Dialing in Catalytic Sites on Metal Organic Framework Nodes: MIL-53(Al) and MIL-68(Al) Probed with Methanol Dehydration Catalysis

Dialing in Catalytic Sites on Metal Organic Framework Nodes: MIL-53(Al) and MIL-68(Al) Probed with Methanol Dehydration Catalysis
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拨入金属有机骨架节点上的催化位点:用甲醇脱水催化探测 MIL-53(Al) 和 MIL-68(Al)

DOI:
10.1021/acsami.0c16559
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发表时间:
2020
影响因子:
9.5
通讯作者:
Yang Dong
Yang Dong
中科院分区:
材料科学2区
文献类型:
--
作者:
Wang Zhengyan;Babucci Melike;Zhang Yafeng;Wen Yujie;Peng Luming;Yang Bing;Gates Bruce C.;Yang Dong

文献摘要

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Many metal organic frameworks (MOFs) incorporate metal oxide clusters as nodes. Node sites where linkers are missing can be catalytic sites. We now show how to dial in the number and occupancy of such sites in MIL-53 and MIL-68, which incorporate aluminum-oxide-like nodes. The methods involve modulators used in synthesis and postsynthesis reactions to control the modulator-derived groups on these sites. We illustrate the methods using formic acid as a modulator, giving formate ligands on the sites, and these can be removed to leave μ2-OH groups and open Lewis acid sites. Methanol dehydration was used as a catalytic reaction to probe these sites, with infrared spectra giving evidence of methoxide ligands as reaction intermediates. Control of node surface chemistry opens the door for placement of a variety of ligands on a wide range of metal oxide cluster nodes for dialing in reactivity and catalytic properties of a potentially immense class of structurally well-defined materials.