Rational Design of a 3D MnII‐Metal–Organic Framework Based on a Nonmetallated Porphyrin Linker for Selective Capture of CO2 and One‐Pot Synthesis of Styrene Carbonates,Chemistry - A European Journal

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Rational Design of a 3D MnII‐Metal–Organic Framework Based on a Nonmetallated Porphyrin Linker for Selective Capture of CO2 and One‐Pot Synthesis of Styrene Carbonates
Chemistry - A European Journal ( IF 3.9 ) Pub Date : 2018-10-17 , DOI: 10.1002/chem.201803842
Nayuesh Sharma ₁ , Sandeep Singh Dhankhar ₁ , Sandeep Kumar ₁ , T. J. Dhilip Kumar ₁ , C. Mallaiah Nagaraja ₁

Affiliation

A 3D Mn^II‐porphyrin metal–organic framework (MOF), [{Mn₂(TCPP)⋅2H₂O}⋅DMF]_n (MOF1) (TCPP=5,10,15,20‐tetrakis(4‐benzoate)porphyrin), was constructed; it exhibits an interesting 3D framework structure with two types of 1D channels of dimensions of 3.94×8.37 Å² and 4.66×4.93 Å² running along the crystallographic a axis. Owing to the presence of a nonmetallated porphyrin cavity, MOF1 exhibits selective storage of CO₂ with an isosteric heat of adsorption value of 32.1 kJ mol⁻¹, which is further supported by theoretical calculations with the calculated binding energy (BE) of 29.78 kJ mol⁻¹. Interestingly, the nonmetallated nature of the porphyrin ligand was exploited for implantation of coordinatively unsaturated Fe^III ions to generate a Fe^III@MOF1 framework, which acts as an efficient recyclable catalyst for the oxidation of styrenes to the corresponding epoxides in the presence of PhIO as an oxidant at room temperature. Moreover, the one‐pot synthesis of styrene carbonates from styrenes and CO₂ was also achieved using Fe^III@MOF1 as a catalyst. The rational design of a porous Mn^II‐porphyrin MOF for the selective capture of CO₂ and the one‐pot synthesis of styrene carbonates at mild conditions is reported.

中文翻译：

基于非金属化卟啉接头的3D MnII-金属有机骨架的合理设计，用于二氧化碳的选择性捕集和苯乙烯碳酸酯的一锅法合成

一种3D锰^II -卟啉金属-有机骨架（MOF），[{的Mn ₂（TCPP）⋅ 2H ₂ ö} ⋅ DMF] _Ñ（MOF 1）（TCPP = 5,10,15,20-四（4-苯甲酸）卟啉），它显示出与两种类型的3.94×8.37埃尺寸1D通道的一个有趣的三维框架结构²和4.66×4.93埃²沿晶体运行一个轴。由于存在非金属化的卟啉腔，MOF 1表现出对CO _2的选择性存储，其等值吸附热值为32.1 kJ mol ^-1，这进一步得到理论计算的支持，计算出的结合能（BE）为29.78 kJ mol ^-1。有趣的是，利用卟啉配体的非金属化性质来注入配位不饱和的Fe ^III离子以生成Fe ^III @MOF 1骨架，该骨架可作为有效的可回收催化剂，用于在PhIO存在下将苯乙烯氧化为相应的环氧化物在室温下用作氧化剂。此外，使用Fe ^III @MOF 1作为催化剂，也可以从苯乙烯和CO ₂一锅法合成苯乙烯碳酸酯。多孔Mn ^II的合理设计报道了在适当条件下使用卟啉MOF选择性捕获CO ₂和一锅法合成苯乙烯碳酸酯的方法。

更新日期：2018-10-17

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