Silica-supported, narrowly distributed, subnanometric Pt–Zn particles from single sites with high propane dehydrogenation performance,Chemical Science

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Silica-supported, narrowly distributed, subnanometric Pt–Zn particles from single sites with high propane dehydrogenation performance
Chemical Science ( IF 7.6 ) Pub Date : 2019/12/23 , DOI: 10.1039/c9sc05599a
Lukas Rochlitz _{1,

2,

3,

4} , Keith Searles _{1,

2,

3,

4} , Jan Alfke _{1,

2,

3,

4,

5} , Dmitry Zemlyanov _{6,

7,

8,

9} , Olga V. Safonova _{4,

5,

10} , Christophe Copéret _{1,

2,

3,

4}

Affiliation

The development of highly productive, selective and stable propane dehydrogenation catalysts for propene production is strategic due to the increasing need for propene and the availability of shale gas, an abundant source of light alkanes. In that context, the combination of surface organometallic chemistry (SOMC) and a thermolytic molecular precursor (TMP) approach is used to prepare bimetallic subnanometric and narrowly distributed Pt–Zn alloyed particles supported on silica via grafting of a Pt precursor on surface OH groups present in a Zn single-site containing material followed by a H₂ reduction treatment. This material, that exhibits a Zn to Pt molar ratio of 3 : 2 in the form of alloyed Pt–Zn particles with a 0.2 to 0.4 fraction of the overall Zn amount remaining as Zn^II sites on the silica surface, catalyzes propane dehydrogenation (PDH) with high productivity (703 g_C₃H₆ g_Pt⁻¹ h⁻¹ to 375 g_C₃H₆ g_Pt⁻¹ h⁻¹) and very low deactivation rates (k_d = 0.027 h⁻¹) over 30 h at high WHSV (75 h⁻¹). This study demonstrates how SOMC can provide access to highly efficient and tailored catalysts through the stepwise introduction of specific elements via grafting to generate small, homogeneously and narrowly distributed supported alloyed nanoparticles at controlled interfaces.

中文翻译：

二氧化硅支撑的，分布狭窄的亚微米级Pt-Zn颗粒，来自单个位置，具有较高的丙烷脱氢性能

由于对丙烯的需求增加和页岩气的可获得性，页岩气是轻质烷烃的丰富来源，开发用于丙烯生产的高生产率，选择性和稳定的丙烷脱氢催化剂具有战略意义。在这种情况下，将表面有机金属化学（SOMC）和热解分子前体（TMP）方法结合使用，通过将Pt前体接枝到存在的表面OH基团上，制备负载在二氧化硅上的双金属亚纳米且分布较窄的Pt-Zn合金颗粒。在含Zn单部位的材料中进行H ₂还原处理。这种材料以合金化的Pt-Zn颗粒的形式显示出Zn与Pt的摩尔比为3：2，而总Zn量的0.2％至0.4％保留为Zn二氧化硅表面上的^II位可以高生产率（703 g_{C ₃ H ₆} g_Pt^-1 h^-1至375 g_{C ₃ H ₆} g_Pt^-1 h^-1）催化丙烷脱氢（PDH），并且失活速率非常低（ ķ _d = 0.027ħ^-1）在高压时WHSV 30小时（75ħ^-1）。这项研究表明，SOMC如何通过逐步引入特定元素，从而提供使用高效，量身定制的催化剂的途径。接枝以在受控界面处生成小的，均匀且狭窄分布的负载合金纳米颗粒。

更新日期：2020-02-13

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