A high-throughput investigation of the role of pH, temperature, concentration, and time on the synthesis of hybrid inorganic-organic materials

A high-throughput investigation of the role of pH, temperature, concentration, and time on the synthesis of hybrid inorganic-organic materials
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DOI:
10.1002/anie.200501766
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发表时间:
2005-01-01
影响因子:
16.6
通讯作者:
Cheetham, AK
Cheetham, AK
中科院分区:
化学1区
文献类型:
--
作者:
Forster, PM;Stock, N;Cheetham, AK

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自20世纪40年代被发现以来,合成的铝硅酸盐沸石因其重要的催化、离子交换和吸附性能而成为主要的研究热点。[1]由于许多商业上重要的沸石可以通过改变简单的变量如温度、反应时间、硅铝比和pH而在没有有机模板的情况下合成,[2]详细了解这些变量在沸石合成中所起的作用[3]仍然是该领域最重要的进展之一。到目前为止,类似的研究在无机-有机混合体系中还很少见。相反,由于网状化学的显著成功,该领域一直专注于了解有机分子在决定杂化材料所采用的整体结构中的作用。[5]因此,尽管已描述了13000多个金属-有机骨架(MOF),[6]很少有金属中心和配体[+]的组合被确定为两个或三个以上的结构。[7]含有水和/或氢氧化物离子的丁二酸钴的五个特征良好的相的存在[8]提供了一个难得的机会来检验各种反应变量在确定哪些结构形成方面的作用。此外,这一系列包括一维、二维和三维体系,其中几个包含无限的Co-O-Co网络,除了相对较高的热稳定性外,这些网络还可能显示出有趣的磁性[9]或催化[10]性质。
Since their discovery in the 1940s, synthetic aluminosilicate zeolites have become a major research focus owing to their commercially important catalytic, ion-exchange, and sorption properties.[1] Because many of the commercially important zeolites may be synthesized without organic templates by altering simple variables such as temperature, reaction time, Si/Al ratio, and pH,[2] a detailed understanding of the role that these variables play in zeolite synthesis [3] remains one of the most important advancements in the field. Similar studies, to date, are rare for hybrid inorganic–organic systems. Instead, as a result of the remarkable success of reticular chemistry,[4] the field has focused on understanding the role of the organic molecules in determining the overall structures that hybrid materials adopt.[5] Consequently, while more than 13000 metal–organic frameworks (MOFs) have been described,[6] there are very few combinations of metal centers and ligands [+] for which more than two or three structures have been identified.[7]The existence of five well-characterized phases of cobalt succinates containing water and/or hydroxide ions [8] offers a rare opportunity to examine the role of various reaction variables in determining which structure forms. Moreover, this family includes one-, two-, and three-dimensional systems, several of which contain infinite Co-O-Co networks,-which may display interesting magnetic [9] or catalytic [10] properties in addition to relatively high thermal stability.[11] However, since these cobalt succinate phases have been