Polymeric Ruthenium Porphyrin-Functionalized Carbon Nanotubes and Graphene for Levulinic Ester Transformations into γ-Valerolactone and Pyrrolidone Derivatives,ACS Omega

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Polymeric Ruthenium Porphyrin-Functionalized Carbon Nanotubes and Graphene for Levulinic Ester Transformations into γ-Valerolactone and Pyrrolidone Derivatives
ACS Omega ( IF 3.7 ) Pub Date : 2017-07-07 00:00:00 , DOI: 10.1021/acsomega.7b00427
Ting Zhang _{1,

2,

3} , Yao Ge _{1,

2,

3} , Xuefeng Wang ₁ , Jinzhu Chen _{2,

3} , Xueli Huang ₁ , Yinnian Liao ₁

Affiliation

Polymeric ruthenium porphyrin-functionalized carbon nanotubes (Ru-PP/CNTs) were prepared by the metallation of polymeric porphyrin-functionalized carbon nanotubes (PP/CNTs) with Ru₃(CO)₁₂, whereas PP/CNTs were obtained by the condensation of terephthaldehyde and pyrrole in the presence of CNTs. The Ru-PP/CNTs have a thin layer of highly cross-linked polymeric ruthenium porphyrin coating over the CNT surface via strong π–π stacking interactions, thus showing a bilayered structure with an amorphous polymeric outer surface and an internal CNT core. Polymeric ruthenium porphyrin-functionalized reduced graphene oxide (Ru-PP/RGO) was prepared with a synthetic procedure similar to Ru-PP/CNTs, with RGO as the internal core. Both Ru-PP/CNTs and Ru-PP/RGO showed excellent catalytic performance toward hydrogenation of biomass-related ethyl levulinate (EL) to γ-valerolactone (GVL) with Ru-centered porphyrin units as the catalytic active species. Under optimized reaction conditions, a GVL yield higher than 99% with a complete conversion of EL was observed over both Ru-PP/CNTs and Ru-PP/RGO. In addition to GVL preparation, the versatile Ru-PP/CNTs can efficiently promote reductive amination of EL with various amines for the synthesis of pyrrolidone derivatives, with the corresponding yields ranging from 96.3 to 88.7%. Moreover, the composite materials of both Ru-PP/CNTs and Ru-PP/RGO behave as heterogeneous catalysts in the reaction system and can be easily reused.

中文翻译：

聚合钌卟啉官能化的碳纳米管和石墨烯，用于酯化酯转化为γ-戊内酯和吡咯烷酮衍生物

通过用Ru ₃（CO）₁₂金属化聚合物卟啉官能化的碳纳米管（PP / CNTs），制备了聚合物钌卟啉官能化的碳纳米管（Ru-PP / CNTs）。，而PP / CNTs是在CNTs存在下通过对苯二甲醛和吡咯缩合得到的。Ru-PP / CNT通过强大的π-π堆积相互作用在CNT表面上形成一层薄层的高度交联的聚合钌卟啉涂层，从而显示出具有无定形聚合物外表面和内部CNT核的双层结构。用类似于Ru-PP / CNTs的合成方法，以RGO为内芯，制备了聚合钌卟啉官能化的还原氧化石墨烯（Ru-PP / RGO）。Ru-PP / CNTs和Ru-PP / RGO均表现出优异的催化性能，其中以Ru为中心的卟啉单元为催化活性物质，将生物质相关的乙酰丙酸乙酯（EL）加氢成γ-戊内酯（GVL）。在优化的反应条件下，在Ru-PP / CNT和Ru-PP / RGO上均观察到GVL产率高于99％，且EL完全转化。除了制备GVL外，通用的Ru-PP / CNT还可以有效地促进EL与各种胺的还原胺化反应，从而合成吡咯烷酮衍生物，相应的收率范围为96.3％至88.7％。此外，Ru-PP / CNT和Ru-PP / RGO的复合材料在反应体系中均作为多相催化剂，可以很容易地重复使用。

更新日期：2017-07-07

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