Enabling Access to Reduced Open-Metal Sites in Metal-Organic Framework Materials through Choice of Anion Identity: The Case of MIL-100(Cr),ACS Materials Letters

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Enabling Access to Reduced Open-Metal Sites in Metal-Organic Framework Materials through Choice of Anion Identity: The Case of MIL-100(Cr)
ACS Materials Letters ( IF 9.6 ) Pub Date : 2020-06-16 , DOI: 10.1021/acsmaterialslett.0c00177
Jacklyn N. Hall ₁ , Praveen Bollini ₁

Affiliation

Metal-organic framework materials (MOFs) offer the opportunity to exploit open-metal sites having well-defined coordination environments, one of the key features of which is open-metal oxidation state. MIL-100(Cr) is a prototypical MOF in this regard, with M²⁺ sites offering the potential for breakthroughs not only in the area of selective gas adsorption but also acid and redox catalysis. We report herein, for the first time, the use of hydroxyl anions in accessing the theoretical maximum density of MIL-100 Cr²⁺ sites. We show, using five complementary characterization techniques, that the use of hydroxyl-endowed MIL-100, unlike the fluoride-containing analogue used extensively in the literature, enables creation of one Cr²⁺ site per node. The results point to anion identity being a key synthetic choice, the judicious use of which could enable control over open-metal oxidation state in MOF materials more broadly.

中文翻译：

通过选择阴离子身份，能够访问金属有机骨架材料中减少的开放金属部位：MIL-100（Cr）的情况

金属有机框架材料（MOF）提供了开发具有明确定义的协调环境的开放金属场所的机会，其中关键特征之一是开放金属的氧化态。在这方面，MIL-100（Cr）是典型的MOF，M ²⁺位点不仅在选择性气体吸附领域而且在酸和氧化还原催化领域都具有突破的潜力。我们在此首次报告了羟基阴离子在获得MIL-100 Cr ²⁺位点的理论最大密度方面的用途。我们显示，使用五种互补的表征技术，与文献中广泛使用的含氟类似物不同，使用羟基赋予的MIL-100可以产生一种Cr ²⁺每个节点的站点。结果表明，阴离子身份是关键的合成选择，明智地使用它可以更广泛地控制MOF材料中的开金属氧化态。

更新日期：2020-07-06

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