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Zr‐Metal‐Organic Framework Catalysts for Oxidative Desulfurization and Their Improvement by Postsynthetic Ligand Exchange
Small Methods ( IF 12.4 ) Pub Date : 2018-08-26 , DOI: 10.1002/smtd.201800203
Guangxia Fu 1 , Bart Bueken 1 , Dirk De Vos 1
Affiliation  

Two types of Zr6‐based metal‐organic frameworks (MOF), {Zr6O4(OH)4(C6H3(COO)3)2(HCOO)6} (MOF‐808) and {Zr6O4(OH)4(C24H15(COO)3)2(HCOO)6} (UMCM‐309) are investigated as heterogeneous catalysts in oxidative desulfurization reactions. Postsynthetic approaches targeting the removal of the coordinating formate ligands are applied to further improve the MOFs’ catalytic activity, resulting in the formation of additional ZrIV open sites. Thus, three modified MOFs, namely MOF‐808‐M, UMCM‐309‐M1, and UMCM‐309‐M2, are synthesized with larger numbers of open sites, as shown by CD3CN chemisorption monitored by Fourier‐transform infrared spectroscopy (FTIR), leading to higher catalytic activity. Even at low catalyst loading, MOF‐808‐M exhibits high catalytic activity in the oxidation of sulfur compounds as well as high selectivity and reusability.

中文翻译:

Zr-金属-有机框架催化剂用于氧化脱硫及其合成后配体交换的改进

两种基于Zr 6的金属有机骨架(MOF),{Zr 6 O 4(OH)4(C 6 H 3(COO)32(HCOO)6 }(MOF-808)和{Zr 6 O 4(OH)4(C 24 H 15(COO)32(HCOO)6}(UMCM‐309)被研究为氧化脱硫反应中的非均相催化剂。靶向去除配位甲酸配体的合成后方法可用于进一步提高MOF的催化活性,从而形成额外的Zr IV开口位点。因此,合成了三个修饰的MOF,即MOF-808-M,UMCM-309-M1和UMCM-309-M2,它们具有大量的开放位点,如通过傅里叶变换红外光谱法监测的CD 3 CN化学吸附所显示的( FTIR),导致更高的催化活性。即使在低催化剂负载下,MOF-808-M在氧化硫化合物方面也显示出高催化活性,并且具有很高的选择性和可重复使用性。
更新日期:2018-08-26
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