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Crystal Structure Directed Catalysis by Aluminum Metal-Organic Framework: Mechanistic Insight into the Role of Coordination of Al Sites and Entrance Size of Catalytic Pocket
ACS Materials Letters ( IF 11.4 ) Pub Date : 2020-05-27 , DOI: 10.1021/acsmaterialslett.9b00527 Ayan Maity 1 , Baljeet Singh 1 , Kshama Sharma 2 , Subhradip Paul 3 , P. K. Madhu 2 , Vivek Polshettiwar 1
ACS Materials Letters ( IF 11.4 ) Pub Date : 2020-05-27 , DOI: 10.1021/acsmaterialslett.9b00527 Ayan Maity 1 , Baljeet Singh 1 , Kshama Sharma 2 , Subhradip Paul 3 , P. K. Madhu 2 , Vivek Polshettiwar 1
Affiliation
The use of metal-organic frameworks (MOFs) in the field of catalysis is growing exponentially due to their high surface area and distinctive active sites. In this work, we report a novel understanding of the active sites responsible for the catalytic activity of aluminum trimesate MOFs and their crystal/framework structure dependency. Here, we have studied the nature of the active sites of Al-MOFs with two different framework structures (MIL-100 and MIL-96). We found that the MOFs with MIL-100 framework structures were highly catalytically active, while the same Al-MOFs with MIL-96 framework structures exhibited poor catalytic activity. This behavior is explained based on the effect of coordinated water molecules on their Brønsted acidity as well as the effect of the coordination of Al sites, specifically hexacoordinated Al3+6c sites and pentacoordinated Al3+5c sites, on their Lewis acidity. The different entrance sizes of the catalytic pocket of MIL-96 and MIL-100 also played critical roles in their catalytic performance.
中文翻译:
铝-金属框架指导的晶体结构催化:铝位点配位作用和催化口袋入口尺寸的机理研究
由于其高表面积和独特的活性位,在催化领域中金属有机骨架(MOF)的使用呈指数增长。在这项工作中,我们报告了对负责对铝均苯三酸酯MOFs的催化活性及其晶体/框架结构依赖性的活性位点的新颖理解。在这里,我们研究了具有两种不同框架结构(MIL-100和MIL-96)的Al-MOF活性位点的性质。我们发现具有MIL-100骨架结构的MOF具有很高的催化活性,而具有MIL-96骨架结构的相同的Al-MOF具有较差的催化活性。基于配位水分子对其布朗斯台德酸度的影响以及铝位点(特别是六配位铝)配位的影响来解释这种行为。3+ 6c位点和五配位Al 3+ 5c位点的路易斯酸度。MIL-96和MIL-100催化袋的不同入口尺寸在其催化性能中也起着关键作用。
更新日期:2020-07-06
中文翻译:
铝-金属框架指导的晶体结构催化:铝位点配位作用和催化口袋入口尺寸的机理研究
由于其高表面积和独特的活性位,在催化领域中金属有机骨架(MOF)的使用呈指数增长。在这项工作中,我们报告了对负责对铝均苯三酸酯MOFs的催化活性及其晶体/框架结构依赖性的活性位点的新颖理解。在这里,我们研究了具有两种不同框架结构(MIL-100和MIL-96)的Al-MOF活性位点的性质。我们发现具有MIL-100骨架结构的MOF具有很高的催化活性,而具有MIL-96骨架结构的相同的Al-MOF具有较差的催化活性。基于配位水分子对其布朗斯台德酸度的影响以及铝位点(特别是六配位铝)配位的影响来解释这种行为。3+ 6c位点和五配位Al 3+ 5c位点的路易斯酸度。MIL-96和MIL-100催化袋的不同入口尺寸在其催化性能中也起着关键作用。