination sites at the surface simultaneously. The group of Alexander Katz has demonstrated that the combination of very bulky ligands and very small nanoparticles lead to a situation that the ligands cannot cover the particle's surface completely. Coordinatively unsaturated sites are the result, which are predicted to be crucial for stabilizing highly active and interesting sites for hydrodesulfurization catalysis. Furthermore, functional groups (electron donating or withdrawing) at the calixarene ligand can influence the electronic structure of the nanoparticle and therefore also their catalytic properties, as well as incorporation of crucial nickel components to the MoS2-based nanoparticles.

立法法规和全球石油原料质量的下降需要更加活跃的催化剂来进行石油产品脱硫。基于二硫化钼 (MoS2) 的加氢脱硫 (HDS) 材料代表了 HDS 催化工业应用和学术研究快速增长的领域。一个关键方面是获得高表面积以促进催化活性，并在高温还原条件下催化过程中稳定小粒径。基于我在博士论文期间合成的小型、高质量 MoS2 纳米颗粒的合成，我的目标是结合这些构建块来合成具有催化活性和坚固的结构，在工作催化条件下保持其高活性和选择性。我的目标是建立对催化结构功能的理解，这将成为我学术生涯发​​展的基础。我寻求在加州大学伯克利分校卡茨教授的研究小组进行博士后研究，因为该小组在杯芳烃配体团簇和纳米粒子表面功能化方面处于世界领先地位，杯芳烃配体充当空间庞大的配体，可防止团聚并同时在表面产生自由配位位点。 Alexander Katz的研究小组已经证明，非常大的配体和非常小的纳米颗粒的结合会导致配体无法完全覆盖颗粒表面。结果是配位不饱和位点，预计这对于稳定加氢脱硫催化的高活性和有趣位点至关重要。此外，杯芳烃配体上的官能团（给电子或吸电子）可以影响纳米粒子的电子结构，从而影响其催化性能，以及关键的镍成分与MoS2基纳米粒子的结合。

项目成果

Understanding the role of Zn2+ in surfactant-free layered silicate delamination: Exfoliation of magadiite

• DOI: 10.1016/j.micromeso.2019.03.048
• 发表时间: 2019-07
• 期刊: Microporous and Mesoporous Materials
• 影响因子: 5.2
• 作者: A. Okrut;Nicolás A. Grosso‐Giordano;Christian Schöttle;S. Zones;Alexander Katz

SSZ-70 borosilicate delamination without sonication: effect of framework topology on olefin epoxidation catalysis.

• DOI: 10.1039/c8dt03044h
• 发表时间: 2018-10
• 期刊: Dalton transactions
• 影响因子: 4
• 作者: A. Okrut;M. Aigner;Christian Schöttle;Nicolás A. Grosso‐Giordano;Son-Jong Hwang;X. Ouyang;S. Zones;Alexander Katz

Bulky Calixarene Ligands Stabilize Supported Iridium Pair-Site Catalysts.

• DOI: 10.1021/jacs.8b13013
• 发表时间: 2019-02
• 期刊: Journal of the American Chemical Society
• 影响因子: 15
• 作者: Christian Schöttle;Erjia Guan;A. Okrut;Nicolás A. Grosso‐Giordano;Andrew P Palermo;A. Solovyov;B. Gates;Alexander Katz

Epoxidation of 1-octene under harsh tail-end conditions in a flow reactor II: impact of delaminated-zeolite catalyst surface area and structural integrity on catalytic performance

流动反应器 II 中恶劣尾端条件下 1-辛烯的环氧化：分层沸石催化剂表面积和结构完整性对催化性能的影响

• DOI: 10.1039/c7re00138j
• 发表时间: 2017
• 期刊: Reaction Chemistry and Engineering
• 影响因子: 3.9
• 作者: M. Aigner;N. A. Grosso-Giordano;C. Schöttle;A. Okrut;S. Zones;A. Katz
• 通讯作者: A. Katz

Synthesis and Electrochemical Stability of Ultrahigh Aspect Ratio Nanoporous Gold after Calixarene-Phosphine Ligand Removal.

• DOI: 10.1021/acsami.9b00754
• 发表时间: 2019-04
• 期刊: ACS applied materials & interfaces
• 影响因子: 9.5
• 作者: Yuhui Xie;Christian Schöttle;Ying Li;C. Carraro;Xinya Zhang;Alexander Katz;R. Maboudian