介孔二氧化硅纳米颗粒负载铑催化剂结构的固态核磁共振研究
A solid-state NMR investigation of the structure of mesoporous silica nanoparticle supported rhodium catalysts.
作者信息
Rapp Jennifer L, Huang Yulin, Natella Michael, Cai Yang, Lin Victor S-Y, Pruski Marek
机构信息
US DOE Ames Laboratory, Iowa State University, Ames, IA 50011, USA.
出版信息
Solid State Nucl Magn Reson. 2009 Apr;35(2):82-6. doi: 10.1016/j.ssnmr.2008.12.004. Epub 2009 Jan 4.
A detailed study of the chemical structure of mesoporous silica catalysts containing rhodium ligands and nanoparticles (RhP-MSN) was carried out by multi-dimensional solid-state NMR techniques. The degree of functionalization of the rhodium-phosphinosilyl complex to the surface of the RhP-MSN channels was determined by (29)Si NMR experiments. The structural assignments of the rhodium-phosphinosilyl complex were unambiguously determined by employing the novel, indirectly detected heteronuclear correlation ((13)C-(1)H and (31)P-(1)H idHETCOR) techniques, which indicated that oxidation of the attached phosphinosilyl groups and detachment of Rh was enhanced upon syngas conversion.
通过多维固态核磁共振技术对含有铑配体和纳米颗粒的介孔二氧化硅催化剂（RhP-MSN）的化学结构进行了详细研究。通过（29）Si核磁共振实验确定了铑-膦基硅基络合物在RhP-MSN通道表面的官能化程度。采用新型间接检测异核相关（（13）C-（1）H和（31）P-（1）H idHETCOR）技术明确确定了铑-膦基硅基络合物的结构归属，结果表明，在合成气转化过程中，附着的膦基硅基的氧化和Rh的脱离增强。
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