Controlled Grafting Synthesis of Silica-Supported Boron for Oxidative Dehydrogenation Catalysis
Controlled Grafting Synthesis of Silica-Supported Boron for Oxidative Dehydrogenation Catalysis
复制标题
氧化脱氢催化剂用二氧化硅负载硼的控制接枝合成
DOI：
10.1021/acs.jpcc.1c01899
复制
发表时间：
2021-06-07
影响因子：
3.7
通讯作者：
Hermans, Ive
中科院分区：
文献类型：
--
作者：
Cendejas, Melissa C.;Dorn, Rick W.;Hermans, Ive
我们介绍了无定形二氧化硅上的Pinacolborane的受控嫁接合成。 B-11固态NMR和红外光谱显示，前体分子单独锚定在表面上，并可以与邻近的未反应硅烷醇基团形成氢键相互作用。氢键的程度可以通过二氧化硅预处理脱水温度来控制。真空植物材料的热处理可产生氧化/水解的硼的簇，无论硼重负荷如何，都说明硼在高温下在二氧化硅表面上非常流动。该材料表现出对二氧化硅支持的硼催化剂预期的丙烷氧化脱氢活性。有趣的是，这些支持的催化剂的动力学行为偏离了先前报道的散装硼材料的动力学行为，从而进一步研究了这些材料的反应动力学。这里获得的合成和催化见解可以为未来的研究提供改进的合成途径和反应动力学的研究。
We present the controlled grafting synthesis of pinacolborane on amorphous silica. B-11 solid-state NMR and IR spectroscopies reveal that the precursor molecule anchors monopodally to the surface and can form hydrogen-bonding interactions with neighboring unreacted silanol groups. The extent of hydrogen bonding can be controlled by the silica pretreatment dehydration temperature. Thermal treatment of the grafted boron materials under vacuum generates clusters of oxidized/hydrolyzed boron regardless of boron weight loading, illustrating that boron is highly mobile on the silica surface at elevated temperatures. The materials exhibit propane oxidative dehydrogenation activity expected for silica-supported boron catalysts. Interestingly, the kinetic behavior of these supported catalysts deviates from that of previously reported bulk boron materials, prompting further studies into the reaction kinetics over these materials. The synthetic and catalytic insights gained here can inform future studies of improved synthesis routes and reaction kinetics.