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Substrate dependence on the fixation of CO2 to cyclic carbonates over reusable porous hybrid solids
Journal of CO2 Utilization ( IF 7.7 ) Pub Date : 2018-06-26 , DOI: 10.1016/j.jcou.2018.06.013
Joel M. Kolle , Abdelhamid Sayari

N,N,N-tributyl-N-propylammonium iodide-functionalized mesoporous silicas (SBA-15 and a silica gel) proved to be efficient, robust and reusable catalysts for the solvent-free synthesis of cyclic carbonates (CCs) from epoxides and CO2. The reusability of the catalysts was found to be dependent on the nature of the support and the substrate. In the presence of 1,2-epoxybutane (1,2-EB) as substrate, the SBA-15-based catalyst (PHS-1) exhibited a constant catalytic activity for five reaction cycles (yield > 96.0%) under mild conditions (1.0 MPa CO2, 100 °C and 4 h). Conversely, in the presence of styrene oxide, a gradual decrease in yield was observed. Based on textural properties and 13C CP-MAS NMR measurements, such decline was attributed to the adsorption of solid reaction product (styrene carbonate - SC) on the catalyst surface. Using a chromatographic silica gel as support and an improved catalyst recovery step gave rise to a highly efficient, robust and fully reusable catalyst (PHS-2) for the synthesis of CCs. Notably, PHS-2 led to a 33–50% decrease in reaction time, and maintained an excellent and steady catalytic activity over 5 cycles in the synthesis of SC (yield > 96% and selectivity > 97%). The amount of trapped solid SC product on PHS-2 surface was also significantly reduced.



中文翻译:

基质对可重复使用的多孔杂化固体上CO 2固定于环状碳酸酯的依赖性

N,N,N-三丁基-N-丙基碘化碘铵官能化的介孔二氧化硅(SBA-15和硅胶)被证明是高效,坚固且可重复使用的催化剂,用于由环氧化物和CO进行无溶剂合成环状碳酸酯(CC)2。发现催化剂的可重复使用性取决于载体和底物的性质。在以1,2-环氧丁烷(1,2-EB)为底物的情况下,基于SBA-15的催化剂(PHS-1)在温和的条件下对五个反应周期表现出恒定的催化活性(收率> 96.0%)(在1.0MPa的CO 2,100℃和4小时)。相反,在氧化苯乙烯的存在下,观察到收率逐渐降低。基于纹理特性和13在C CP-MAS NMR测量中,这种下降归因于固体反应产物(碳酸苯乙烯-SC)在催化剂表面的吸附。使用色谱硅胶作为载体和改进的催化剂回收步骤产生了用于合成CC的高效,坚固且可完全重复使用的催化剂(PHS-2)。值得注意的是,PHS-2缩短了反应时间33-50%,并在SC合成的5个循环中保持了出色且稳定的催化活性(产率> 96%,选择性> 97%)。PHS-2表面上捕获的固体SC产物的量也显着减少。

更新日期:2018-06-26
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