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.

立法法规和降低全球石油原料的质量需要所有更活跃的催化剂，以使石油产品脱硫。基于钼二硫化物（MOS2）的氢化硫化材料（HDS）代表了工业应用和HDS催化学术研究的快速生长领域。一个关键的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。基于我在博士学位论文期间合成的小型，高质量的MOS2纳米颗粒的合成，我的目标是将这些构件纳入合成催化活性和健壮的结构，以在工作催化条件下保留其高活性和选择性。我的目标是创建催化结构功能理解，这将成为发展我的学术生涯的基础。我试图在加利福尼亚大学伯克利分校的Katz教授研究小组中进行博士后研究，因为该小组是calixarene配体的簇和纳米粒子表面功能化的世界领导者，它们在空间上是散装的配体，可防止散布的配体，可防止凝聚并在表面同时进行自由协调。亚历山大·卡茨（Alexander Katz）组表明，非常笨重的配体和非常小的纳米颗粒的结合导致了配体无法完全覆盖颗粒表面的情况。结果是不饱和位点的结果，预计这对于稳定高度活跃和有趣的位点至关重要。此外，在卡利克萨烯配体处的官能团（捐赠或退出的电子）可以影响纳米颗粒的电子结构，因此还会影响其催化特性，并将其掺入基于MOS2的纳米颗粒的重要镍成分。

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