Oriented designing the microenvironment of catalytic sites is essential for understanding catalytic processes. In this work, EDTA was first grafted in UiO-66 and then chelated Rh to obtain an efficient catalyst for 1-hexene hydroformylation reaction. EDTA not only served as a chelation site for Rh immobilization in UiO-66, but also markedly influenced the structure and properties of Rh/UiO-66. The incorporation of EDTA reduced the micropore content and suppressed the formation of heavy products. Moreover, the grafted EDTA regulated the electronic state of Rh effectively to improve the CO and propene adsorption, thus constructing an appropriate microenvironment for hydroformylation. Therefore, EDTA-modified Rh/U-E catalyst exhibited higher aldehydes yield, TOF and stability than Rh/U without EDTA. The dual role of EDTA in anchoring Rh sites and modulating the microenvironment for hydroformylation provides more prospects for designing customized MOFs-based catalysts.

中文翻译：

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在 UiO-66 中接枝 EDTA 调节 Rh 微环境以进行 1-己烯氢甲酰化

定向设计催化位点的微环境对于理解催化过程至关重要。本工作首先将EDTA接枝到UiO-66上，然后螯合Rh，得到1-己烯加氢甲酰化反应的高效催化剂。 EDTA不仅作为UiO-66中Rh固定的螯合位点，而且显着影响Rh/UiO-66的结构和性质。 EDTA 的加入降低了微孔含量并抑制了重产物的形成。此外，接枝的EDTA有效调节Rh的电子态，提高CO和丙烯的吸附，从而构建合适的加氢甲酰化微环境。因此，EDTA 修饰的 Rh/UE 催化剂比不含 EDTA 的 Rh/U 表现出更高的醛收率、TOF 和稳定性。 EDTA 在锚定 Rh 位点和调节加氢甲酰化微环境方面的双重作用为设计定制的 MOF 基催化剂提供了更多前景。