Cooperative Interplay of Brønsted Acid and Lewis Acid Sites in MIL-101(Cr) for Cross-Dehydrogenative Coupling of C–H Bonds,ACS Applied Materials & Interfaces

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Cooperative Interplay of Brønsted Acid and Lewis Acid Sites in MIL-101(Cr) for Cross-Dehydrogenative Coupling of C–H Bonds
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-03-02 , DOI: 10.1021/acsami.0c20369
Jingwen Chen _{1,

2} , Yuanyuan Zhang _{1,

2} , Xiaoling Chen ₁ , Siyun Dai ₁ , Zongbi Bao _{1,

2} , Qiwei Yang _{1,

2} , Qilong Ren _{1,

2} , Zhiguo Zhang _{1,

2}

Affiliation

Cross-dehydrogenative coupling (CDC) is an effective tool for carbon–carbon bond formation in chemical synthesis. Herein, we report a metal–organic framework (MOF) possessing dual Lewis acidic Cr sites and sulfonic acid sites (MIL-101(Cr)–SO₃H) as an efficient catalytic material for direct cross-coupling of xanthene and different nucleophiles using O₂ as the oxidant. The highly porous structure of MIL-101(Cr)–SO₃H enables the free access of reactants to the catalytic active sites inside MOF pores. Kinetic studies indicated that the Cr sites of MOF accelerate the rate-limiting autoxidation reaction of xanthene, which synergistically work with the sulfonic acid group on MOF ligands in promoting the CDC reactions. Besides, the catalytic system shows excellent functional group compatibility, and a variety of valuable xanthene derivatives were synthesized with satisfactory yields. Furthermore, MIL-101(Cr)–SO₃H can be reused and its catalytic activity and crystal structure remain after six consecutive runs.

中文翻译：

MIL-101（Cr）中Brønsted酸和Lewis酸位点之间的相互作用，用于C–H键的交叉脱氢偶联

交叉脱氢偶联（CDC）是化学合成中碳-碳键形成的有效工具。在这里，我们报告一个金属-有机骨架（MOF），具有路易斯酸的两个酸性Cr位点和一个磺酸位点（MIL-101（Cr）-SO ₃ H），作为一种有效的催化材料，用于using吨和不同亲核试剂的直接交叉偶联。 O ₂作为氧化剂。MIL-101（Cr）–SO ₃的高度多孔结构H使反应物自由进入MOF孔内的催化活性位。动力学研究表明，MOF的Cr位点加速了x吨的限速自氧化反应，它与MOF配体上的磺酸基协同作用促进CDC反应。此外，该催化体系显示出优异的官能团相容性，并且以令人满意的产率合成了多种有价值的x吨衍生物。此外，MIL-101（Cr）-SO ₃ H可以重复使用，并且连续六次运行后仍具有催化活性和晶体结构。

更新日期：2021-03-10

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